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Sample records for actinide analysis system

  1. Thermal analysis for fuel handling system for sodium cooled reactor considering minor actinide-bearing metal fuel.

    SciTech Connect

    Chikazawa, Y.; Grandy, C.; Nuclear Engineering Division

    2009-03-01

    The Advanced Burner Reactor (ABR) is one of the components of the Global Nuclear Energy Partnership (GNEP) used to close the fuel cycle. ABR is a sodium-cooled fast reactor that is used to consume transuranic elements resulting from the reprocessing of light water reactor spent nuclear fuel. ABR-1000 [1000 MW(thermal)] is a fast reactor concept created at Argonne National Laboratory to be used as a reference concept for various future trade-offs. ABR-1000 meets the GNEP goals although it uses what is considered base sodium fast reactor technology for its systems and components. One of the considerations of any fast reactor plant concept is the ability to perform fuel-handling operations with new and spent fast reactor fuel. The transmutation fuel proposed as the ABR fuel has a very little experience base, and thus, this paper investigates a fuel-handling concept and potential issues of handling fast reactor fuel containing minor actinides. In this study, two thermal analyses supporting a conceptual design study on the ABR-1000 fuel-handling system were carried out. One analysis investigated passive dry spent fuel storage, and the other analysis investigated a fresh fuel shipping cask. Passive dry storage can be made suitable for the ABR-1000 spent fuel storage with sodium-bonded metal fuel. The thermal analysis shows that spent fast reactor fuel with a decay heat of 2 kW or less can be stored passively in a helium atmosphere. The 2-kW value seems to be a reasonable and practical level, and a combination of reasonably-sized in-sodium storage followed by passive dry storage could be a candidate for spent fuel storage for the next-generation sodium-cooled reactor with sodium-bonded metal fuel. Requirements for the shipping casks for minor actinide-bearing fuel with a high decay heat level are also discussed in this paper. The shipping cask for fresh sodium-cooled-reactor fuel should be a dry type to reduce the reaction between residual moisture on fresh fuel and the

  2. Advanced Aqueous Separation Systems for Actinide Partitioning

    SciTech Connect

    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.

  3. Systematization of actinides using cluster analysis

    SciTech Connect

    Kopyrin, A.A.; Terent`eva, T.N.; Khramov, N.N.

    1994-11-01

    A representation of the actinides in multidimensional property space is proposed for systematization of these elements using cluster analysis. Literature data for their atomic properties are used. Owing to the wide variation of published ionization potentials, medians are used to estimate them. Vertical dendograms are used for classification on the basis of distances between the actinides in atomic-property space. The properties of actinium and lawrencium are furthest removed from the main group. Thorium and mendelevium exhibit individualized properties. A cluster based on the einsteinium-fermium pair is joined by californium.

  4. Advanced Aqueous Separation Systems for Actinide Partitioning

    SciTech Connect

    Nash, Ken; Martin, Leigh; Lumetta, Gregg

    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

  5. Analysis of large soil samples for actinides

    DOEpatents

    Maxwell, III; Sherrod L.

    2009-03-24

    A method of analyzing relatively large soil samples for actinides by employing a separation process that includes cerium fluoride precipitation for removing the soil matrix and precipitates plutonium, americium, and curium with cerium and hydrofluoric acid followed by separating these actinides using chromatography cartridges.

  6. Electrochemical decontamination system for actinide processing gloveboxes

    SciTech Connect

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

    1998-03-01

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

  7. Actinide geochemistry: from the molecular level to the real system.

    PubMed

    Geckeis, Horst; Rabung, Thomas

    2008-12-12

    Geochemical processes leading to either mobilization or retention of radionuclides in an aquifer system are significantly influenced by their interaction with rock, sediment and colloid surfaces. Therefore, a sound safety assessment of nuclear waste disposal requires the elucidation and quantification of those processes. State-of-the-art analytical techniques as e.g. laser- and X-ray spectroscopy are increasingly applied to study solid-liquid interface reactions to obtain molecular level speciation insight. We have studied the sorption of trivalent lanthanides and actinides onto aluminium oxides, hydroxides and purified clay minerals by the time-resolved laser fluorescence spectroscopy and X-ray-absorption spectroscopy. Chemical constitution and structure of surface bound actinides are proposed based on spectroscopic information. Open questions still remain with regard to the exact nature of mineral surface ligands and the mineral/water interface. Similarities of spectroscopic data obtained for M(III) sorbed onto gamma-alumina, and clay minerals suggest the formation of very comparable inner-sphere surface complexes such as S-O-An(III)(OH)x(2-x)(H2O)5-x at pH > 5. Those speciation data are found consistent with those predicted by surface complexation modelling. The applicability of data obtained for pure mineral phases to actinide sorption onto heterogeneously composed natural clay rock is examined by experiments and by geochemical modelling. Good agreement of experiment and model calculations is found for U(VI) and trivalent actinide/lanthanide sorption to natural clay rock. The agreement of spectroscopy, geochemical modelling and batch experiments with natural rock samples and purified minerals increases the reliability in model predictions. The assessment of colloid borne actinide migration observed in various laboratory and field studies calls for detailed information on actinide-colloid interaction. Kinetic stabilization of colloid bound actinides can be due

  8. Actinide geochemistry: from the molecular level to the real system.

    PubMed

    Geckeis, Horst; Rabung, Thomas

    2008-12-12

    Geochemical processes leading to either mobilization or retention of radionuclides in an aquifer system are significantly influenced by their interaction with rock, sediment and colloid surfaces. Therefore, a sound safety assessment of nuclear waste disposal requires the elucidation and quantification of those processes. State-of-the-art analytical techniques as e.g. laser- and X-ray spectroscopy are increasingly applied to study solid-liquid interface reactions to obtain molecular level speciation insight. We have studied the sorption of trivalent lanthanides and actinides onto aluminium oxides, hydroxides and purified clay minerals by the time-resolved laser fluorescence spectroscopy and X-ray-absorption spectroscopy. Chemical constitution and structure of surface bound actinides are proposed based on spectroscopic information. Open questions still remain with regard to the exact nature of mineral surface ligands and the mineral/water interface. Similarities of spectroscopic data obtained for M(III) sorbed onto gamma-alumina, and clay minerals suggest the formation of very comparable inner-sphere surface complexes such as S-O-An(III)(OH)x(2-x)(H2O)5-x at pH > 5. Those speciation data are found consistent with those predicted by surface complexation modelling. The applicability of data obtained for pure mineral phases to actinide sorption onto heterogeneously composed natural clay rock is examined by experiments and by geochemical modelling. Good agreement of experiment and model calculations is found for U(VI) and trivalent actinide/lanthanide sorption to natural clay rock. The agreement of spectroscopy, geochemical modelling and batch experiments with natural rock samples and purified minerals increases the reliability in model predictions. The assessment of colloid borne actinide migration observed in various laboratory and field studies calls for detailed information on actinide-colloid interaction. Kinetic stabilization of colloid bound actinides can be due

  9. Ultratrace analysis of transuranic actinides by laser-induced fluorescence

    DOEpatents

    Miller, S.M.

    1983-10-31

    Ultratrace quantities of transuranic actinides are detected indirectly by their effect on the fluorescent emissions of a preselected fluorescent species. Transuranic actinides in a sample are coprecipitated with a host lattice material containing at least one preselected fluorescent species. The actinide either quenches or enhances the laser-induced fluorescence of the preselected fluorescent species. The degree of enhancement or quenching is quantitatively related to the concentration of actinide in the sample.

  10. Ultratrace analysis of transuranic actinides by laser-induced fluorescence

    DOEpatents

    Miller, Steven M.

    1988-01-01

    Ultratrace quantities of transuranic actinides are detected indirectly by their effect on the fluorescent emissions of a preselected fluorescent species. Transuranic actinides in a sample are coprecipitated with a host lattice material containing at least one preselected fluorescent species. The actinide either quenches or enhances the laser-induced fluorescence of the preselected fluorescent species. The degree of enhancement or quenching is quantitatively related to the concentration of actinide in the sample.

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

    SciTech Connect

    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.

  12. Response of actinides to flux changes in high-flux systems

    SciTech Connect

    Sailor, W.C.

    1993-08-01

    When discussing the transmutation of actinides in accelerator-based transmutation of waste (ATW) systems, there has been some concern about the dynamics of the actinides under high transient fluxes. For the condition of a pure neptunium feed, it has been estimated that the {sup 238}Np/{sup 237}Np ratio increase due to an increasing flux may lead to an unstable, positive reactivity growth. In the analysis here a perturbation method is used to calculate the response of the entire set of actinides in a general way, that allows for more species than just Np. The time response of the system can be calculated, i.e., a plot of fuel composition and reactivity versus time after a change in flux can be made. The effects of fission products can also be included. The procedure extremely accurate on short time scales ({approximately}1000 sec) for the flux levels we contemplate. Calculational results indicate that the reactivity insertions are always smaller than previously estimated.

  13. Progress toward accurate high spatial resolution actinide analysis by EPMA

    NASA Astrophysics Data System (ADS)

    Jercinovic, M. J.; Allaz, J. M.; Williams, M. L.

    2010-12-01

    High precision, high spatial resolution EPMA of actinides is a significant issue for geochronology, resource geochemistry, and studies involving the nuclear fuel cycle. Particular interest focuses on understanding of the behavior of Th and U in the growth and breakdown reactions relevant to actinide-bearing phases (monazite, zircon, thorite, allanite, etc.), and geochemical fractionation processes involving Th and U in fluid interactions. Unfortunately, the measurement of minor and trace concentrations of U in the presence of major concentrations of Th and/or REEs is particularly problematic, especially in complexly zoned phases with large compositional variation on the micro or nanoscale - spatial resolutions now accessible with modern instruments. Sub-micron, high precision compositional analysis of minor components is feasible in very high Z phases where scattering is limited at lower kV (15kV or less) and where the beam diameter can be kept below 400nm at high current (e.g. 200-500nA). High collection efficiency spectrometers and high performance electron optics in EPMA now allow the use of lower overvoltage through an exceptional range in beam current, facilitating higher spatial resolution quantitative analysis. The U LIII edge at 17.2 kV precludes L-series analysis at low kV (high spatial resolution), requiring careful measurements of the actinide M series. Also, U-La detection (wavelength = 0.9A) requires the use of LiF (220) or (420), not generally available on most instruments. Strong peak overlaps of Th on U make highly accurate interference correction mandatory, with problems compounded by the ThMIV and ThMV absorption edges affecting peak, background, and interference calibration measurements (especially the interference of the Th M line family on UMb). Complex REE bearing phases such as monazite, zircon, and allanite have particularly complex interference issues due to multiple peak and background overlaps from elements present in the activation

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

    NASA Technical Reports Server (NTRS)

    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.

  15. Actinide Selective Systems for Environmental Extraction and Sensing Applications

    SciTech Connect

    Xianghong Wu; Mohan Singh Bharara; Tate, Brandon K.; Tonks, Stephen A.; Vilseck, Jonah Z.; Gorden, Anne Elizabeth Vivian

    2008-07-01

    The potential environmental and health concerns surrounding actinides and the use of nuclear fuels limits the acceptance of nuclear power by the public. This in turn, hinders the capability of this country to take advantage of nuclear power. Expanding our fundamental knowledge of actinide coordination chemistry will allow for the development of improved actinide sensors, new separations methods, or new means of radioactive waste remediation. We have designed and optimized a solution-phase parallel method for the synthesis of a library of symmetrical 2-quinoxalinol salens, Schiff-base type ligands with a 2-quinoxalinol incorporated into the salen backbone. This combines the rigid salen coordination framework with the quinoxaline properties that impart properties for use in colorimetric or fluorescent sensors. These have now been incorporated into organic soluble resins for metal extraction. (authors)

  16. ACTINIDE REMOVAL PROCESS SAMPLE ANALYSIS, CHEMICAL MODELING, AND FILTRATION EVALUATION

    SciTech Connect

    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.

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

    SciTech Connect

    Cao, Y.; Gohar, Y.

    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

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

    NASA Astrophysics Data System (ADS)

    Croce, M. P.; Bond, E. M.; Hoover, A. S.; Kunde, G. J.; Mocko, V.; Rabin, M. W.; Weisse-Bernstein, N. R.; Wolfsberg, L. E.; Bennett, D. A.; Hays-Wehle, J.; Schmidt, D. R.; Ullom, J. N.

    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.

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

    SciTech Connect

    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.

  20. Test of Actinide-Lanthanide Separation in an Aluminum-Based Pyrochemical System

    SciTech Connect

    Rault, Laurence; Heusch, Murielle; Allibert, Michel; Lemort, Florent; Deschane, Xavier; Boen, Roger

    2002-08-15

    The investigation of the actinide and lanthanide distribution between a liquid metal and a molten fluoride salt shows a significant increase of the separation coefficient by using an aluminum-based pyrochemical system instead of a zinc-based system. The obtained values partly depend on the LiF/AlF{sub 3} ratio and can reach more than 30 000 when AlF{sub 3} is in excess with regard to the formation of the cryolite (Li{sub 3} AlF{sub 6}). Furthermore, in the metal phase, the aluminum interacts with the lanthanides to a lesser extent than in other usual metallic solvents. This opens a new way to explore the feasibility of the separation of actinides and lanthanides in the field of nuclear fuel reprocessing.

  1. Novel Separation of Actinides

    SciTech Connect

    Mariella, R

    2011-02-17

    The separation of actinides and other elements of interest for nuclear forensics and threat reduction is currently performed using decades-old chemistries and ion-exchange columns. We propose to determine the technical feasibility of a novel method for separating actinide ions in solution. This method is based upon isotachophoresis (ITP), which has been applied in the purification of pharmaceuticals and other biochemical applications. This technique has the potential to separate inorganic ions more effectively than existing methods, which is key to analyzing very small samples. We will perform a quantitative assessment of the effectiveness of specific isotachophoretic approaches including predicting the physical and chemical properties, such as ion mobility, of inorganic ions under specific solvent conditions using a combination of ab initio calculations and semi-empirical methods. We expect to obtain a thorough understanding of the analytical systems parameters under which ITP is most effective for the separation of inorganic samples, including the influence of the double layer surrounding actinide ions, the Debye length for different ions and ion complexes, and Debye-Hueckel limits. Inorganic separations are key to nuclear forensics for countering terrorism and nuclear proliferation. If found to be feasible and potentially superior to currently used separation approaches, ITP could provide the conceptual basis for an improved means to separate samples of nuclear explosion debris for nuclear forensic analysis, in support of the Laboratory's missions in homeland and national security.

  2. Electrochemically-Modulated Separation and Mass Spectrometric Analysis of Actinides in Difficult Matrices

    SciTech Connect

    Duckworth, Douglas C.; Liezers, Martin; Lehn, Scott A.; Douglas, Matthew

    2009-01-01

    Electrochemically-modulated separations (EMS) are a straightforward means of isolating and pre-concentrating elements for on-line mass spectrometric analysis. Elements are accumulated at electrochemical working electrodes and subsequently released into a clean carrier solution for spectroscopic analysis. EMS can employ solely aqueous chemistry and uses electrochemical redox adjustment of oxidation state to “trigger” reversible chelation / complexation. Less tractable elements (e.g., uranium and plutonium), based on redox potentials, can therefore be extracted from difficult matrices following redox adjustment and chelation with electrode chelation sites. Simply put, separation is achieved by a small voltage step that is applied to the target electrode to turn “on” or “off” the specific actinide affinity of an electrode. This separation technology employs both redox and chelation chemistry to effect highly selective accumulation of target actinides, and results in element separation, matrix elimination and analyte preconcentration. Prior studies have developed protocols and preliminary insight into EMS processes for U and Pu. U and Pu are released upon oxidation and reduction, respectively, allowing complete separation due to widely divergent redox potentials. T The coupling of EMS on-line with ICP-MS for elemental and isotopic analysis of uranium and plutonium is presented, with a focus on analytical performance metrics and applicability to safeguards and process monitoring via nondestructive analyses.

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

    NASA Astrophysics Data System (ADS)

    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.

  4. Actinides-1981

    SciTech Connect

    Not Available

    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.

  5. Decay analysis of pre-actinide and trans-actinide nuclei formed using various projectiles on a 197Au target at ECN*=60 MeV

    NASA Astrophysics Data System (ADS)

    Grover, Neha; Kaur, Gurvinder; Sharma, Manoj K.

    2016-01-01

    The collective clusterization approach of the dynamical cluster decay model (DCM) has been applied to study the decay of odd mass nuclei 223Pa*, 215Fr*, 227Np*, and 233Am*, which are formed in heavy-ion-induced reactions. The aim of this study is to investigate the decay pattern and related behavior of these heavy mass nuclei formed in four distinct reactions involving different projectiles (with mass A =18 -36 ) induced on 197Au target nucleus. Further, in order to analyze the role of deformations, the calculations have been done by considering spherical choice of fragmentation as well as with inclusion of quadrupole (β2) deformation. For the heavy mass region, with fission being the dominant decay mode, an attempt has been made to investigate the effect of projectile mass in reference to fission decay patterns of the pre-actinide 215Fr* nucleus and the trans-actinide nuclei 227Np* 223Pa*, 223Am* and formed at common excitation energy, ECN*=60 MeV . Besides this, the shell closure effects and the role of orientation have been explored, which suggest the presence of a noncompound nucleus process such as quasifission (QF) for the odd mass nuclei under consideration. For both the compound nucleus and the noncompound nucleus processes, the results obtained using DCM are found to have nice agreement with experimental observations. The isotopic and isobaric analysis is also worked out so as to have a comprehensive idea about the dynamics involved.

  6. Computational Tools for Predictive Modeling of Properties in Complex Actinide Systems

    SciTech Connect

    Autschbach, Jochen; Govind, Niranjan; Atta Fynn, Raymond; Bylaska, Eric J.; Weare, John H.; de Jong, Wibe A.

    2015-03-30

    In this chapter we focus on methodological and computational aspects that are key to accurately modeling the spectroscopic and thermodynamic properties of molecular systems containing actinides within the density functional theory (DFT) framework. Our focus is on properties that require either an accurate relativistic all-electron description or an accurate description of the dynamical behavior of actinide species in an environment at finite temperature, or both. The implementation of the methods and the calculations discussed in this chapter were done with the NWChem software suite (Valiev et al. 2010). In the first two sections we discuss two methods that account for relativistic effects, the ZORA and the X2C Hamiltonian. Section 1.2.1 discusses the implementation of the approximate relativistic ZORA Hamiltonian and its extension to magnetic properties. Section 1.3 focuses on the exact X2C Hamiltonian and the application of this methodology to obtain accurate molecular properties. In Section 1.4 we examine the role of a dynamical environment at finite temperature as well as the presence of other ions on the thermodynamics of hydrolysis and exchange reaction mechanisms. Finally, Section 1.5 discusses the modeling of XAS (EXAFS, XANES) properties in realistic environments accounting for both the dynamics of the system and (for XANES) the relativistic effects.

  7. Thermochemistry of the actinides

    SciTech Connect

    Kleinschmidt, P.D.

    1993-10-01

    The measurement of equilibria by Knudsen effusion techniques and the enthalpy of formation of the actinide atoms is briefly discussed. Thermochemical data on the sublimation of the actinide fluorides is used to calculate the enthalpies of formation and entropies of the gaseous species. Estimates are made for enthalpies and entropies of the tetrafluorides and trifluorides for those systems where data is not available. The pressure of important species in the tetrafluoride sublimation processes is calculated based on this thermochemical data.

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

    NASA Astrophysics Data System (ADS)

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

    2011-09-01

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

  9. Double liquid membrane system for the removal of actinides and lanthanides from acidic nuclear wastes

    SciTech Connect

    Chiarizia, R.; Danesi, P.R.

    1985-01-01

    Supported liquid membranes (SLM), consisting of an organic solution of n-octyl-(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) and tributyl-phosphate (TBP) in decalin are able to perform selective separation and concentration of actinide and lanthanide ions from aqueous nitrate feed solutions and synthetic nuclear wastes. In the membrane process a possible strip solution is a mixture of formic acid and hydroxylammonium formate (HAF). The effectiveness of this strip solution is reduced and eventually nullified by the simultaneous transfer through the SLM of nitric acid which accumulates in the strip solution. A possible way to overcome this drawback is to make use of a second SLM consisting of a primary amine which is able to extract only HNO/sub 3/ from the strip solution. In this work the results obtained by experimentally studying the membrane system: synthetic nuclear waste/CMPO-TBP membrane/HCOOH-HAF strip solution/primary amine membrane/NaOH solution, are reported. They show that the use of a second liquid membrane is effective in controlling the HNO/sub 3/ concentration in the strip solution, thus allowing the actinide and lanthanide ions removal from the feed solution to proceed to completion. 15 refs., 10 figs., 1 tab.

  10. Double liquid membrane system for the removal of actinides and lanthanides from acidic nuclear wastes

    SciTech Connect

    Chiarizia, R.; Danesi, P.R.

    1987-01-01

    Supported liquid membranes (SLM), consisting of an organic solution of n-octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) and tributyl-phosphate (TBP) in decalin are able to perform selective separation and concentration of actinide and lanthanide ions from aqueous nitrate feed solutions and synthetic nuclear wastes. In the membrane process a possible strip solution is a mixture of formic acid and hydroxylammonium formate (HAF). The effectiveness of this strip solution is reduced and eventually nullified by the simultaneous transfer through the SLM of HNO3 which accumulates in the strip solution. A possible way to overcome this drawback is to make use of a second SLM consisting of a primary amine which is able to extract only HNO3 from the strip solution. In this work the results obtained by experimentally studying the membrane system: synthetic nuclear waste/CMPO-TBP membrane/HCOOH-HAF strip solution/primary amine membrane/NaOH solution, are reported. They show that the use of a second liquid membrane is effective in controlling the HNO3 concentration in the strip solution, thus allowing the actinide and lanthanide ions removal from the feed solution to proceed to completion.

  11. High Precision Isotopic Analysis of Actinide Bearing Materials: Performance of a New Generation of Purpose Built Actinide Multi-Collector ICPMS Instruments

    SciTech Connect

    Eiden, Gregory C.; Duffin, Andrew M.; Liezers, Martin; Ward, Jesse D.; Robinson, John W.; Hart, Garret L.; Pratt, Sandra H.; Springer, Kellen WE; Carman, April J.; Duckworth, Douglas C.

    2014-11-14

    Recently, a new class of multi-collector inductively coupled plasma mass spectrometers (MC-ICPMS) has been introduced commercially that includes detector arrays purpose built for actinide measurements. These detector arrays significantly enhance the data quality possible for applications encountered in nuclear forensics. Two such instruments are described in this paper, the NeptunePlusTM, developed by Thermo-Fisher (Bremen, Germany), and the NuPlasma2, developed by Nu Instruments (Wrexham, UK). Research results are presented that have been obtained by the authors using the first commercial NeptunePlusTM. This paper also presents performance characteristics and results for traditional liquid introduction, including a means for ultra-trace detection via electrochemical separation prior to solution nebulization, as well as solid sample introduction with femtosecond-laser ablation. We also discuss the advantages and limitations of the current systems for detection of the transient signals associated with these two methods for introducing sample into the plasma.

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

    PubMed

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

    2015-06-01

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

  13. Model Analysis of Low-Level Actinide Waste Disposal in Deep Boreholes

    NASA Astrophysics Data System (ADS)

    Glascoe, L. G.; Wolfsberg, A. V.

    2001-12-01

    Deep borehole disposal is considered as a possible mechanism for the safe removal of Greater Than Class C (GTCC) low level actinide waste (Am-241, Pu-239, and Pu-238). Of the three actinides in GTCC waste, only Pu-239 has a half-life greater than 500 years and, thus, will have the longest environmental presence. However, Am-241 and Pu-238 have the potential to create most of the heat associated with GTCC waste disposal in deep boreholes. Therefore, this study considers the nonisothermal release and subsequent migration toward a pumping well of the most persistent radionuclide, Pu-239, from a deep emplacement borehole taking into account the heat created by decay of all three actinides. The Finite-Element Heat- and Mass-Transfer code, FEHM, is employed to simulate three-dimensional, non-isothermal flow and solute transport using particle tracking. Multiple scenarios considering various source emplacement depths, aquifer properties, and hydraulic conditions are evaluated in a sensitivity analysis that seeks to demonstrate competing and offsetting processes affecting the concentration of Pu-239 in the pumped well 100 m down gradient from the borehole source. In general, lower groundwater fluxes, associated with lower gradients and/or lower aquifer permeabilities, lead to less dissolution of the source waste. However, conditions of decreasing groundwater flux also create larger sized capture zones by the pumping well, thus escalating the likelihood of pumping contaminants originating from a source deeper than the pumping well. Retardation by sorption of Pu-239, both in alluvial aquifers and following diffusion from fractures in a tuff aquifer, plays an important role both in delaying radionuclide migration and in reducing the peak aqueous concentration at the pumping well. This work was performed under the auspices of the U.S. Department of Energy by University of California Lawrence Livermore National Laboratory under contract No. W-7405-Eng-48. This work was

  14. Novel drug delivery systems for actinides (uranium and plutonium) decontamination agents.

    PubMed

    Fattal, Elias; Tsapis, Nicolas; Phan, Guillaume

    2015-08-01

    The possibility of accidents in the nuclear industry or of nuclear terrorist attacks makes the development of new decontamination strategies crucial. Among radionuclides, actinides such as uranium and plutonium and their different isotopes are considered as the most dangerous contaminants, plutonium displaying mostly a radiological toxicity whereas uranium exhibits mainly a chemical toxicity. Contamination occurs through ingestion, skin or lung exposure with subsequent absorption and distribution of the radionuclides to different tissues where they induce damaging effects. Different chelating agents have been synthesized but their efficacy is limited by their low tissue specificity and high toxicity. For these reasons, several groups have developed smart delivery systems to increase the local concentration of the chelating agent or to improve its biodistribution. The aim of this review is to highlight these strategies.

  15. Understanding the Chemistry of the Actinides in HL Waste Tank Systems: Actinide Speciation in Oxalic Acid Solutions in the Presence of Significant Quantities of Aluminum, Iron, and Manganese

    SciTech Connect

    Clark, Sue

    2006-07-30

    The overall goal of this research plan is to provide a thermodynamic basis for describing actinide speciation over a range of tank-like conditions, including elevated temperature, elevated OH- concentrations, and the presence of various organic ligands. With support from DOE's EMSP program, we have made significant progress towards measuring thermodynamic parameters for actinide complexation as a function of temperature. We have used the needs of the ESP modelers to guide our work to date, and we have made important progress defining the effect of temperature for actinide complexation by organic, and for hydrolysis of the hexa- and pentvalent oxidation states.

  16. Minior Actinide Doppler Coefficient Measurement Assessment

    SciTech Connect

    Nolan E. Hertel; Dwayne Blaylock

    2008-04-10

    The "Minor Actinide Doppler Coefficient Measurement Assessment" was a Department of Energy (DOE) U-NERI funded project intended to assess the viability of using either the FLATTOP or the COMET critical assembly to measure high temperature Doppler coefficients. The goal of the project was to calculate using the MCNP5 code the gram amounts of Np-237, Pu-238, Pu-239, Pu-241, AM-241, AM-242m, Am-243, and CM-244 needed to produce a 1E-5 in reactivity for a change in operating temperature 800C to 1000C. After determining the viability of using the assemblies and calculating the amounts of each actinide an experiment will be designed to verify the calculated results. The calculations and any doncuted experiments are designed to support the Advanced Fuel Cycle Initiative in conducting safety analysis of advanced fast reactor or acceoerator-driven transmutation systems with fuel containing high minor actinide content.

  17. Fission-product data analysis from actinide samples exposed in the Dounreay Prototype Fast Reactor

    SciTech Connect

    Murphy, B.D.; Dickens, J.K.; Walker, R.L.; Newton, T.D.

    1994-12-31

    Since 1979 a cooperative agreement has been in effect between the United States and the United Kingdom to investigate the irradiation of various actinide species placed in the core of the Dounreay Prototype Fast Reactor (PFR). The irradiated species were isotopes of thorium, protactinium, uranium, neptunium, plutonium, americium, and curium. A set of actinide samples (mg quantities) was exposed to about 490 effective full power days (EFPD) of reactor operations. The fission-product results are reported here. The actinide results will be report elsewhere.

  18. Aqueous Biphasic Systems Based on Salting-Out Polyethylene Glycol or Ionic Solutions: Strategies for Actinide or Fission Product Separations

    SciTech Connect

    Rogers, Robin D.; Gutowski, Keith E.; Griffin, Scott T.; Holbrey, John D.

    2004-03-29

    Aqueous biphasic systems can be formed by salting-out (with kosmotropic, waterstructuring salts) water soluble polymers (e.g., polyethylene glycol) or aqueous solutions of a wide range of hydrophilic ionic liquids based on imidazolium, pyridinium, phosphonium and ammonium cations. The use of these novel liquid/liquid biphases for separation of actinides or other fission products associated with nuclear wastes (e.g., pertechnetate salts) has been demonstrated and will be described in this presentation.

  19. Strongly Correlated Electron Behaviors and Heavy Fermions in Anomalous Rare-earth and actinide Systems

    NASA Astrophysics Data System (ADS)

    Coqblin, B.

    2006-07-01

    After an introduction on the different cases of anomalous rare-earth systems, we start to present the case of intermediate valence, with the example of the phase diagram of Cerium and the study of the Anderson Hamiltonian. Then, we discuss the Kondo effect for a single impurity, with a perturbation calculation above the Kondo temperature and the exact single-impurity solution showing a heavy fermion behaviour below it. Then, the Kondo effect for Ce, Yb and other anomalous rare-earth impurities and their different transport properties arc discussed, with in particular a description of the Schrieffer-Wolff transformation and of the "Coqblin-Schrieffer" Hamiltonian without and with crystalline field effects. The properties of actinide metals and compounds are also discussed and both the spin fluctuation model applied to Plutonium or Neptunium metals or compounds and the undercreened Kondo-lattice model applied to Uranium Kondo and ferromagnetic compounds are presented. The Kondo-lattice problem is also discussed, with a special emphasis on the Doniach diagram, the mean-field approximations, the competition between the Kondo effect and the magnetic order, the spin glass-Kondo competition and the multi-channel Kondo effect. A brief summary of the superconductivity occurring in Ce, U or even Pu systems is finally presented.

  20. Fundamental aspects of actinide-zirconium pyrochlore oxides: Systematic comparison of the Pu, Am, Cm, Bk and Cf systems

    NASA Astrophysics Data System (ADS)

    Haire, R. G.; Raison, P. E.

    2000-07-01

    Zirconium- and hafnium-based oxide materials have gained attraction for various nuclear applications. These materials have features in common with one of the early, well-publicized inorganic ceramics for immobilizing nuclear waste. Our interests have addressed the fundamental structural and chemical properties of these oxide systems. We pursued both the crystal chemical constraints of the oxide matrices, as well as the importance of the chemistry of the f-elements. By incorporating five actinide elements in our studies, we were able to compare systematically the materials science of these materials with the fundamental chemistry and electronic configurations of these actinides employed. It is expected that this basic information will be useful technologically in the realm of tailor-made materials for different applications.

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

    SciTech Connect

    O'Hara, David

    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.

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

    NASA Astrophysics Data System (ADS)

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

    2014-09-01

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

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

    SciTech Connect

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

    2014-09-30

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

  4. Actinide partitioning-transmutation program final report. VII. Long-term risk analysis of the geologic repository

    SciTech Connect

    Logan, S.E.; Conarty, R.L.; Ng, H.S.; Rahal, L.J.; Shirley, C.G.

    1980-09-01

    This report supports the overall assessment by Oak Ridge National Laboratory of actinide partitioning and transmutation by providing an analysis of the long-term risks associated with the terminal storage of wastes from a fuel cycle which incorporates partitioning and transmutation (P-T) and wastes from a cycle which does not. The system model and associated computer code, called AMRAW (Assessment Method for Radioactive Waste), are used for the analysis and are applied to the Los Medanos area in southeastern New Mexico. Because a conservative approach is used throughout, calculated results are believed to be consistently higher than reasonable expectations from actual disruptive incidents at the site and therefore are not directly suited for comparison with other analyses of the particular geologic location. The assessment is made with (1) the probabilistic, or risk, mode that uses combinations of reasonable possible release incidents with their probability of occurrence distributed and applied throughout the assessment period, and (2) the consequence mode that forces discrete release events to occur at specific times. An assessment period of 1 million years is used. The principal results are: (1) In all but the expulsive modes, /sup 99/Tc and /sup 129/I completely dominate cumulative effects based on their transport to man through leaching and movement with groundwater, effecting about 33,000 health effects (deaths) over the 1 million years; (2) P-T has only limited effectiveness in reducing long-term risk from a radionuclide waste repository under the conditions studied, and such effectiveness is essentially confined to the extremely unlikely (probability of occurrence 10/sup -12//year) expulsive events; (3) Removal or immobilization of /sup 99/Tc and /sup 129/I might provide benefits sufficiently tangible to warrant special consideration.

  5. Preliminary Calculational Analysis of the Actinide Samples from FP-4 Exposed in the Dounreay Prototype Fast Reactor

    SciTech Connect

    Murphy, B.D.

    1993-01-01

    This report discusses the current status of results from an extensive experiment on the irradiation of selected actinides in a fast reactor. These actinides ranged from thorium to curium. They were irradiated in the core of the Dounreay Prototype Fast Reactor. Rates for depletion, transmutation, and fission-product generation were experimentally measured, and, in turn, were calculated using current cross-section and fission-yield data. Much of the emphasis is on the comparison between experimental and calculated values for both actinide and fission-product concentrations. Some of the discussion touches on the adequacy of current cross-section and fission-yield data. However, the main purposes of the report are (1) to collect in one place the most recent experimental and calculated data, (2) to discuss the comparisons between the experimental and calculated results, (3) to discuss each sample that was irradiated giving details of any adjustments needed or specific problems encountered, and (4) to give a chronology of the analysis as it pertained to the set of samples (referred to as FP-4 samples) that constitutes the most extensively irradiated and final set. The results and trends reported here, together with those discussions touching on current knowledge about cross sections and fission yields, are intended to serve as a starting point for further analysis. In general, these results are encouraging with regard to the adequacy of much of the currently available nuclear data in this region of the periodic table. But there are some cases where adjustments and improvements can be suggested. However, the application of these results in consolidating current cross-section and fission-yield data must await further analysis.

  6. Preliminary calculational analysis of the actinide samples from FP-4 exposed in the Dounreay Prototype Fast Reactor

    SciTech Connect

    Murphy, B.D.; Raman, S.; Newton, T.D.

    1996-12-01

    This report discusses the current status of results from an extensive experiment on the irradiation of selected actinides in a fast reactor. These actinides ranged from thorium to curium. They were irradiated in the core of the Dounreay Prototype Fast Reactor. Rates for depletion, transmutation, and fission-product generation were experimentally measured, and, in turn, were calculated using current cross-section and fission-yield data. Much of the emphasis is on the comparison between experimental and calculated values for both actinide and fission-product concentrations. Some of the discussion touches on the adequacy of current cross-section and fission-yield data. However, the main purposes of the report are: to collect in one place the most recent yield data, to discuss the comparisons between the experimental and calculated results, to discuss each sample that was irradiated giving details of any adjustments needed or specific problems encountered, and to give a chronology of the analysis as it pertained to the set of samples (referred to as FP-4 samples) that constitutes the most extensively irradiated and final set. The results and trends reported here, together with those discussions touching on current knowledge about cross sections and fission yields, are intended to serve as a starting point for further analysis. In general, these results are encouraging with regard to the adequacy of much of the currently available nuclear data in this region of the periodic table. But there are some cases where adjustments and improvements can be suggested. However, the application of these results in consolidating current cross-section and fission-yield data must await further analysis.

  7. Micro-Analysis of Actinide Minerals for Nuclear Forensics and Treaty Verification

    SciTech Connect

    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.

  8. Synthesis and characterization of a tetrathiafulvalene-salphen actinide complex.

    PubMed

    Bejger, Christopher; Tian, Yong-Hui; Barker, Beau J; Boland, Kevin S; Scott, Brian L; Batista, Enrique R; Kozimor, Stosh A; Sessler, Jonathan L

    2013-05-21

    A new tetrathiafulvalene-salphen uranyl complex has been prepared. The system was designed to study the electronic coupling between actinides and a redox active ligand framework. Theoretical and experimental methods--including DFT calculations, single crystal X-ray analysis, cyclic voltammetry, NMR and IR spectroscopies--were used to characterize this new uranyl complex.

  9. Environmental speciation of actinides.

    PubMed

    Maher, Kate; Bargar, John R; Brown, Gordon E

    2013-04-01

    Although minor in abundance in Earth's crust (U, 2-4 ppm; Th, 10-15 ppm) and in seawater (U, 0.003 ppm; Th, 0.0007 ppm), light actinides (Th, Pa, U, Np, Pu, Am, and Cm) are important environmental contaminants associated with anthropogenic activities such as the mining and milling of uranium ores, generation of nuclear energy, and storage of legacy waste resulting from the manufacturing and testing of nuclear weapons. In this review, we discuss the abundance, production, and environmental sources of naturally occurring and some man-made light actinides. As is the case with other environmental contaminants, the solubility, transport properties, bioavailability, and toxicity of actinides are dependent on their speciation (composition, oxidation state, molecular-level structure, and nature of the phase in which the contaminant element or molecule occurs). We review the aqueous speciation of U, Np, and Pu as a function of pH and Eh, their interaction with common inorganic and organic ligands in natural waters, and some of the common U-containing minerals. We also discuss the interaction of U, Np, Pu, and Am solution complexes with common Earth materials, including minerals, colloids, gels, natural organic matter (NOM), and microbial organisms, based on simplified model system studies. These surface interactions can inhibit (e.g., sorption to mineral surfaces, formation of insoluble biominerals) or enhance (e.g., colloid-facilitated transport) the dispersal of light actinides in the biosphere and in some cases (e.g., interaction with dissimilatory metal-reducing bacteria, NOM, or Mn- and Fe-containing minerals) can modify the oxidation states and, consequently, the behavior of redox-sensitive light actinides (U, Np, and Pu). Finally, we review the speciation of U and Pu, their chemical transformations, and cleanup histories at several U.S. Department of Energy field sites that have been used to mill U ores, produce fissile materials for reactors and weapons, and store

  10. Environmental speciation of actinides.

    PubMed

    Maher, Kate; Bargar, John R; Brown, Gordon E

    2013-04-01

    Although minor in abundance in Earth's crust (U, 2-4 ppm; Th, 10-15 ppm) and in seawater (U, 0.003 ppm; Th, 0.0007 ppm), light actinides (Th, Pa, U, Np, Pu, Am, and Cm) are important environmental contaminants associated with anthropogenic activities such as the mining and milling of uranium ores, generation of nuclear energy, and storage of legacy waste resulting from the manufacturing and testing of nuclear weapons. In this review, we discuss the abundance, production, and environmental sources of naturally occurring and some man-made light actinides. As is the case with other environmental contaminants, the solubility, transport properties, bioavailability, and toxicity of actinides are dependent on their speciation (composition, oxidation state, molecular-level structure, and nature of the phase in which the contaminant element or molecule occurs). We review the aqueous speciation of U, Np, and Pu as a function of pH and Eh, their interaction with common inorganic and organic ligands in natural waters, and some of the common U-containing minerals. We also discuss the interaction of U, Np, Pu, and Am solution complexes with common Earth materials, including minerals, colloids, gels, natural organic matter (NOM), and microbial organisms, based on simplified model system studies. These surface interactions can inhibit (e.g., sorption to mineral surfaces, formation of insoluble biominerals) or enhance (e.g., colloid-facilitated transport) the dispersal of light actinides in the biosphere and in some cases (e.g., interaction with dissimilatory metal-reducing bacteria, NOM, or Mn- and Fe-containing minerals) can modify the oxidation states and, consequently, the behavior of redox-sensitive light actinides (U, Np, and Pu). Finally, we review the speciation of U and Pu, their chemical transformations, and cleanup histories at several U.S. Department of Energy field sites that have been used to mill U ores, produce fissile materials for reactors and weapons, and store

  11. Analysis of incident-energy dependence of delayed neutron yields in actinides

    SciTech Connect

    Nasir, Mohamad Nasrun bin Mohd Metorima, Kouhei Ohsawa, Takaaki Hashimoto, Kengo

    2015-04-29

    The changes of delayed neutron yields (ν{sub d}) of Actinides have been analyzed for incident energy up to 20MeV using realized data of precursor after prompt neutron emission, from semi-empirical model, and delayed neutron emission probability data (P{sub n}) to carry out a summation method. The evaluated nuclear data of the delayed neutron yields of actinide nuclides are still uncertain at the present and the cause of the energy dependence has not been fully understood. In this study, the fission yields of precursor were calculated considering the change of the fission fragment mass yield based on the superposition of fives Gaussian distribution; and the change of the prompt neutrons number associated with the incident energy dependence. Thus, the incident energy dependent behavior of delayed neutron was analyzed.The total number of delayed neutron is expressed as ν{sub d}=∑Y{sub i} • P{sub ni} in the summation method, where Y{sub i} is the mass yields of precursor i and P{sub ni} is the delayed neutron emission probability of precursor i. The value of Y{sub i} is derived from calculation of post neutron emission mass distribution using 5 Gaussian equations with the consideration of large distribution of the fission fragments. The prompt neutron emission ν{sub p} increases at higher incident-energy but there are two different models; one model says that the fission fragment mass dependence that prompt neutron emission increases uniformly regardless of the fission fragments mass; and the other says that the major increases occur at heavy fission fragments area. In this study, the changes of delayed neutron yields by the two models have been investigated.

  12. Actinide sulfite tetrahydrate and actinide oxysulfite tetrahydrate

    SciTech Connect

    Baugh, D.; Watt, G.

    1980-07-08

    A compound is prepared that comprises an actinide sulfite tetrahydrate selected from the group consisting of uranium (IV) sulfite tetrahydrate and plutonium (IV) sulfite tetrahydrate. A compound is also prepared that comprises an actinide oxysulfite tetrahydrate selected from the group consisting of uranium (IV) oxysulfite tetrahydrate and plutonium (IV) oxysulfite tetrahydrate

  13. Kinetics of actinide complexation reactions

    SciTech Connect

    Nash, K.L.; Sullivan, J.C.

    1997-09-01

    Though the literature records extensive compilations of the thermodynamics of actinide complexation reactions, the kinetics of complex formation and dissociation reactions of actinide ions in aqueous solutions have not been extensively investigated. In light of the central role played by such reactions in actinide process and environmental chemistry, this situation is somewhat surprising. The authors report herein a summary of what is known about actinide complexation kinetics. The systems include actinide ions in the four principal oxidation states (III, IV, V, and VI) and complex formation and dissociation rates with both simple and complex ligands. Most of the work reported was conducted in acidic media, but a few address reactions in neutral and alkaline solutions. Complex formation reactions tend in general to be rapid, accessible only to rapid-scan and equilibrium perturbation techniques. Complex dissociation reactions exhibit a wider range of rates and are generally more accessible using standard analytical methods. Literature results are described and correlated with the known properties of the individual ions.

  14. Actinide-ion sensor

    DOEpatents

    Li, Shelly X; Jue, Jan-fong; Herbst, Ronald Scott; Herrmann, Steven Douglas

    2015-01-13

    An apparatus for the real-time, in-situ monitoring of actinide-ion concentrations. A working electrolyte is positioned within the interior of a container. The working electrolyte is separated from a reference electrolyte by a separator. A working electrode is at least partially in contact with the working electrolyte. A reference electrode is at least partially in contact with the reference electrolyte. A voltmeter is electrically connected to the working electrode and the reference electrode. The working electrolyte comprises an actinide-ion of interest. The separator is ionically conductive to the actinide-ion of interest. The separator comprises an actinide, Zr, and Nb. Preferably, the actinide of the separator is Am or Np, more preferably Pu. In one embodiment, the actinide of the separator is the actinide of interest. In another embodiment, the separator further comprises P and O.

  15. Preliminary considerations concerning actinide solubilities

    SciTech Connect

    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.

  16. Actinide co-conversion by internal gelation

    SciTech Connect

    Robisson, Anne-Charlotte; Dauby, Jacques; Dumont-Shintu, Corinne; Machon, Estelle; Grandjean, Stephane

    2007-07-01

    Suitable microstructures and homogenous microspheres of actinide compounds are of interest for future nuclear fuel or transmutation target concepts to prevent the generation and dispersal of actinide powder. Sol-gel routes are being investigated as one of the possible solutions for producing these compounds. Preliminary work is described involving internal gelation to synthesize mixed compounds including minor actinides, particularly mixed actinide or mixed actinide-inert element compounds. A parameter study is discussed to highlight the importance of the initial broth composition for obtaining gel microspheres without major defects (cracks, craters, etc.). In particular, conditions are defined to produce gel beads from Zr(IV)/Y(III)/Ce(III) or Zr(IV)/An(III) systems. After gelation, the heat treatment of these microspheres is described for the purpose of better understanding the formation of cracks after calcination and verifying the effective synthesis of an oxide solid-solution. (authors)

  17. Actinide extraction methods

    DOEpatents

    Peterman, Dean R [Idaho Falls, ID; Klaehn, John R [Idaho Falls, ID; Harrup, Mason K [Idaho Falls, ID; Tillotson, Richard D [Moore, ID; Law, Jack D [Pocatello, ID

    2010-09-21

    Methods of separating actinides from lanthanides are disclosed. A regio-specific/stereo-specific dithiophosphinic acid having organic moieties is provided in an organic solvent that is then contacted with an acidic medium containing an actinide and a lanthanide. The method can extend to separating actinides from one another. Actinides are extracted as a complex with the dithiophosphinic acid. Separation compositions include an aqueous phase, an organic phase, dithiophosphinic acid, and at least one actinide. The compositions may include additional actinides and/or lanthanides. A method of producing a dithiophosphinic acid comprising at least two organic moieties selected from aromatics and alkyls, each moiety having at least one functional group is also disclosed. A source of sulfur is reacted with a halophosphine. An ammonium salt of the dithiophosphinic acid product is precipitated out of the reaction mixture. The precipitated salt is dissolved in ether. The ether is removed to yield the dithiophosphinic acid.

  18. Research in actinide chemistry

    SciTech Connect

    Choppin, G.R.

    1993-01-01

    This research studies the behavior of the actinide elements in aqueous solution. The high radioactivity of the transuranium actinides limits the concentrations which can be studied and, consequently, limits the experimental techniques. However, oxidation state analogs (trivalent lanthanides, tetravalent thorium, and hexavalent uranium) do not suffer from these limitations. Behavior of actinides in the environment are a major USDOE concern, whether in connection with long-term releases from a repository, releases from stored defense wastes or accidental releases in reprocessing, etc. Principal goal of our research was expand the thermodynamic data base on complexation of actinides by natural ligands (e.g., OH[sup [minus

  19. Isotope ratio analysis of actinides, fission products, and geolocators by high-efficiency multi-collector thermal ionization mass spectrometry

    NASA Astrophysics Data System (ADS)

    Bürger, S.; Riciputi, L. R.; Bostick, D. A.; Turgeon, S.; McBay, E. H.; Lavelle, M.

    2009-09-01

    A ThermoFisher "Triton" multi-collector thermal ionization mass spectrometer (MC-TIMS) was evaluated for trace and ultra-trace level isotope ratio analysis of actinides (uranium, plutonium, and americium), fission products and geolocators (strontium, cesium, and neodymium). Total efficiencies (atoms loaded to ions detected) of up to 0.5-2% for U, Pu, and Am, and 1-30% for Sr, Cs, and Nd can be reported employing resin bead load techniques onto flat ribbon Re filaments or resin beads loaded into a millimeter-sized cavity drilled into a Re rod. This results in detection limits of <0.1 fg (104 atoms to 105 atoms) for 239-242+244Pu, 233+236U, 241-243Am, 89,90Sr, and 134,135,137Cs, and <=1 pg for natural Nd isotopes (limited by the chemical processing blank) using a secondary electron multiplier (SEM) or multiple-ion counters (MICs). Relative standard deviations (RSD) as small as 0.1% and abundance sensitivities of 1 × 106 or better using a SEM are reported here. Precisions of RSD [approximate]0.01-0.001% using a multi-collector Faraday cup array can be achieved at sub-nanogram concentrations for strontium and neodymium and are suitable to gain crucial geolocation information. The analytical protocols reported herein are of particular value for nuclear forensic and nuclear safeguard applications.

  20. Chemistry of lower valent actinide halides

    SciTech Connect

    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.

  1. Actinide recovery process

    DOEpatents

    Muscatello, Anthony C.; Navratil, James D.; Saba, Mark T.

    1987-07-28

    Process for the removal of plutonium polymer and ionic actinides from aqueous solutions by absorption onto a solid extractant loaded on a solid inert support such as polystyrenedivinylbenzene. The absorbed actinides can then be recovered by incineration, by stripping with organic solvents, or by acid digestion. Preferred solid extractants are trioctylphosphine oxide and octylphenyl-N,N-diisobutylcarbamoylmethylphosphine oxide and the like.

  2. Thermodynamic Properties of Actinides and Actinide Compounds

    NASA Astrophysics Data System (ADS)

    Konings, Rudy J. M.; Morss, Lester R.; Fuger, Jean

    The necessity of obtaining accurate thermodynamic quantities for the actinide elements and their compounds was recognized at the outset of the Manhattan Project, when a dedicated team of scientists and engineers initiated the program to exploit nuclear energy for military purposes. Since the end of World War II, both fundamental and applied objectives have motivated a great deal of further study of actinide thermodynamics. This chapter brings together many research papers and critical reviews on this subject. It also seeks to assess, to systematize, and to predict important properties of the actinide elements, ions, and compounds, especially for species in which there is significant interest and for which there is an experimental basis for the prediction.

  3. Method for preparing actinide nitrides

    DOEpatents

    Bryan, G.H.; Cleveland, J.M.; Heiple, C.R.

    1975-12-01

    Actinide nitrides, and particularly plutonium and uranium nitrides, are prepared by reacting an ammonia solution of an actinide compound with an ammonia solution of a reactant or reductant metal, to form finely divided actinide nitride precipitate which may then be appropriately separated from the solution. The actinide nitride precipitate is particularly suitable for forming nuclear fuels.

  4. Actinide partitioning-transmutation program final report. VI. Short-term risk analysis of reprocessing, refabrication, and transportation: summary

    SciTech Connect

    Fullwood, R.; Jackson, R.

    1980-03-01

    A Partitioning-Transmutation (PT) fuel cycle is being compared to a Reference cycle employing conventional fuel-material recovery methods. The PT cycle uses enhanced recovery methods so that most of the long-lived actinides are recycled to nuclear power plants and transmuted thereby reducing the waste toxicity. This report compares the two fuel cycles on the basis of the short-term radiological and nonradiological risks. The accidental radiological risk to the public is analyzed by estimating the probabilities of sets of accidents; the consequences are calculated using the risk, which is RAC code. Routine radiological risks to the public are estimated from the calculated release amounts, also using the CRAC code. Radiological occupational risks are determined from prior experience, projected standards, and estimates of accident risk. Nonradiological risks are calculated from the number of personnel involved, historical experience, and epidemiological studies. Result of this analysis is that the short-term risk of PT is 2.9 times greater than that of the Reference cycle, primarily due to the larger amount of industry. The nonradiological risk which is about 150 times greater than the radiological risk. If the radiological risk is consdered alone, the ratio of PT to Reference risk is 3, composed as follows: radiological operations affecting the public 5, radiological operations affecting the workers 1.7, and radiological accidents affecting the public 1.4, all in the order of decreasing risk. The absolute risk as estimated for the fuel cycle portions considered in this report is 0.91 fatality/GWe-year for the PT cycle and 0.34 fatality/GWe-year for the reference cycle; this compares with 1.5 for nuclear and 150 for coal. All of the risks assumed here are associated with the production of one billion watts of electricity (GWe) per year.

  5. Actinide partitioning-transmutation program final report. VI. Short-term risk analysis of reprocessing, refabrication, and transportation: appendix

    SciTech Connect

    Fullwood, R.R.; Jackson, R.

    1980-01-01

    The Chemical Technology Division of the Oak Ridge National Laboratory has prepared a set of documents that evaluate a Partitioning-Transmutation (PT) fuel cycle relative to a Reference cycle employing conventional fuel-material recovery methods. The PT cycle uses enhanced recovery methods so that most of the long-lived actinides are recycled to nuclear power plants and transmuted to shorter-lived materials, thereby reducing the waste toxicity. This report compares the two fuel cycles on the basis of the short-term radiological and nonradiological risks they present to the public and to workers. The accidental radiological risk to the public is analyzed by estimating the probabilities of sets of accidents; the consequences are calculated using the CRAC code appropriately modified for the material composition. Routine radiological risks to the public are estimated from the calculated release amounts; the effects are calculated using the CRAC code. Radiological occupational risks are determined from prior experience, projected standards, and estimates of accident risk. Nonradiological risks are calculated from the number of personnel involved, historical experience, and epidemiological studies. The result of this analysis is that the short-term risk of PT is 2.9 times greater than that of the Reference cycle, primarily due to the larger amount of industry. This conclusion is strongly dominated by the nonradiological risk, which is about 150 times greater than the radiological risk. The absolute risk as estimated for the fuel cycle portions considered in this report is 0.91 fatalities/GWe-year for the PT cycle and 0.34 fatalities/GWe-year for the Reference cycle. This should be compared with Inhaber's estimate of 1.5 for nuclear and 150 for coal. All of the risks assumed here are associated with the production of one billion watts of electricity (GWe) per year.

  6. PREFACE: Actinides 2009

    NASA Astrophysics Data System (ADS)

    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)

  7. Partitioning and Leaching Behavior of Actinides and Rare Earth Elements in a Zirconolite- Bearing Hydrothermal Vein System

    SciTech Connect

    Payne, Timothy E.; Hart, Kaye P.; Lumpkin, Gregory R.; McGlinn, Peter J.; Giere, Reto

    2007-07-01

    Chemical extraction techniques and scanning electron microscopy were used to study the distribution and behavior of actinides and rare earth elements (REE) in hydrothermal veins at Adamello (Italy). The six samples discussed in this paper were from the phlogopite zone, which is one of the major vein zones. The samples were similar in their bulk chemical composition, mineralogy, and leaching behavior of major elements (determined by extraction with 9 M HCl). However, there were major differences in the extractability of REE and actinides. The most significant influence on the leaching characteristics appears to be the amounts of U, Th and REE incorporated in resistant host phases (zirconolite and titanite) rather than readily leached phases (such as apatite). Uranium and Th are very highly enriched in zirconolite grains. Actinides were more readily leached from samples with a higher content of U and Th, relative to the amount of zirconium. The results show that REE and actinides present in chemically resistant host minerals can be retained under aggressive leaching conditions. (authors)

  8. Actinides in the Geosphere

    NASA Astrophysics Data System (ADS)

    Runde, Wolfgang; Neu, Mary P.

    Since the 1950s actinides have been used to benefit industry, science, health, and national security. The largest industrial application, electricity generation from uranium and thorium fuels, is growing worldwide. Thus, more actinides are being mined, produced, used and processed than ever before. The future of nuclear energy hinges on how these increasing amounts of actinides are contained in each stage of the fuel cycle, including disposition. In addition, uranium and plutonium were built up during the Cold War between the United States and the Former Soviet Union for defense purposes and nuclear energy.

  9. Rapid determination of actinides in seawater samples

    DOE PAGES

    Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.; Utsey, Robin C.; McAlister, Daniel R.

    2014-03-09

    A new rapid method for the determination of actinides in seawater samples has been developed at the Savannah River National Laboratory. The actinides can be measured by alpha spectrometry or inductively-coupled plasma mass spectrometry. The new method employs novel pre-concentration steps to collect the actinide isotopes quickly from 80 L or more of seawater. Actinides are co-precipitated using an iron hydroxide co-precipitation step enhanced with Ti+3 reductant, followed by lanthanum fluoride co-precipitation. Stacked TEVA Resin and TRU Resin cartridges are used to rapidly separate Pu, U, and Np isotopes from seawater samples. TEVA Resin and DGA Resin were used tomore » separate and measure Pu, Am and Cm isotopes in seawater volumes up to 80 L. This robust method is ideal for emergency seawater samples following a radiological incident. It can also be used, however, for the routine analysis of seawater samples for oceanographic studies to enhance efficiency and productivity. In contrast, many current methods to determine actinides in seawater can take 1–2 weeks and provide chemical yields of ~30–60 %. This new sample preparation method can be performed in 4–8 h with tracer yields of ~85–95 %. By employing a rapid, robust sample preparation method with high chemical yields, less seawater is needed to achieve lower or comparable detection limits for actinide isotopes with less time and effort.« less

  10. Actinide recovery method -- Large soil samples

    SciTech Connect

    Maxwell , S.L. III

    2000-04-25

    There is a need to measure actinides in environmental samples with lower and lower detection limits, requiring larger sample sizes. This analysis is adversely affected by sample-matrix interferences, which make analyzing soil samples above five-grams very difficult. A new Actinide-Recovery Method has been developed by the Savannah River Site Central Laboratory to preconcentrate actinides from large-soil samples. Diphonix Resin (Eichrom Industries), a 1994 R and D 100 winner, is used to preconcentrate the actinides from large soil samples, which are bound powerfully to the resin's diphosphonic acid groups. A rapid microwave-digestion technique is used to remove the actinides from the Diphonix Resin, which effectively eliminates interfering matrix components from the soil matrix. The microwave-digestion technique is more effective and less tedious than catalyzed hydrogen peroxide digestions of the resin or digestion of diphosphonic stripping agents such as HEDPA. After resin digestion, the actinides are recovered in a small volume of nitric acid which can be loaded onto small extraction chromatography columns, such as TEVA Resin, U-TEVA Resin or TRU Resin (Eichrom Industries). Small, selective extraction columns do not generate large volumes of liquid waste and provide consistent tracer recoveries after soil matrix elimination.

  11. Quantum Chemical Studies of Actinides and Lanthanides: From Small Molecules to Nanoclusters

    NASA Astrophysics Data System (ADS)

    Vlaisavljevich, Bess

    Research into actinides is of high interest because of their potential applications as an energy source and for the environmental implications therein. Global concern has arisen since the development of the actinide concept in the 1940s led to the industrial scale use of the commercial nuclear energy cycle and nuclear weapons production. Large quantities of waste have been generated from these processes inspiring efforts to address fundamental questions in actinide science. In this regard, the objective of this work is to use theory to provide insight and predictions into actinide chemistry, where experimental work is extremely challenging because of the intrinsic difficulties of the experiments themselves and the safety issues associated with this type of chemistry. This thesis is a collection of theoretical studies of actinide chemistry falling into three categories: quantum chemical and matrix isolation studies of small molecules, the electronic structure of organoactinide systems, and uranyl peroxide nanoclusters and other solid state actinide compounds. The work herein not only spans a wide range of systems size but also investigates a range of chemical problems. Various quantum chemical approaches have been employed. Wave function-based methods have been used to study the electronic structure of actinide containing molecules of small to middle-size. Among these methods, the complete active space self consistent field (CASSCF) approach with corrections from second-order perturbation theory (CASPT2), the generalized active space SCF (GASSCF) approach, and Moller-Plesset second-order perturbation theory (MP2) have been employed. Likewise, density functional theory (DFT) has been used along with analysis tools like bond energy decomposition, bond orders, and Bader's Atoms in Molecules. From these quantum chemical results, comparison with experimentally obtained structures and spectra are made.

  12. "Computational Modeling of Actinide Complexes"

    SciTech Connect

    Balasubramanian, K

    2007-03-07

    We will present our recent studies on computational actinide chemistry of complexes which are not only interesting from the standpoint of actinide coordination chemistry but also of relevance to environmental management of high-level nuclear wastes. We will be discussing our recent collaborative efforts with Professor Heino Nitsche of LBNL whose research group has been actively carrying out experimental studies on these species. Computations of actinide complexes are also quintessential to our understanding of the complexes found in geochemical, biochemical environments and actinide chemistry relevant to advanced nuclear systems. In particular we have been studying uranyl, plutonyl, and Cm(III) complexes are in aqueous solution. These studies are made with a variety of relativistic methods such as coupled cluster methods, DFT, and complete active space multi-configuration self-consistent-field (CASSCF) followed by large-scale CI computations and relativistic CI (RCI) computations up to 60 million configurations. Our computational studies on actinide complexes were motivated by ongoing EXAFS studies of speciated complexes in geo and biochemical environments carried out by Prof Heino Nitsche's group at Berkeley, Dr. David Clark at Los Alamos and Dr. Gibson's work on small actinide molecules at ORNL. The hydrolysis reactions of urnayl, neputyl and plutonyl complexes have received considerable attention due to their geochemical and biochemical importance but the results of free energies in solution and the mechanism of deprotonation have been topic of considerable uncertainty. We have computed deprotonating and migration of one water molecule from the first solvation shell to the second shell in UO{sub 2}(H{sub 2}O){sub 5}{sup 2+}, UO{sub 2}(H{sub 2}O){sub 5}{sup 2+}NpO{sub 2}(H{sub 2}O){sub 6}{sup +}, and PuO{sub 2}(H{sub 2}O){sub 5}{sup 2+} complexes. Our computed Gibbs free energy(7.27 kcal/m) in solution for the first time agrees with the experiment (7.1 kcal

  13. Overview of actinide chemistry in the WIPP

    SciTech Connect

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

    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

  14. Actinide speciation in relation to biological processes.

    PubMed

    Ansoborlo, Eric; Prat, Odette; Moisy, Philippe; Den Auwer, Christophe; Guilbaud, Philippe; Carriere, M; Gouget, Barbara; Duffield, John; Doizi, Denis; Vercouter, Thomas; Moulin, Christophe; Moulin, Valérie

    2006-11-01

    In case of accidental release of radionuclides into the environment, actinides represent a severe health risk to human beings following internal contamination (inhalation, ingestion or wound). For a better understanding of the actinide behaviour in man (in term of metabolism, retention, excretion) and in specific biological systems (organs, cells or biochemical pathways), it is of prime importance to have a good knowledge of the relevant actinide solution chemistry and biochemistry, in particular of the thermodynamic constants needed for computing actinide speciation. To a large extent, speciation governs bioavailability and toxicity of elements and has a significant impact on the mechanisms by which toxics accumulate in cell compartments and organs and by which elements are transferred and transported from cell to cell. From another viewpoint, speciation is the prerequisite for the design and success of potential decorporation therapies. The purpose of this review is to present the state of the art of actinide knowledge within biological media. It is also to discuss how actinide speciation can be determined or predicted and to highlight the areas where information is lacking with the aim to encourage new research efforts.

  15. Actinide abundances in ordinary chondrites

    NASA Technical Reports Server (NTRS)

    Hagee, B.; Bernatowicz, T. J.; Podosek, F. A.; Johnson, M. L.; Burnett, D. S.

    1990-01-01

    Measurements of actinide and light REE (LREE) abundances and of phosphate abundances in equilibrated ordinary chondrites were obtained and were used to define the Pu abundance in the solar system and to determine the degree of variation of actinide and LREE abundances. The results were also used to compare directly the Pu/U ratio with the earlier obtained ratio determined indirectly, as (Pu/Nd)x(Nd/U), assuming that Pu behaves chemically as a LREE. The data, combined with high-accuracy isotope-dilution data from the literature, show that the degree of gram-scale variability of the Th, U, and LREE abundances for equilibrated ordinary chondrites is a factor of 2-3 for absolute abundances and up to 50 percent for relative abundances. The observed variations are interpreted as reflecting the differences in the compositions and/or proportions of solar nebula components accreted to ordinary chondrite parent bodies.

  16. Identification and Speciation of Actinides in the Environment

    NASA Astrophysics Data System (ADS)

    Degueldre, Claude

    All actinide isotopes are radioactive. Since the middle of the last century, new bactinide and transactinide isotopes have been artificially produced and the use of several of the naturally occurring actinide isotopes has increased. This production is due to the nuclear power industry and the military fabrication and use of nuclear weapons. These activities have created anxiety about the introduction of actinide elements into the environment. Consequently, environmental systems that contain or are exploited for natural actinides, or, are potentially contaminated by anthropogenic actinides, must be investigated. The analytical techniques introduced in this chapter are used, after sampling when required, to identify and quantify the actinide isotopes and to determine the species in which they are present.

  17. Actinide recovery process

    DOEpatents

    Muscatello, A.C.; Navratil, J.D.; Saba, M.T.

    1985-06-13

    Process for the removal of plutonium polymer and ionic actinides from aqueous solutions by absorption onto a solid extractant loaded on a solid inert support such as polystyrene-divinylbenzene. The absorbed actinides can then be recovered by incineration, by stripping with organic solvents, or by acid digestion. Preferred solid extractants are trioctylphosphine oxide and octylphenyl-N,N-diisobutylcarbamoylmethylphosphine oxide and the like. 2 tabs.

  18. PRODUCTION OF ACTINIDE METAL

    DOEpatents

    Knighton, J.B.

    1963-11-01

    A process of reducing actinide oxide to the metal with magnesium-zinc alloy in a flux of 5 mole% of magnesium fluoride and 95 mole% of magnesium chloride plus lithium, sodium, potassium, calcium, strontium, or barium chloride is presented. The flux contains at least 14 mole% of magnesium cation at 600-- 900 deg C in air. The formed magnesium-zinc-actinide alloy is separated from the magnesium-oxide-containing flux. (AEC)

  19. The applicability of MGA method for depleted and natural uranium isotopic analysis in the presence of actinides (232Th, 237Np, 233Pa and 241Am).

    PubMed

    Yücel, Haluk

    2007-11-01

    The multi-group analysis (MGA) method for the determination of uranium isotopic abundances in depleted uranium (DU) and natural uranium (NU) samples is applied in this study. A set of non-destructive gamma-ray measurements of DU and NU samples were performed using a planar Ge detector. The relative abundances of 235U and 238U isotopes were compared with the declared values of the standards. The relative abundance for 235U obtained by MGA for a "clean" DU or NU sample with a content of uranium>1wt% is determined with an accuracy of about +/-5%. However, when several actinides such as 232Th, 237Np, 233Pa and 241Am are present along with uranium isotopes simulating "dirty" DU or NU, it has been observed that MGA method gives erroneous results. The 235U abundance results for the samples were 6-25 times higher than the declared values in the presence of above-mentioned actinides, since MGA is utilized the X-ray and gamma-ray peaks in the 80-130 keV energy region, covering XKalpha and XKbeta regions. After the least-squares fitting of the spectra, it is found that the increases in the intensities of the X-ray and gamma-ray peaks of uranium are remarkably larger in the complex 80-130 keV region. On the other hand, it is observed that the interferences of the actinide peaks are relatively less dominant in the higher gamma-ray region of 130-300 keV. The results imply the need for dirty DU and NU samples that the MGA method should utilize the higher energy gamma-rays (up to 1001 keV of (234m)Pa) combined with lower energies of the spectra, which may be collected in a two detector mode (a planar Ge and a high efficient coaxial Ge).

  20. The applicability of MGA method for depleted and natural uranium isotopic analysis in the presence of actinides (232Th, 237Np, 233Pa and 241Am).

    PubMed

    Yücel, Haluk

    2007-11-01

    The multi-group analysis (MGA) method for the determination of uranium isotopic abundances in depleted uranium (DU) and natural uranium (NU) samples is applied in this study. A set of non-destructive gamma-ray measurements of DU and NU samples were performed using a planar Ge detector. The relative abundances of 235U and 238U isotopes were compared with the declared values of the standards. The relative abundance for 235U obtained by MGA for a "clean" DU or NU sample with a content of uranium>1wt% is determined with an accuracy of about +/-5%. However, when several actinides such as 232Th, 237Np, 233Pa and 241Am are present along with uranium isotopes simulating "dirty" DU or NU, it has been observed that MGA method gives erroneous results. The 235U abundance results for the samples were 6-25 times higher than the declared values in the presence of above-mentioned actinides, since MGA is utilized the X-ray and gamma-ray peaks in the 80-130 keV energy region, covering XKalpha and XKbeta regions. After the least-squares fitting of the spectra, it is found that the increases in the intensities of the X-ray and gamma-ray peaks of uranium are remarkably larger in the complex 80-130 keV region. On the other hand, it is observed that the interferences of the actinide peaks are relatively less dominant in the higher gamma-ray region of 130-300 keV. The results imply the need for dirty DU and NU samples that the MGA method should utilize the higher energy gamma-rays (up to 1001 keV of (234m)Pa) combined with lower energies of the spectra, which may be collected in a two detector mode (a planar Ge and a high efficient coaxial Ge). PMID:17606378

  1. Development of the Actinide-Lanthanide Separation (ALSEP) Process

    SciTech Connect

    Lumetta, Gregg J.; Carter, Jennifer C.; Niver, Cynthia M.; Gelis, Artem V.

    2014-09-30

    Separating the minor actinide elements (Am and Cm) from acidic high-level raffinates arising from the reprocessing of irradiated nuclear fuel is an important step in closing the nuclear fuel cycle. Most proposed approaches to this problem involve two solvent extraction steps: 1) co-extraction of the trivalent lanthanides and actinides, followed by 2) separation of the actinides from the lanthanides. The objective of our work is to develop a single solvent-extraction process for isolating the minor actinide elements. We report here a solvent containing N,N,N',N'-tetra(2 ethylhexyl)diglycolamide (T2EHDGA) combined with 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) that can be used to separate the minor actinides in a single solvent-extraction process. T2EHDGA serves to co-extract the trivalent actinide and lanthanide ions from nitric acid solution. Switching the aqueous phase chemistry to a citrate buffered solution of N-(2-hydroxyethyl)ethylenediamine-N,N',N'-triacetic acid at pH 2.5 to 4 results in selective transfer of the actinides to the aqueous phase, thus affecting separation of the actinides from the lanthanides. Separation factors between the lanthanides and actinides are approximately 20 in the pH range of 3 to 4, and the distribution ratios are not highly dependent on the pH in this system.

  2. Nonaqueous actinide hydride dissolution and production of actinide $beta$- diketonates

    DOEpatents

    Crisler, L.R.

    1975-11-11

    Actinide beta-diketonate complex molecular compounds are produced by reacting a beta-diketone compound with a hydride of the actinide material in a mixture of carbon tetrachloride and methanol. (auth)

  3. Isotopic biases for actinide-only burnup credit

    SciTech Connect

    Rahimi, M.; Lancaster, D.; Hoeffer, B.; Nichols, M.

    1997-04-01

    The primary purpose of this paper is to present the new methodology for establishing bias and uncertainty associated with isotopic prediction in spent fuel assemblies for burnup credit analysis. The analysis applies to the design of criticality control systems for spent fuel casks. A total of 54 spent fuel samples were modeled and analyzed using the Shielding Analyses Sequence (SAS2H). Multiple regression analysis and a trending test were performed to develop isotopic correction factors for 10 actinide burnup credit isotopes. 5 refs., 1 tab.

  4. Bioreduction amenability testing of actinide contaminated soils. The systems: Am{sup 241}-Pu{sup 238}, Am{sup 241}-Pu{sup 239/40}, U

    SciTech Connect

    Korich, D.G.; Sharp, J.E.

    1995-01-01

    Bioreductive processing of actinide contaminated soils can achieve extraction levels in excess of 97% for both plutonium and uranium contaminants. Reasonable reaction rates of 4 to 6 day resident times for Pu-Am have been demonstrated on 4 gram sample charges. Longer reaction times of 17 days required for uranium extraction can be improved by soil sample preconditioning and/or an increase in process reagent concentrations. The environmentally benign treatment process operates at pH 6--7, preserves the original soil matrix, and utilizes standard processing equipment. The process reagent component (inoculum SD-1 and biological growth medium PX100{trademark}) are available for utilization in an integrated system. Process techniques developed by MBX, involving graduated volume bioreactors have been proven to alleviate biological toxicity problems in treatment leachates. Bioreduction processing of actinide contaminated soils, preconditioning of soil charges, and recycling or vegetation of unacceptable tailings can be combined to provide an effective and environmentally attractive method of remediation. The soil test program was designed to determine the applicability of the MBX bioreductive technology to solubilize Pu and Am from RFP, Mound and LANL soils and uranium from Hanford and Fernald soils.

  5. TUCS/phosphate mineralization of actinides

    SciTech Connect

    Nash, K.L.

    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.

  6. A systematic analysis of the spectra of trivalent actinide chlorides in D sub 3 h site symmetry

    SciTech Connect

    Carnall, W.T. )

    1992-06-15

    The optical spectra of actinide ions in the compound AnCl{sub 3} and doped into single-crystal LaCl{sub 3} were interpreted in terms of transitions within 5{ital f}{sup {ital N}} configurations. Energy-level calculations were carried out using an effective-operator Hamiltonian, the parameters of which were determined by fitting experimental data. Atomic and crystal-field matrices were diagonalized simultaneously assuming an approximate {ital D}{sub 3{ital h}} site symmetry. Spectroscopic data were taken from the literature but in most cases supplemented by unpublished measurements in absorption and in fluorescence. Data for each ion were analyzed independently, then the model parameters were intercompared and in many cases adjusted such that in the final fitting process the principal interactions showed uniform trends in parameter values with increasing atomic number. Consistent with analyses of the spectra of lanthanide ions in both LaCl{sub 3} and LaF{sub 3}, abrupt changes in magnitude of certain crystal-field parameters were found near the center of the 5{ital f}{sup {ital N}} series. This resulted in two groups of parameter values, but with consistent trends for both halves of the series, and generally very good agreement between observed and computed energies. A new energy-level chart based on computed crystal-field level energies for each trivalent actinide ion has been prepared.

  7. Systems Analysis.

    ERIC Educational Resources Information Center

    Loucks, D. P.; Bell, J. M.

    1978-01-01

    Presents a literature review of the analysis of the administrative systems of various environmental programs related to water quality and pollution policy. A list of 70 references published in 1976 and 1977 is also presented. (HM)

  8. Applications of time-resolved laser fluorescence spectroscopy to the environmental biogeochemistry of actinides.

    PubMed

    Collins, Richard N; Saito, Takumi; Aoyagi, Noboru; Payne, Timothy E; Kimura, Takaumi; Waite, T David

    2011-01-01

    Time-resolved laser fluorescence spectroscopy (TRLFS) is a useful means of identifying certain actinide species resulting from various biogeochemical processes. In general, TRLFS differentiates chemical species of a fluorescent metal ion through analysis of different excitation and emission spectra and decay lifetimes. Although this spectroscopic technique has largely been applied to the analysis of actinide and lanthanide ions having fluorescence decay lifetimes on the order of microseconds, such as UO , Cm, and Eu, continuing development of ultra-fast and cryogenic TRLFS systems offers the possibility to obtain speciation information on metal ions having room-temperature fluorescence decay lifetimes on the order of nanoseconds to picoseconds. The main advantage of TRLFS over other advanced spectroscopic techniques is the ability to determine in situ metal speciation at environmentally relevant micromolar to picomolar concentrations. In the context of environmental biogeochemistry, TRLFS has principally been applied to studies of (i) metal speciation in aqueous and solid phases and (ii) the coordination environment of metal ions sorbed to mineral and bacterial surfaces. In this review, the principles of TRLFS are described, and the literature reporting the application of this methodology to the speciation of actinides in systems of biogeochemical interest is assessed. Significant developments in TRLFS methodology and advanced data analysis are highlighted, and we outline how these developments have the potential to further our mechanistic understanding of actinide biogeochemistry.

  9. Actinide abundances in ordinary chondrites

    USGS Publications Warehouse

    Hagee, B.; Bernatowicz, T.J.; Podosek, F.A.; Johnson, M.L.; Burnett, D.S.; Tatsumoto, M.

    1990-01-01

    Measurements of 244Pu fission Xe, U, Th, and light REE (LREE) abundances, along with modal petrographic determinations of phosphate abundances, were carried out on equilibrated ordinary chondrites in order to define better the solar system Pu abundance and to determine the degree of variation of actinide and LREE abundances. Our data permit comparison of the directly measured Pu/ U ratio with that determined indirectly as (Pu/Nd) ?? (Nd/U) assuming that Pu behaves chemically as a LREE. Except for Guaren??a, and perhaps H chondrites in general, Pu concentrations are similar to that determined previously for St. Se??verin, although less precise because of higher trapped Xe contents. Trapped 130Xe 136Xe ratios appear to vary from meteorite to meteorite, but, relative to AVCC, all are similar in the sense of having less of the interstellar heavy Xe found in carbonaceous chondrite acid residues. The Pu/U and Pu/Nd ratios are consistent with previous data for St. Se??verin, but both tend to be slightly higher than those inferred from previous data on Angra dos Reis. Although significant variations exist, the distribution of our Th/U ratios, along with other precise isotope dilution data for ordinary chondrites, is rather symmetric about the CI chondrite value; however, actinide/(LREE) ratios are systematically lower than the CI value. Variations in actinide or LREE absolute and relative abundances are interpreted as reflecting differences in the proportions and/or compositions of more primitive components (chondrules and CAI materials?) incorporated into different regions of the ordinary chondrite parent bodies. The observed variations of Th/U, Nd/U, or Ce/U suggest that measurements of Pu/U on any single equilibrated ordinary chondrite specimen, such as St. Se??verin, should statistically be within ??20-30% of the average solar system value, although it is also clear that anomalous samples exist. ?? 1990.

  10. Minor Actinides Recycling in PWRs

    SciTech Connect

    Delpech, M.; Golfier, H.; Vasile, A.; Varaine, F.; Boucher, L.; Greneche, D.

    2006-07-01

    Recycling of minor actinides in current and near future PWR is considered as one of the options of the general waste management strategy. This paper presents the analysis of this option both from the core physics and fuel cycle point of view. A first indicator of the efficiency of different neutron spectra for transmutation purposes is the capture to fission cross sections ratio which is less favourable by a factor between 5 to 10 in PWRs compared to fast reactors. Another indicator presented is the production of high ranking isotopes like Curium, Berkelium or Californium in the thermal or epithermal spectrum conditions of PWR cores by successive neutron captures. The impact of the accumulation of this elements on the fabrication process of such PWR fuels strongly penalizes this option. The main constraint on minor actinides loadings in PWR (or fast reactors) fuels are related to their direct impact (or the impact of their transmutation products) on the reactivity coefficients, the reactivity control means and the core kinetics parameters. The main fuel cycle physical parameters like the neutron source, the alpha decay power, the gamma and neutrons dose rate and the criticality aspects are also affected. Recent neutronic calculations based on a reference core of the Evolutionary Pressurized Reactor (EPR), indicates typical maximum values of 1 % loadings. Different fuel design options for minor actinides transmutation purposes in PWRs are presented: UOX and MOX, homogeneous and heterogeneous assemblies. In this later case, Americium loading is concentrated in specific pins of a standard UOX assembly. Recycling of Neptunium in UOX and MOX fuels was also studied to improve the proliferation resistance of the fuel. The impact on the core physics and penalties on Uranium enrichment were underlined in this case. (authors)

  11. A systematic analysis of the spectra of trivalent actinide chlorides in D sub 3h site symmetry

    SciTech Connect

    Carnall, W.T.

    1989-11-01

    The optical spectra of actinide ions in the compound AnCl{sub 3} and doped into single crystal LaCl{sub 3} were interpreted in terms of transitions within 5f{sup N} configurations. Energy-level calculations were carried out using an effective operator Hamiltonian, the parameters of which were determined by fitting experimental data. Atomic and crystal-field matrices were diagonalized simultaneously assuming an approximate D{sub 3h} site symmetry. The spectroscopic data were taken from the literature but in most cases supplemented by unpublished measurements in absorption and in fluorescence. Spectroscopic data for each ion were analyzed independently, then the model parameters were intercompared and in many cases adjusted such that in the final fitting process the principal interactions showed uniform trends in parameter values with increasing atomic number. Consistent with analyses of the spectra of lanthanide ions in both LaCl{sub 3} and LaF{sub 3}, abrupt changes in magnitude of certain crystal-field parameters were found near the center of the 5f{sup N}-series. This resulted in two groups of parameter values, but with consistent trends for both halves of the series, and generally very good agreement between observed and computed energies. A new energy level chart based on computed crystal-field level energies for each trivalent actinide ion has been prepared. in addition, the parameters of the atomic part of each 5f{sup N} Hamiltonian were used to calculate the matrix elements of U{sup ({lambda})} for selected transitions. The values were tabulated to facilitate calculation of intensity-related parameters for 5f{sup N}-transitions using the Judd-Ofelt theory. 44 refs., 10 figs., 3 tabs.

  12. Actinide Lanthanide Separation Process – ALSEP

    SciTech Connect

    Gelis, Artem V.; Lumetta, Gregg J.

    2014-01-29

    Separation of the minor actinides (Am, Cm) from the lanthanides at an industrial scale remains a significant technical challenge for closing the nuclear fuel cycle. To increase the safety of used nuclear fuel (UNF) reprocessing, as well as reduce associated costs, a novel solvent extraction process has been developed. The process allows for partitioning minor actinides, lanthanides and fission products following uranium/plutonium/neptunium removal; minimizing the number of separation steps, flowsheets, chemical consumption, and waste. This new process, Actinide Lanthanide SEParation (ALSEP), uses an organic solvent consisting of a neutral diglycolamide extractant, either N,N,N',N'-tetra(2 ethylhexyl)diglycolamide (T2EHDGA) or N,N,N',N'-tetraoctyldiglycolamide (TODGA), and an acidic extractant 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]), dissolved in an aliphatic diluent (e.g. n-dodecane). The An/Ln co-extraction is conducted from moderate-to-strong nitric acid, while the selective stripping of the minor actinides from the lanthanides is carried out using a polyaminocarboxylic acid/citrate buffered solution at pH anywhere between 3 and 4.5. The extraction and separation of the actinides from the fission products is very effective in a wide range of HNO3 concentrations and the minimum separation factors for lanthanide/Am exceed 30 for Nd/Am, reaching > 60 for Eu/Am under some conditions. The experimental results presented here demonstrate the great potential for a combined system, consisting of a neutral extractant such as T2EHDGA or TODGA, and an acidic extractant such as HEH[EHP], for separating the minor actinides from the lanthanides.

  13. Actinide halide complexes

    SciTech Connect

    Avens, L.R.; Zwick, B.D.; Sattelberger, A.P.; Clark, D.L.; Watkin, J.G.

    1991-02-07

    A compound of the formula MX{sub n}L{sub m} wherein M = Th, Pu, Np,or Am thorium, X = a halide atom, n = 3 or 4, L is a coordinating ligand selected from the group consisting of aprotic Lewis bases having an oxygen-, nitrogen-, sulfur-, or phosphorus-donor, and m is 3 or 4 for monodentate ligands or is 2 for bidentate ligands, where n + m = 7 or 8 for monodentate ligands or 5 or 6 for bidentate ligands, a compound of the formula MX{sub n} wherein M, X, and n are as previously defined, and a process of preparing such actinide metal compounds including admixing the actinide metal in an aprotic Lewis base as a coordinating solvent in the presence of a halogen-containing oxidant, are provided.

  14. Rapid determination of actinides in asphalt samples

    DOE PAGES

    Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.

    2014-01-12

    A new rapid method for the determination of actinides in asphalt samples has been developed that can be used in emergency response situations or for routine analysis If a radiological dispersive device (RDD), Improvised Nuclear Device (IND) or a nuclear accident such as the accident at the Fukushima Nuclear Power Plant in March, 2011 occurs, there will be an urgent need for rapid analyses of many different environmental matrices, including asphalt materials, to support dose mitigation and environmental clean up. The new method for the determination of actinides in asphalt utilizes a rapid furnace step to destroy bitumen and organicsmore » present in the asphalt and sodium hydroxide fusion to digest the remaining sample. Sample preconcentration steps are used to collect the actinides and a new stacked TRU Resin + DGA Resin column method is employed to separate the actinide isotopes in the asphalt samples. The TRU Resin plus DGA Resin separation approach, which allows sequential separation of plutonium, uranium, americium and curium isotopes in asphalt samples, can be applied to soil samples as well.« less

  15. Rapid determination of actinides in asphalt samples

    SciTech Connect

    Maxwell, Sherrod L.; Culligan, Brian K.; Hutchison, Jay B.

    2014-01-12

    A new rapid method for the determination of actinides in asphalt samples has been developed that can be used in emergency response situations or for routine analysis If a radiological dispersive device (RDD), Improvised Nuclear Device (IND) or a nuclear accident such as the accident at the Fukushima Nuclear Power Plant in March, 2011 occurs, there will be an urgent need for rapid analyses of many different environmental matrices, including asphalt materials, to support dose mitigation and environmental clean up. The new method for the determination of actinides in asphalt utilizes a rapid furnace step to destroy bitumen and organics present in the asphalt and sodium hydroxide fusion to digest the remaining sample. Sample preconcentration steps are used to collect the actinides and a new stacked TRU Resin + DGA Resin column method is employed to separate the actinide isotopes in the asphalt samples. The TRU Resin plus DGA Resin separation approach, which allows sequential separation of plutonium, uranium, americium and curium isotopes in asphalt samples, can be applied to soil samples as well.

  16. Isotope ratio analysis of actinides, fission products, and geolocators by high-efficiency multi-collector thermal ionization mass spectrometry

    SciTech Connect

    Bürger, Stefan; Riciputi, Lee R; Bostick, Debra A; Turgeon, Steven; McBay, Eddie H; Lavelle, Mark

    2009-01-01

    A ThermoFisher 'Triton' multi-collector thermal ionization mass spectrometer (MC-TIMS) was evaluated for trace and ultra-trace level isotoperatioanalysis of actinides (uranium, plutonium, and americium), fission products and geolocators (strontium, cesium, and neodymium). Total efficiencies (atoms loaded to ions detected) of up to 0.5-2% for U, Pu, and Am, and 1-30% for Sr, Cs, and Nd can be reported employing resin bead load techniques onto flat ribbon Re filaments or resin beads loaded into a millimeter-sized cavity drilled into a Re rod. This results in detection limits of <0.1 fg (10{sup 4} atoms to 10{sup 5} atoms) for {sup 239-242+244}Pu, {sup 233+236}U, {sup 241-243}Am, {sup 89,90}Sr, and {sup 134,135,137}Cs, and {le} 1 pg for natural Nd isotopes (limited by the chemical processing blank) using a secondary electron multiplier (SEM) or multiple-ion counters (MICs). Relative standard deviations (RSD) as small as 0.1% and abundance sensitivities of 1 x 10{sup 6} or better using a SEM are reported here. Precisions of RSD {approx} 0.01-0.001% using a multi-collector Faraday cup array can be achieved at sub-nanogram concentrations for strontium and neodymium and are suitable to gain crucial geolocation information. The analytical protocols reported herein are of particular value for nuclear forensic and nuclear safeguard applications.

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

    SciTech Connect

    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.

  18. Chemistry of lower valent actinide halides. Final report

    SciTech Connect

    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.

  19. Actinide measurements by AMS using fluoride matrices

    NASA Astrophysics Data System (ADS)

    Cornett, R. J.; Kazi, Z. H.; Zhao, X.-L.; Chartrand, M. G.; Charles, R. J.; Kieser, W. E.

    2015-10-01

    Actinides can be measured by alpha spectroscopy (AS), mass spectroscopy or accelerator mass spectrometry (AMS). We tested a simple method to separate Pu and Am isotopes from the sample matrix using a single extraction chromatography column. The actinides in the column eluent were then measured by AS or AMS using a fluoride target matrix. Pu and Am were coprecipitated with NdF3. The strongest AMS beams of Pu and Am were produced when there was a large excess of fluoride donor atoms in the target and the NdF3 precipitates were diluted about 6-8 fold with PbF2. The measured concentrations of 239,240Pu and 241Am agreed with the concentrations in standards of known activity and with two IAEA certified reference materials. Measurements of 239,240Pu and 241Am made at A.E. Lalonde AMS Laboratory agree, within their statistical uncertainty, with independent measurements made using the IsoTrace AMS system. This work demonstrated that fluoride targets can produce reliable beams of actinide anions and that the measurement of actinides using fluorides agree with published values in certified reference materials.

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

    PubMed

    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. PMID:27427893

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

    PubMed

    Veliscek-Carolan, Jessica

    2016-11-15

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

  2. PROCESS OF PRODUCING ACTINIDE METALS

    DOEpatents

    Magel, T.T.

    1959-07-14

    The preparation of actinide metals in workable, coherent form is described. In general, the objects of the invention are achieved by heating a mixture of an oxide and a halide of an actinide metal such as uranium with an alkali metal on alkaline earth metal reducing agent in the presence of iodine.

  3. Intramolecular energy transfer in actinide complexes of 6-methyl-2-(2-pyridyl)-benzimidazole (biz): comparison between Cm{sup 3+} and Tb{sup 3+} systems

    SciTech Connect

    Assefa, Zerihun . E-mail: assefaz@ornl.gov; Yaita, T.; Haire, R.G.; Tachimori, S.

    2005-02-15

    Coordination of the 6-methyl-2-(2-pyridyl)-benzimidazole ligand with actinide and lanthanide species can produce enhanced emission due to increased efficiency of intramolecular energy transfer to metal centers. A comparison between the curium and terbium systems indicates that the position of the ligand's triplet state is critical for the enhanced emission. The energy gap between the ligand's triplet state and the acceptor level in curium is about 1000cm{sup -1}, as compared to a {approx}600cm{sup -1} gap in the terbium system. Due to the larger gap, the back transfer with curium is reduced and the radiative yield is significantly higher. The quantum yield for this 'sensitized' emission increases to 6.2%, compared to the 0.26% value attained for the metal centered excitation prior to ligand addition. In the terbium case, the smaller donor/acceptor gap enhances back transfer and the energy transfer is less efficient than with the curium system.

  4. Actinide halide complexes

    DOEpatents

    Avens, Larry R.; Zwick, Bill D.; Sattelberger, Alfred P.; Clark, David L.; Watkin, John G.

    1992-01-01

    A compound of the formula MX.sub.n L.sub.m wherein M is a metal atom selected from the group consisting of thorium, plutonium, neptunium or americium, X is a halide atom, n is an integer selected from the group of three or four, L is a coordinating ligand selected from the group consisting of aprotic Lewis bases having an oxygen-, nitrogen-, sulfur-, or phosphorus-donor, and m is an integer selected from the group of three or four for monodentate ligands or is the integer two for bidentate ligands, where the sum of n+m equals seven or eight for monodentate ligands or five or six for bidentate ligands, a compound of the formula MX.sub.n wherein M, X, and n are as previously defined, and a process of preparing such actinide metal compounds including admixing the actinide metal in an aprotic Lewis base as a coordinating solvent in the presence of a halogen-containing oxidant, are provided.

  5. Actinide halide complexes

    DOEpatents

    Avens, L.R.; Zwick, B.D.; Sattelberger, A.P.; Clark, D.L.; Watkin, J.G.

    1992-11-24

    A compound is described of the formula MX[sub n]L[sub m] wherein M is a metal atom selected from the group consisting of thorium, plutonium, neptunium or americium, X is a halide atom, n is an integer selected from the group of three or four, L is a coordinating ligand selected from the group consisting of aprotic Lewis bases having an oxygen-, nitrogen-, sulfur-, or phosphorus-donor, and m is an integer selected from the group of three or four for monodentate ligands or is the integer two for bidentate ligands, where the sum of n+m equals seven or eight for monodentate ligands or five or six for bidentate ligands. A compound of the formula MX[sub n] wherein M, X, and n are as previously defined, and a process of preparing such actinide metal compounds are described including admixing the actinide metal in an aprotic Lewis base as a coordinating solvent in the presence of a halogen-containing oxidant.

  6. Performance of the Lead-Alloy Cooled Concept Balanced for Actinide Burning and Electricity Production

    SciTech Connect

    Pavel Hejzlar; Cliff Davis

    2004-09-01

    A lead-bismuth-cooled fast reactor concept targeted for a balanced mission of actinide burning and low-cost electricity production is proposed and its performance analyzed. The design explores the potential benefits of thorium-based fuel in actinide-burning cores, in particular in terms of the reduction of the large reactivity swing and enhancement of the small Doppler coefficient typical of fertile-free actinide burners. Reduced electricity production cost is pursued through a longer cycle length than that used for fertile-free burners and thus a higher capacity factor. It is shown that the concept can achieve a high transuranics destruction rate, which is only 20% lower than that of an accelerator-driven system with fertile-free fuel. The small negative fuel temperature reactivity coefficient, small positive coolant temperature reactivity coefficient, and negative core radial expansion coefficient provide self-regulating characteristics so that the reactor is capable of inherent shutdown during major transients without scram, as in the Integral Fast Reactor. This is confirmed by thermal-hydraulic analysis of several transients without scram, including primary coolant pump trip, station blackout, and reactivity step insertion, which showed that the reactor was able to meet all identified thermal limits. However, the benefits of high actinide consumption and small reactivity swing can be attained only if the uranium from the discharged fuel is separated and not recycled. This additional uranium separation step and thorium reprocessing significantly increase the fuel cycle costs. Because the higher fuel cycle cost has a larger impact on the overall cost of electricity than the savings from the higher capacity factor afforded through use of thorium, this concept appears less promising than the fertile-free actinide burners.

  7. Performance of the Lead-Alloy-Cooled Reactor Concept Balanced for Actinide Burning and Electricity Production

    SciTech Connect

    Hejzlar, Pavel; Davis, Cliff B.

    2004-09-15

    A lead-bismuth-cooled fast reactor concept targeted for a balanced mission of actinide burning and low-cost electricity production is proposed and its performance analyzed. The design explores the potential benefits of thorium-based fuel in actinide-burning cores, in particular in terms of the reduction of the large reactivity swing and enhancement of the small Doppler coefficient typical of fertile-free actinide burners. Reduced electricity production cost is pursued through a longer cycle length than that used for fertile-free burners and thus a higher capacity factor. It is shown that the concept can achieve a high transuranics destruction rate, which is only 20% lower than that of an accelerator-driven system with fertile-free fuel. The small negative fuel temperature reactivity coefficient, small positive coolant temperature reactivity coefficient, and negative core radial expansion coefficient provide self-regulating characteristics so that the reactor is capable of inherent shutdown during major transients without scram, as in the Integral Fast Reactor. This is confirmed by thermal-hydraulic analysis of several transients without scram, including primary coolant pump trip, station blackout, and reactivity step insertion, which showed that the reactor was able to meet all identified thermal limits. However, the benefits of high actinide consumption and small reactivity swing can be attained only if the uranium from the discharged fuel is separated and not recycled. This additional uranium separation step and thorium reprocessing significantly increase the fuel cycle costs. Because the higher fuel cycle cost has a larger impact on the overall cost of electricity than the savings from the higher capacity factor afforded through use of thorium, this concept appears less promising than the fertile-free actinide burners.

  8. Colloidal behavior of actinides in an oligotrophic lake

    SciTech Connect

    Orlandini, K.A.; Penrose, W.R.; Findlay, M.W. ); Harvey, B.R.; Lovett, M.B. )

    1990-05-01

    Understanding the speciation of low levels of actinides from fallout and from local sources in freshwater systems is important if the authors are to predict their distributions in the environment. Since these materials make excellent tracers for determining sedimentation rates and other environmental parameters, it is important to determine their physical and chemical properties in relatively pristine systems. Reported here are the results of actinide analyses in an artificial, oligotrophic lake in northwest Wales, United Kingdom, which is used as a source of cooling water for a nuclear power plant. The concentrations of the actinide elements plutonium, americium, thorium, and curium, and their distributions among different colloidal sizes were determined. The majority of the actinides in the (nominal 100,000 MW) or 100-nm pore sizes; the actinides appeared to be bound reversibly to colloidal material of unknown composition. The two environmentally stable oxidation states of plutonium, IV and V, could be separated by ultrafiltration. These results indicate that submicron colloidal material can dominate the aqueous properties of actinides.

  9. Managing Inventories of Heavy Actinides

    SciTech Connect

    Wham, Robert M; Patton, Bradley D

    2011-01-01

    The Department of Energy (DOE) has stored a limited inventory of heavy actinides contained in irradiated targets, some partially processed, at the Savannah River Site (SRS) and Oak Ridge National Laboratory (ORNL). The 'heavy actinides' of interest include plutonium, americium, and curium isotopes; specifically 242Pu and 244Pu, 243Am, and 244/246/248Cm. No alternate supplies of these heavy actinides and no other capabilities for producing them are currently available. Some of these heavy actinide materials are important for use as feedstock for producing heavy isotopes and elements needed for research and commercial application. The rare isotope 244Pu is valuable for research, environmental safeguards, and nuclear forensics. Because the production of these heavy actinides was made possible only by the enormous investment of time and money associated with defense production efforts, the remaining inventories of these rare nuclear materials are an important part of the legacy of the Nuclear Weapons Program. Significant unique heavy actinide inventories reside in irradiated Mark-18A and Mark-42 targets at SRS and ORNL, with no plans to separate and store the isotopes for future use. Although the costs of preserving these heavy actinide materials would be considerable, for all practical purposes they are irreplaceable. The effort required to reproduce these heavy actinides today would likely cost billions of dollars and encompass a series of irradiation and chemical separation cycles for at least 50 years; thus, reproduction is virtually impossible. DOE has a limited window of opportunity to recover and preserve these heavy actinides before they are disposed of as waste. A path forward is presented to recover and manage these irreplaceable National Asset materials for future use in research, nuclear forensics, and other potential applications.

  10. Effects of deformations and orientations in the fission of the actinide nuclear system 254Fm* formed in the 11B + 243Am reaction

    NASA Astrophysics Data System (ADS)

    Kaur, Manpreet; Sharma, Manoj K.; Gupta, Raj K.

    2012-12-01

    We have studied the decay of actinide nuclear system 254Fm* formed in 11B + 243Am reaction using the dynamical cluster decay model (DCM), with choices of spherical, quadrupole deformation β2 alone and higher multipole deformations β2-β4. For β2 deformations, the optimum orientations θiopt are used whereas for higher multipole deformations the compact orientations θic of decaying fragments are taken in to account. Besides static-β2 deformations, the effects of dynamical-β2 deformations are also explored. The calculated cross sections find excellent agreement with the available experimental data with spherical as well as deformed choices of fragmentations, enabling us to account for the role of important nuclear deformation effects in the 11B-induced nuclear reaction. Spontaneous decay of 254Fm with cold elongated configuration and optimum orientation is also worked out. The mass distributions of excited fermium isotopes in the neighborhood of 254Fm* are also explored. In addition, the roles of temperature, angular momentum, and fission fragment anisotropies are investigated in the context of the chosen reaction.

  11. Modelling the behaviour of oxide fuels containing minor actinides with urania, thoria and zirconia matrices in an accelerator-driven system

    NASA Astrophysics Data System (ADS)

    Sobolev, V.; Lemehov, S.; Messaoudi, N.; Van Uffelen, P.; Aı̈t Abderrahim, H.

    2003-06-01

    The Belgian Nuclear Research Centre, SCK • CEN, is currently working on the pre-design of the multipurpose accelerator-driven system (ADS) MYRRHA. A demonstration of the possibility of transmutation of minor actinides and long-lived fission products with a realistic design of experimental fuel targets and prognosis of their behaviour under typical ADS conditions is an important task in the MYRRHA project. In the present article, the irradiation behaviour of three different oxide fuel mixtures, containing americium and plutonium - (Am,Pu,U)O 2- x with urania matrix, (Am,Pu,Th)O 2- x with thoria matrix and (Am,Y,Pu,Zr)O 2- x with inert zirconia matrix stabilised by yttria - were simulated with the new fuel performance code MACROS, which is under development and testing at the SCK • CEN. All the fuel rods were considered to be of the same design and sizes: annular fuel pellets, helium bounded with the stainless steel cladding, and a large gas plenum. The liquid lead-bismuth eutectic was used as coolant. Typical irradiation conditions of the hottest fuel assembly of the MYRRHA subcritical core were pre-calculated with the MCNPX code and used in the following calculations as the input data. The results of prediction of the thermo-mechanical behaviour of the designed rods with the considered fuels during three irradiation cycles of 90 EFPD are presented and discussed.

  12. Actinide Burning in CANDU Reactors

    SciTech Connect

    Hyland, B.; Dyck, G.R.

    2007-07-01

    Actinide burning in CANDU reactors has been studied as a method of reducing the actinide content of spent nuclear fuel from light water reactors, and thereby decreasing the associated long term decay heat load. In this work simulations were performed of actinides mixed with natural uranium to form a mixed oxide (MOX) fuel, and also mixed with silicon carbide to form an inert matrix (IMF) fuel. Both of these fuels were taken to a higher burnup than has previously been studied. The total transuranic element destruction calculated was 40% for the MOX fuel and 71% for the IMF. (authors)

  13. High-burnup core design using minor actinide-containing metal fuel

    SciTech Connect

    Ohta, Hirokazu; Ogata, Takanari; Obara, T.

    2013-07-01

    A neutronic design study of metal fuel fast reactor (FR) cores is conducted on the basis of an innovative fuel design concept to achieve an extremely high burnup and realize an efficient fuel cycle system. Since it is expected that the burnup reactivity swing will become extremely large in an unprecedented high burnup core, minor actinides (MAs) from light water reactors (LWRs) are added to fresh fuel to improve the core internal conversion. Core neutronic analysis revealed that high burnups of about 200 MWd/kg for a small-scale core and about 300 MWd/kg for a large-scale core can be attained while suppressing the burnup reactivity swing to almost the same level as that of conventional cores with normal burnup. An actinide burnup analysis has shown that the MA consumption ratio is improved to about 60% and that the accumulated MAs originating from LWRs can be efficiently consumed by the high-burnup metal fuel FR. (authors)

  14. Actinide Source Term Program, position paper. Revision 1

    SciTech Connect

    Novak, C.F.; Papenguth, H.W.; Crafts, C.C.; Dhooge, N.J.

    1994-11-15

    The Actinide Source Term represents the quantity of actinides that could be mobilized within WIPP brines and could migrate with the brines away from the disposal room vicinity. This document presents the various proposed methods for estimating this source term, with a particular focus on defining these methods and evaluating the defensibility of the models for mobile actinide concentrations. The conclusions reached in this document are: the 92 PA {open_quotes}expert panel{close_quotes} model for mobile actinide concentrations is not defensible; and, although it is extremely conservative, the {open_quotes}inventory limits{close_quotes} model is the only existing defensible model for the actinide source term. The model effort in progress, {open_quotes}chemical modeling of mobile actinide concentrations{close_quotes}, supported by a laboratory effort that is also in progress, is designed to provide a reasonable description of the system and be scientifically realistic and supplant the {open_quotes}Inventory limits{close_quotes} model.

  15. Environmental research on actinide elements

    SciTech Connect

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

    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)

  16. Separation of actinides using capillary extraction chromatography-inductively coupled plasma mass spectrometry.

    PubMed

    Peterson, Dominic S; Montoya, Velma M

    2009-08-01

    Trace levels of actinides have been separated on capillary extraction chromatography columns. Detection of the actinides was achieved using an inductively coupled plasma mass spectrometer, which was coupled with the extraction chromatography system. In this study, we compare 30-cm long, 4.6 mm i.d. columns to capillary columns (750 microm i.d.) with lengths from 30 cm up to 150 cm. The columns that were tested were packed with TRU resin. We were able to separate a mixture of five actinides ((232)Th, (238)U, (237)Np, (239)Pu, and (241)Am). This work has application to rapid bioassay as well as automated separations of actinide materials.

  17. Production and measurement of minor actinides in the commercial fuel cycle

    SciTech Connect

    Stanbro, W.D.

    1997-03-01

    The minor actinide elements, particularly neptunium and americium, are produced as a normal byproduct of the operation of thermal power reactors. Because of the existence of long-lived isotopes of these elements, they constitute the major sources of the residual radiation in spent fuel or in wastes resulting from reprocessing. This has led to examinations by some countries of the possibility of separating the minor actinides from waste products. The papers found in this report address the production of minor actinides in common thermal power reactors as well as approaches to measure these materials in various media. The first paper in this volume, {open_quotes}Production of Minor Actinides in the Commercial Fuel Cycle,{close_quotes} uses calculations with the ORIGEN2 reactor and decay code to estimate the amounts of minor actinides in spent fuel and separated plutonium as a function of reactor irradiation and the time after discharge. The second paper, {open_quotes}Destructive Assay of Minor Actinides,{close_quotes} describes a number of promising approaches for the chemical analysis of minor actinides in the various forms in which they are found at reprocessing plants. The next paper, {open_quotes}Hybrid KED/XRF Measurement of Minor Actinides in Reprocessing Plants,{close_quotes} uses the results of a simulation model to examine the possible applications of the hybrid KED/XRF instrument to the determination of minor actinides in some of the solutions found in reprocessing plants. In {open_quotes}Calorimetric Assay of Minor Actinides,{close_quotes} the authors show some possible extensions of this powerful technique beyond the normal plutonium assays to include the minor actinides. Finally, the last paper in this volume, {open_quotes}Environment Measurements of Transuranic Nuclides,{close_quotes} discusses what is known about the levels of the minor actinides in the environment and ways to analyze for these materials in environmental matrices.

  18. Theoretical investigation on multiple bonds in terminal actinide nitride complexes.

    PubMed

    Wu, Qun-Yan; Wang, Cong-Zhi; Lan, Jian-Hui; Xiao, Cheng-Liang; Wang, Xiang-Ke; Zhao, Yu-Liang; Chai, Zhi-Fang; Shi, Wei-Qun

    2014-09-15

    A series of actinide (An) species of L-An-N compounds [An = Pa-Pu, L = [N(CH2CH2NSiPr(i)3)3](3-), Pr(i) = CH(CH3)2] have been investigated using scalar relativistic density functional theory (DFT) without considering spin-orbit coupling effects. The ground state geometric and electronic structures and natural bond orbital (NBO) analysis of actinide compounds were studied systematically in neutral and anionic forms. It was found that with increasing actinide atomic number, the bond length of terminal multiple An-N1 bond decreases, in accordance with the actinide contraction. The Mayer bond order of An-N1 decreases gradually from An = Pa to Pu, which indicates a decrease in bond strength. The terminal multiple bond for L-An-N compounds contains one σ and two π molecular orbitals, and the contributions of the 6d orbital to covalency are larger in magnitude than the 5f orbital based on NBO analysis and topological analysis of electron density. This work may help in understanding of the bonding nature of An-N multiple bonds and elucidating the trends and electronic structure changes across the actinide series. It can also shed light on the construction of novel An-N multiple bonds.

  19. Crystal growth methods dedicated to low solubility actinide oxalates

    NASA Astrophysics Data System (ADS)

    Tamain, C.; Arab-Chapelet, B.; Rivenet, M.; Grandjean, S.; Abraham, F.

    2016-04-01

    Two novel crystal growth syntheses dedicated to low solubility actinide-oxalate systems and adapted to glove box handling are described. These methods based on the use of precursors of either actinide metal or oxalic acid have been optimized on lanthanide systems (analogue of actinides(III)) and then assessed on real actinide systems. They allow the synthesis of several actinide oxalate single crystals, Am2(C2O4)3(H2O)3·xH2O, Th(C2O4)2·6H2O, M2+x[PuIV2-xPuIIIx(C2O4)5]·nH2O and M1-x[PuIII1-xPuIVx(C2O4)2·H2O]·nH2O. It is the first time that these well-known compounds are formed by crystal growth methods, thus enabling direct structural studies on transuranic element systems and acquisition of basic data beyond deductions from isomorphic (or not) lanthanide compounds. Characterizations by X-ray diffraction, UV-visible solid spectroscopy, demonstrate the potentialities of these two crystal growth methods to obtain oxalate compounds.

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

    SciTech Connect

    Jarvinen, G.; Barrans, R.; Schroeder, N.; Wade, K.; Jones, M.; Smith, B.F.; Mills, J.; Howard, G.; Freiser, H.; Muralidharan, S.

    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. 33rd Actinide Separations Conference

    SciTech Connect

    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.

  2. Gas core reactors for actinide transmutation and breeder applications

    NASA Technical Reports Server (NTRS)

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

    1978-01-01

    This work consists of design power plant studies for four types of reactor systems: uranium plasma core breeder, uranium plasma core actinide transmuter, UF6 breeder and UF6 actinide transmuter. The plasma core systems can be coupled to MHD generators to obtain high efficiency electrical power generation. A 1074 MWt UF6 breeder reactor was designed with a breeding ratio of 1.002 to guard against diversion of fuel. Using molten salt technology and a superheated steam cycle, an efficiency of 39.2% was obtained for the plant and the U233 inventory in the core and heat exchangers was limited to 105 Kg. It was found that the UF6 reactor can produce high fluxes (10 to the 14th power n/sq cm-sec) necessary for efficient burnup of actinide. However, the buildup of fissile isotopes posed severe heat transfer problems. Therefore, the flux in the actinide region must be decreased with time. Consequently, only beginning-of-life conditions were considered for the power plant design. A 577 MWt UF6 actinide transmutation reactor power plant was designed to operate with 39.3% efficiency and 102 Kg of U233 in the core and heat exchanger for beginning-of-life conditions.

  3. Actinides and Life's Origins.

    PubMed

    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

  4. Actinides and Life's Origins.

    PubMed

    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

  5. Nuclear waste forms for actinides

    PubMed Central

    Ewing, Rodney C.

    1999-01-01

    The disposition of actinides, most recently 239Pu from dismantled nuclear weapons, requires effective containment of waste generated by the nuclear fuel cycle. Because actinides (e.g., 239Pu and 237Np) are long-lived, they have a major impact on risk assessments of geologic repositories. Thus, demonstrable, long-term chemical and mechanical durability are essential properties of waste forms for the immobilization of actinides. Mineralogic and geologic studies provide excellent candidate phases for immobilization and a unique database that cannot be duplicated by a purely materials science approach. The “mineralogic approach” is illustrated by a discussion of zircon as a phase for the immobilization of excess weapons plutonium. PMID:10097054

  6. Actinide cation-cation complexes

    SciTech Connect

    Stoyer, N.J.; Seaborg, G.T.

    1994-12-01

    The +5 oxidation state of U, Np, Pu, and Am is a linear dioxo cation (AnO{sub 2}{sup +}) with a formal charge of +1. These cations form complexes with a variety of other cations, including actinide cations. Other oxidation states of actinides do not form these cation-cation complexes with any cation other than AnO{sub 2}{sup +}; therefore, cation-cation complexes indicate something unique about AnO{sub 2}{sup +} cations compared to actinide cations in general. The first cation-cation complex, NpO{sub 2}{sup +}{center_dot}UO{sub 2}{sup 2+}, was reported by Sullivan, Hindman, and Zielen in 1961. Of the four actinides that form AnO{sub 2}{sup +} species, the cation-cation complexes of NpO{sub 2}{sup +} have been studied most extensively while the other actinides have not. The only PuO{sub 2}{sup +} cation-cation complexes that have been studied are with Fe{sup 3+} and Cr{sup 3+} and neither one has had its equilibrium constant measured. Actinides have small molar absorptivities and cation-cation complexes have small equilibrium constants; therefore, to overcome these obstacles a sensitive technique is required. Spectroscopic techniques are used most often to study cation-cation complexes. Laser-Induced Photacoustic Spectroscopy equilibrium constants for the complexes NpO{sub 2}{sup +}{center_dot}UO{sub 2}{sup 2+}, NpO{sub 2}{sup +}{center_dot}Th{sup 4+}, PuO{sub 2}{sup +}{center_dot}UO{sub 2}{sup 2+}, and PuO{sub 2}{sup +}{center_dot}Th{sup 4+} at an ionic strength of 6 M using LIPAS are 2.4 {plus_minus} 0.2, 1.8 {plus_minus} 0.9, 2.2 {plus_minus} 1.5, and {approx}0.8 M{sup {minus}1}.

  7. Status of nuclear data for actinides

    SciTech Connect

    Guzhovskii, B.Y.; Gorelov, V.P.; Grebennikov, A.N.

    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.

  8. Thermodynamics of carbothermic synthesis of actinide mononitrides

    NASA Astrophysics Data System (ADS)

    Ogawa, Toru; Shirasu, Yoshiro; Minato, Kazuo; Serizawa, Hiroyuki

    1997-08-01

    Carbothermic synthesis will be further applied to the fabrication of nitride fuels containing minor actinides (MA) such as neptunium, americium and curium. A thorough understanding of the carbothermic synthesis of UN will be beneficial in the development of the MA-containing fuels. Thermodynamic analysis was carried out for conditions of practical interest in order to better understand the recent fabrication experiences. Two types of solution phases, oxynitride and carbonitride phases, were taken into account. The PuNO ternary isotherm was assessed for the modelling of M(C, N, O). With the understanding of the UN synthesis, the fabrication problems of Am-containing nitrides are discussed.

  9. Actinide Thermodynamics at Elevated Temperatures

    SciTech Connect

    Friese, Judah I.; Rao, Linfeng; Xia, Yuanxian; Bachelor, Paula P.; Tian, Guoxin

    2007-11-16

    The postclosure chemical environment in the proposed Yucca Mountain repository is expected to experience elevated temperatures. Predicting migration of actinides is possible if sufficient, reliable thermodynamic data on hydrolysis and complexation are available for these temperatures. Data are scarce and scattered for 25 degrees C, and nonexistent for elevated temperatures. This collaborative project between LBNL and PNNL collects thermodynamic data at elevated temperatures on actinide complexes with inorganic ligands that may be present in Yucca Mountain. The ligands include hydroxide, fluoride, sulfate, phosphate and carbonate. Thermodynamic parameters of complexation, including stability constants, enthalpy, entropy and heat capacity of complexation, are measured with a variety of techniques including solvent extraction, potentiometry, spectrophotometry and calorimetry

  10. Magnetic exchange coupling in actinide-containing molecules.

    PubMed

    Rinehart, Jeffrey D; Harris, T David; Kozimor, Stosh A; Bartlett, Bart M; Long, Jeffrey R

    2009-04-20

    Recent progress in the assembly of actinide-containing coordination clusters has generated systems in which the first glimpses of magnetic exchange coupling can be recognized. Such systems are of interest owing to the prospects for involving 5f electrons in stronger magnetic exchange than has been observed for electrons in the more contracted 4f orbitals of the lanthanide elements. Here, we survey the actinide-containing molecules thought to exhibit magnetic exchange interactions, including multiuranium, uranium-lanthanide, uranium-transition metal, and uranium-radical species. Interpretation of the magnetic susceptibility data for compounds of this type is complicated by the combination of spin-orbit coupling and ligand-field effects arising for actinide ions. Nevertheless, for systems where analogues featuring diamagnetic replacement components for the non-actinide spin centers can be synthesized, a data subtraction approach can be utilized to probe the presence of exchange coupling. In addition, methods have been developed for employing the resulting data to estimate lower and upper bounds for the exchange constant. Emphasis is placed on evaluation of the linear clusters (cyclam)M[(mu-Cl)U(Me(2)Pz)(4)](2) (M = Co, Ni, Cu, Zn; cyclam = 1,4,8,11-tetraazacyclotetradecane; Me(2)Pz(-) = 3,5-dimethylpyrazolate), for which strong ferromagnetic exchange with 15 cm(-1) < or = J < or = 48 cm(-1) is observed for the Co(II)-containing species. Owing to the modular synthetic approach employed, this system in particular offers numerous opportunities for adjusting the strength of the magnetic exchange coupling and the total number of unpaired electrons. To this end, the prospects of such modularity are discussed through the lens of several new related clusters. Ultimately, it is hoped that this research will be of utility in the development of electronic structure models that successfully describe the magnetic behavior of actinide compounds and will perhaps even lead to new

  11. Mathematical modeling of the effects of aerobic and anaerobic chelate bioegradation on actinide speciation.

    SciTech Connect

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

    1998-03-19

    Biodegradation of natural and anthropogenic chelating agents directly and indirectly affects the speciation, and, hence, the mobility of actinides in subsurface environments. We combined mathematical modeling with laboratory experimentation to investigate the effects of aerobic and anaerobic chelate biodegradation on actinide [Np(IV/V), Pu(IV)] speciation. Under aerobic conditions, nitrilotriacetic acid (NTA) biodegradation rates were strongly influenced by the actinide concentration. Actinide-chelate complexation reduced the relative abundance of available growth substrate in solution and actinide species present or released during chelate degradation were toxic to the organisms. Aerobic bio-utilization of the chelates as electron-donor substrates directly affected actinide speciation by releasing the radionuclides from complexed form into solution, where their fate was controlled by inorganic ligands in the system. Actinide speciation was also indirectly affected by pH changes caused by organic biodegradation. The two concurrent processes of organic biodegradation and actinide aqueous chemistry were accurately linked and described using CCBATCH, a computer model developed at Northwestern University to investigate the dynamics of coupled biological and chemical reactions in mixed waste subsurface environments. CCBATCH was then used to simulate the fate of Np during anaerobic citrate biodegradation. The modeling studies suggested that, under some conditions, chelate degradation can increase Np(IV) solubility due to carbonate complexation in closed aqueous systems.

  12. FY2010 Annual Report for the Actinide Isomer Detection Project

    SciTech Connect

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

    2011-01-01

    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 Special Nuclear Materials (SNM). Future work will include a follow-up measurement scheduled for December 2010 at LBNL. Lessons learned from the July 2010 measurements will be incorporated into these new measurements. Analysis of both the July and December experiments will be completed in a few months. A research paper to be submitted to a peer-reviewed journal will be drafted if the conclusions from the measurements warrant publication.

  13. Uranium in granites from the Southwestern United States: actinide parent-daughter systems, sites and mobilization. First year report

    SciTech Connect

    Silver, L T; Williams, I S; Woodhead, J A

    1980-10-01

    Some of the principal findings of the study on the Lawler Peak Granite are: the granite is dated precisely by this work at 1411 +- 3 m.y., confirming its synchroneity with a great regional terrane of granites. Uranium is presently 8-10 times crustal abundance and thorium 2-3 times in this granite. Uranium is found to be enriched in at least eight, possibly ten, primary igneous mineral species over the whole-rock values. Individual mineral species show distinct levels in, and characteristics ranges of, uranium concentration. It appears that in a uraniferous granite such as this, conventional accuracy mineral suites probably cannot account for most of the uranium in the rock, and more rare, high U-concentration phases also are present and are significant uranium hosts. It appears that at least two different geological episodes have contributed to the disturbance of the U-Th-Pb isotope systems. Studies of various sites for transient dispersal of uranium, thorium, and radiogenic lead isotopes indicate a non-uniform dispersal of these components. It appears that the bulk rock has lost at least 24 percent of its original uranium endowment, accepting limited or no radiogenic lead or thorium migration from the sample.

  14. Safe actinide disposition in molten salt reactors

    SciTech Connect

    Gat, U.

    1997-03-01

    Safe molten salt reactors (MSR) can readily accommodate the burning of all fissile actinides. Only minor compromises associated with plutonium are required. The MSRs can dispose safely of actinides and long lived isotopes to result in safer and simpler waste. Disposing of actinides in MSRs does increase the source term of a safety optimized MSR. It is concluded that the burning and transmutation of actinides in MSRs can be done in a safe manner. Development is needed for the processing to handle and separate the actinides. Calculations are needed to establish the neutron economy and the fuel management. 9 refs.

  15. A new opportunity: coincident spectroscopy in neutron-deficient actinides

    NASA Astrophysics Data System (ADS)

    Gothe, Oliver; Gates, J. M.; Gregorich, K. E.; Baartman, B.; Fallon, P.; Esker, N. E.; Kwarsick, J.; Machiavelli, A. O.; Mudder, P. R.; Olive, D. T.; Pang, G.; Rissanen, J.; Nitsche, H.

    2014-09-01

    Due to high γ-ray background rates heavy element production facilities are usually not sensitive to the electron capture decay of neutron deficient actinides. We have developed new capabilities at the Berkeley Gas Filled Separator (BGS) that allow us to study these isotopes. The highly selective and efficient separation of compound nucleus evaporation residue products using the BGS couple with a rapid delivery to a low-background detector facility, opens up many new possibilities for nuclear decay and structure studies in the neutron deficient actinides. The decay of these actinides produces vacancies in the K-shell resulting in x-rays uniquely identifying the Z of the decay products. We present the first results of this new methodology in studying the nuclear structure of fermium-254 by observing the gamma rays in coincidence with fermium x-rays. Coincident gamma-decay spectroscopy gives us a new tool to study the nuclear structure of previously inaccessible systems.

  16. Separations of actinides, lanthanides and other metals

    DOEpatents

    Smith, Barbara F.; Jarvinen, Gordon D.; Ensor, Dale D.

    1995-01-01

    An organic extracting solution comprised of a bis(acylpyrazolone or a substituted bis(acylpyrazolone) and an extraction method useful for separating certain elements of the actinide series of the periodic table having a valence of four from one other, and also from one or more of the substances in a group consisting of hexavalent actinides, trivalent actinides, trivalent lanthanides, trivalent iron, trivalent aluminum, divalent metals, and monovalent metals and also from one or more of the substances in a group consisting of hexavalent actinides, trivalent actinides, trivalent lanthanides, trivalent iron, trivalent aluminum, divalent metals, and monovalent metals and also useful for separating hexavalent actinides from one or more of the substances in a group consisting of trivalent actinides, trivalent lanthanides, trivalent iron, trivalent aluminum, divalent metals, and monovalent metals.

  17. Thermally unstable complexants/phosphate mineralization of actinides

    SciTech Connect

    Nash, K.

    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.

  18. Extraction of actinides into aqueous polyethylene glycol solutions from carbonate media in the presence of alizarin complexone

    SciTech Connect

    Molochnikova, N.P.; Frenkel', V.Ya.; Myasoedov, B.F.; Shkinev, V.M.; Spivakov, B.Ya.; Zolotov, Yu.A.

    1987-01-01

    Actinide extraction in a two-phase aqueous system based on polyethylene glycol from carbonate solutions of various compositions in presence of alizarin complexone is studied. It is shown that the nature of the alkali metals affects actinide extraction into the polyethylene glycol phase. Tri- and tetravalent actinides are extracted maximally from sodium carbonate solutions. Separation of actinides in different oxidation states is more effective in potassium carbonate solutions. The behavior of americium in different oxidation states in the system carbonate-polyethylene glycol-complexone is studied. The possibility of extraction separation of microamount of americium(V) from curium in carbonate solutions in presence of alizarin complexone is shown.

  19. Grouped actinide separation in advanced nuclear fuel cycles

    SciTech Connect

    Glatz, J.P.; Malmbeck, R.; Ougier, M.; Soucek, P.; Murakamin, T.; Tsukada, T.; Koyama, T.

    2013-07-01

    Aiming at cleaner waste streams (containing only the short-lived fission products) a partitioning and transmutation (P-T) scheme can significantly reduce the quantities of long-lived radionuclides consigned to waste. Many issues and options are being discussed and studied at present in view of selecting the optimal route. The choice is between individual treatment of the relevant elements and a grouped treatment of all actinides together. In the European Collaborative Project ACSEPT (Actinide recycling by Separation and Transmutation), grouped separation options derived from an aqueous extraction or from a dry pyroprocessing route were extensively investigated. Successful demonstration tests for both systems have been carried out in the frame of this project. The aqueous process called GANEX (Grouped Actinide Extraction) is composed of 2 cycles, a first one to recover the major part of U followed by a co-extraction of Np, Pu, Am, and Cm altogether. The pyro-reprocessing primarily applicable to metallic fuels such as the U-Pu-Zr alloy originally developed by the Argonne National Laboratory (US) in the mid 1980s, has also been applied to the METAPHIX fuels containing up to 5% of minor actinides and 5% of lanthanides (e.g. U{sub 60}Pu{sub 20}-Zr{sub 10}Am{sub 2}Nd{sub 3.5}Y{sub 0.5}Ce{sub 0.5}Gd{sub 0.5}). A grouped actinide separation has been successfully carried out by electrorefining on solid Al cathodes. At present the recovery of the actinides from the alloy formed with Al upon electrodeposition is under investigation, because an efficient P-T cycle requires multiple re-fabrication and re-irradiation. (authors)

  20. Actinide Sorption in a Brine/Dolomite Rock System: Evaluating the Degree of Conservatism in Kd Ranges used in Performance Assessment Modeling for the WIPP Nuclear Waste Repository

    NASA Astrophysics Data System (ADS)

    Dittrich, T. M.; Reed, D. T.

    2015-12-01

    The Waste Isolation Pilot Plant (WIPP) near Carlsbad, NM is the only operating nuclear waste repository in the US and has been accepting transuranic (TRU) waste since 1999. The WIPP is located in a salt deposit approximately 650 m below the surface and performance assessment (PA) modeling for a 10,000 year period is required to recertify the operating license with the US EPA every five years. The main pathway of concern for environmental release of radioactivity is a human intrusion caused by drilling into a pressurized brine reservoir below the repository. This could result in the flooding of the repository and subsequent transport in the high transmissivity layer (dolomite-rich Culebra formation) above the waste disposal rooms. We evaluate the degree of conservatism in the estimated sorption partition coefficients (Kds) ranges used in the PA based on an approach developed with granite rock and actinides (Dittrich and Reimus, 2015; Dittrich et al., 2015). Sorption onto the waste storage material (Fe drums) may also play a role in mobile actinide concentrations. We will present (1) a conceptual overview of how Kds are used in the PA model, (2) technical background of the evolution of the ranges and (3) results from batch and column experiments and model predictions for Kds with WIPP dolomite and clays, brine with various actinides, and ligands (e.g., acetate, citrate, EDTA) that could promote transport. The current Kd ranges used in performance models are based on oxidation state and are 5-400, 0.5-10,000, 0.03-200, and 0.03-20 mL g-1 for elements with oxidation states of III, IV, V, and VI, respectively. Based on redox conditions predicted in the brines, possible actinide species include Pu(III), Pu(IV), U(IV), U(VI), Np(IV), Np(V), Am(III), and Th(IV). We will also discuss the challenges of upscaling from lab experiments to field scale predictions, the role of colloids, and the effect of engineered barrier materials (e.g., MgO) on transport conditions. Dittrich

  1. ACTINIDE BIOCOLLOID FORMATION IN BRINE BY HALOPHILIC BACTERIA

    SciTech Connect

    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.

  2. Actinide Biocolloid Formation in Brine by Halophilic Bacteria

    SciTech Connect

    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.

  3. Actinide biocolloid formation in brine by halophilic bacteria

    SciTech Connect

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

    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.

  4. RAPID SEPARATION OF ACTINIDES AND RADIOSTRONTIUM IN VEGETATION SAMPLES

    SciTech Connect

    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.

  5. Actinide Packaging and Storage Facility (APSF)

    SciTech Connect

    Lavietes, A.D.

    1999-10-01

    The Actinide Packaging and Storage Facility (APSF) was designed to provide long-term storage of radionuclides. Task A.229 defined the requirement for a small, low-power radiation detection capability. This detection system was to be deployed as a component of an autonomously guided vehicle (AGV) located within the storage vault of the facility and necessarily had to exhibit the qualities of low maintenance, long lifetime, and stable performance typically required of unattended monitoring systems. The detection system would interface directly with the on-board computer developed as part of the AGV under a separate task. The overall task for this system would be to provide isotopic identification of the material stored within this facility.

  6. Process for recovering actinide values

    DOEpatents

    Horwitz, E. Philip; Mason, George W.

    1980-01-01

    A process for rendering actinide values recoverable from sodium carbonate scrub waste solutions containing these and other values along with organic compounds resulting from the radiolytic and hydrolytic degradation of neutral organophosphorous extractants such as tri-n butyl phosphate (TBP) and dihexyl-N,N-diethyl carbamylmethylene phosphonate (DHDECAMP) which have been used in the reprocessing of irradiated nuclear reactor fuels. The scrub waste solution is preferably made acidic with mineral acid, to form a feed solution which is then contacted with a water-immiscible, highly polar organic extractant which selectively extracts the degradation products from the feed solution. The feed solution can then be processed to recover the actinides for storage or recycled back into the high-level waste process stream. The extractant is recycled after stripping the degradation products with a neutral sodium carbonate solution.

  7. Evaluation of actinide biosorption by microorganisms

    SciTech Connect

    Happel, A.M.

    1996-06-01

    Conventional methods for removing metals from aqueous solutions include chemical precipitation, chemical oxidation or reduction, ion exchange, reverse osmosis, electrochemical treatment and evaporation. The removal of radionuclides from aqueous waste streams has largely relied on ion exchange methods which can be prohibitively costly given increasingly stringent regulatory effluent limits. The use of microbial cells as biosorbants for heavy metals offers a potential alternative to existing methods for decontamination or recovery of heavy metals from a variety of industrial waste streams and contaminated ground waters. The toxicity and the extreme and variable conditions present in many radionuclide containing waste streams may preclude the use of living microorganisms and favor the use of non-living biomass for the removal of actinides from these waste streams. In the work presented here, we have examined the biosorption of uranium by non-living, non-metabolizing microbial biomass thus avoiding the problems associated with living systems. We are investigating biosorption with the long term goal of developing microbial technologies for the remediation of actinides.

  8. Fusion-Fission Burner for Transuranic Actinides

    NASA Astrophysics Data System (ADS)

    Choi, Chan

    2013-10-01

    The 14-MeV DT fusion neutron spectrum from mirror confinement fusion can provide a unique capability to transmute the transuranic isotopes from light water reactors (LWR). The transuranic (TRU) actinides, high-level radioactive wastes, from spent LWR fuel pose serious worldwide problem with long-term decay heat and radiotoxicity. However, ``transmuted'' TRU actinides can not only reduce the inventory of the TRU in the spent fuel repository but also generate additional energy. Typical commercial LWR fuel assemblies for BWR (boiling water reactor) and PWR (pressurized water reactor) measure its assembly lengths with 4.470 m and 4.059 m, respectively, while its corresponding fuel rod lengths are 4.064 m and 3.851 m. Mirror-based fusion reactor has inherently simple geometry for transmutation blanket with steady-state reactor operation. Recent development of gas-dynamic mirror configuration has additional attractive feature with reduced size in central plasma chamber, thus providing a unique capability for incorporating the spent fuel assemblies into transmutation blanket designs. The system parameters for the gas-dynamic mirror-based hybrid burner will be discussed.

  9. Actinide Recovery Method for Large Soil Samples

    SciTech Connect

    Maxwell, S.L. III; Nichols, S.

    1998-11-01

    A new Actinide Recovery Method has been developed by the Savannah River Site Central Laboratory to preconcentrate actinides in very large soil samples. Diphonix Resin(r) is used eliminate soil matrix interferences and preconcentrate actinides after soil leaching or soil fusion. A rapid microwave digestion technique is used to remove the actinides from the Diphonix Resin(r). After the resin digestion, the actinides are recovered in a small volume of nitric acid which can be easily loaded onto small extraction-chromatography columns, such as TEVA Resin(r), U-TEVA Resin(r) or TRU Resin(r) (Eichrom Industries). This method enables the application of small, selective extraction-columns to recover actinides from very large soil samples with high selectivity, consistent tracer recoveries and minimal liquid waste.

  10. Actinide Waste Forms and Radiation Effects

    NASA Astrophysics Data System (ADS)

    Ewing, R. C.; Weber, W. J.

    Over the past few decades, many studies of actinides in glasses and ceramics have been conducted that have contributed substantially to the increased understanding of actinide incorporation in solids and radiation effects due to actinide decay. These studies have included fundamental research on actinides in solids and applied research and development related to the immobilization of the high level wastes (HLW) from commercial nuclear power plants and processing of nuclear weapons materials, environmental restoration in the nuclear weapons complex, and the immobilization of weapons-grade plutonium as a result of disarmament activities. Thus, the immobilization of actinides has become a pressing issue for the twenty-first century (Ewing, 1999), and plutonium immobilization, in particular, has received considerable attention in the USA (Muller et al., 2002; Muller and Weber, 2001). The investigation of actinides and

  11. High-resolution solid-state oxygen-17 NMR of actinide-bearing compounds: an insight into the 5f chemistry.

    PubMed

    Martel, Laura; Magnani, Nicola; Vigier, Jean-Francois; Boshoven, Jacobus; Selfslag, Chris; Farnan, Ian; Griveau, Jean-Christophe; Somers, Joseph; Fanghänel, Thomas

    2014-07-01

    A massive interest has been generated lately by the improvement of solid-state magic-angle spinning (MAS) NMR methods for the study of a broad range of paramagnetic organic and inorganic materials. The open-shell cations at the origin of this paramagnetism can be metals, transition metals, or rare-earth elements. Actinide-bearing compounds and their 5f unpaired electrons remain elusive in this intensive research area due to their well-known high radiotoxicity. A dedicated effort enabling the handling of these highly radioactive materials now allows their analysis using high-resolution MAS NMR (>55 kHz). Here, the study of the local structure of a series of actinide dioxides, namely, ThO2, UO2, NpO2, PuO2, and AmO2, using solid-state (17)O MAS NMR is reported. An important increase of the spectral resolution is found due to the removal of the dipolar broadening proving the efficiency of this technique for structural analysis. The NMR parameters in these systems with numerous and unpaired 5f electrons were interpreted using an empirical approach. Single-ion model calculations were performed for the first time to determine the z component of electron spin on each of the actinide atoms, which is proportional to the shifts. A similar variation thereof was observed only for the heavier actinides of this study.

  12. Fall MRS 2003: Actinides Symposium

    SciTech Connect

    Tobin, J

    2003-11-24

    {lg_bullet} The focus was on fundamental actinide science and its role. {lg_bullet} History- none except the Nuclear Waste Management Symposia {lg_bullet} Joint Sessions- none but we are open to it in the future. {lg_bullet} Tutorials- none but we are open to it in the future. {lg_bullet} 3 days: 16 Invited talks; 36 Contributed Talks; 10 Posters

  13. Experimental Evaluation of Actinide Transport in a Fractured Granodiorite

    SciTech Connect

    Dittrich, Timothy M.; Reimus, Paul W.

    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)

  14. Actinides recovery from irradiated metallic fuel in LiCl-KCl melts

    NASA Astrophysics Data System (ADS)

    Murakami, T.; Rodrigues, A.; Ougier, M.; Iizuka, M.; Tsukada, T.; Glatz, J.-P.

    2015-11-01

    Electrorefining of irradiated metallic fuels was successfully demonstrated: Actinides (U, Pu, Np, Am and Cm) in the fuels were dissolved in LiCl-KCl melts with high dissolution ratios, while U was selectively deposited on a solid cathode and the simultaneous recovery of actinides in a liquid Cd cathode was confirmed. The behavior of actinides, the fuel matrix stabilizer Zr and fission products such as lanthanide, alkaline, alkaline earth and noble metal, at the electrorefining is discussed based on the ICP-MS analysis of the samples taken from molten salt electrolyte, anode fuel residues and cathode deposits.

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

    SciTech Connect

    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.

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

    SciTech Connect

    Ruggiero, Christy

    2003-06-01

    This project seeks 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 hereby investigated though characterization of actinide-phytosiderophore complexes (independently of plants), and characterization of plant uptake of such complexes.

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

    SciTech Connect

    Ruggiero, Christy

    2004-06-01

    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 phytosiderophoreproducing 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 increased chelation of actinides, which may increase 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.

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

    SciTech Connect

    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.

  19. Isotopic validation for PWR actinide-only burnup credit using Yankee Rowe data

    SciTech Connect

    1997-11-01

    Safety analyses of criticality control systems for transportation packages include an assumption that the spent nuclear fuel (SNF) loaded into the package is fresh or unirradiated. In other words, the spent fuel is assumed to have its original, as-manufactured U-235 isotopic content. The ``fresh fuel`` assumption is very conservative since the potential reactivity of the nuclear fuel is substantially reduced after being irradiated in the reactor core. The concept of taking credit for this reduction in nuclear fuel reactivity due to burnup of the fuel, instead of using the fresh fuel assumption in the criticality safety analysis, is referred to as ``Burnup Credit.`` Burnup credit uses the actual physical composition of the fuel and accounts for the net reduction of fissile material and the buildup of neutron absorbers in the fuel as it is irradiated. Neutron absorbers include actinides and other isotopes generated as a result of the fission process. Using only the change in actinide isotopes in the burnup credit criticality analysis is referred to as ``Actinide-Only Burnup Credit.`` The use of burnup credit in the design of criticality control systems enables more spent fuel to be placed in a package. Increased package capacity results in a reduced number of storage, shipping and disposal containers for a given number of SNF assemblies. Fewer shipments result in a lower risk of accidents associated with the handling and transportation of spent fuel, thus reducing both radiological and nonradiological risk to the public. This paper describes the modeling and the results of comparison between measured and calculated isotopic inventories for a selected number of samples taken from a Yankee Rowe spent fuel assembly.

  20. The INE-Beamline for actinide science at ANKA

    SciTech Connect

    Rothe, J.; Dardenne, K.; Denecke, M. A.; Kienzler, B.; Loeble, M.; Metz, V.; Steppert, M.; Vitova, T.; Geckeis, H.; Butorin, S.; Seibert, A.; Walther, C.

    2012-04-15

    Since its inauguration in 2005, the INE-Beamline for actinide research at the synchrotron source ANKA (KIT North Campus) provides dedicated instrumentation for x-ray spectroscopic characterization of actinide samples and other radioactive materials. R and D work at the beamline focuses on various aspects of nuclear waste disposal within INE's mission to provide the scientific basis for assessing long-term safety of a final nuclear waste repository. The INE-Beamline is accessible for the actinide and radiochemistry community through the ANKA proposal system and the European Union Integrated Infrastructure Initiative ACTINET-I3. Experiments with activities up to 1 x 10{sup +6} times the European exemption limit are feasible within a safe but flexible containment concept. Measurements with monochromatic radiation are performed at photon energies varying between {approx}2.1 keV (P K-edge) and {approx}25 keV (Pd K-edge), including the lanthanide L-edges and the actinide M- and L3-edges up to Cf. The close proximity of the INE-Beamline to INE controlled area labs offers infrastructure unique in Europe for the spectroscopic and microscopic characterization of actinide samples. The modular beamline design enables sufficient flexibility to adapt sample environments and detection systems to many scientific questions. The well-established bulk techniques x-ray absorption fine structure (XAFS) spectroscopy in transmission and fluorescence mode have been augmented by advanced methods using a microfocused beam, including (confocal) XAFS/x-ray fluorescence detection and a combination of (micro-)XAFS and (micro-)x-ray diffraction. Additional instrumentation for high energy-resolution x-ray emission spectroscopy has been successfully developed and tested.

  1. Performance Measurement Analysis System

    1989-06-01

    The PMAS4.0 (Performance Measurement Analysis System) is a user-oriented system designed to track the cost and schedule performance of Department of Energy (DOE) major projects (MPs) and major system acquisitions (MSAs) reporting under DOE Order 5700.4A, Project Management System. PMAS4.0 provides for the analysis of performance measurement data produced from management control systems complying with the Federal Government''s Cost and Schedule Control Systems Criteria.

  2. Prompt fission neutron spectra of actinides

    DOE PAGES

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

    2016-01-06

    Here, 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.

  3. Lauriston S. Taylor Lecture: the quest for therapeutic actinide chelators.

    PubMed

    Durbin, Patricia W

    2008-11-01

    All of the actinides are radioactive. Taken into the body, they damage and induce cancer in bone and liver, and in the lungs if inhaled, and U(VI) is a chemical kidney poison. Containment of radionuclides is fundamental to radiation protection, but if it is breached accidentally or deliberately, decontamination of exposed persons is needed to reduce the consequences of radionuclide intake. The only known way to reduce the health risks of internally deposited actinides is to accelerate their excretion with chelating agents. Ethylendiaminetetraacetic acid (EDTA) and diethylenetriaminepentaacetic acid (DTPA) were introduced in the 1950's. DTPA is now clinically accepted, but its oral activity is low, it must be injected as a Ca(II) or Zn(II) chelate to avoid toxicity, and it is structurally unsuitable for chelating U(VI) or Np(V). Actinide penetration into the mammalian iron transport and storage systems suggested that actinide ions would form stable complexes with the Fe(III)-binding units found in potent selective natural iron chelators (siderophores). Testing of that biomimetic approach began in the late 1970's with the design, production, and assessment for in vivo Pu(IV) chelation of synthetic multidentate ligands based on the backbone structures and Fe(III)-binding groups of siderophores. New efficacious actinide chelators have emerged from that program, in particular, octadentate 3,4,3-LI(1,2-HOPO) and tetradentate 5-LIO(Me-3,2-HOPO) have potential for clinical acceptance. Both are much more effective than CaNa3-DTPA for decorporation of Pu(IV), Am(III), U(VI), and Np(IV,V), they are orally active, and toxicity is acceptably low at effective dosage.

  4. Separation of actinides from lanthanides

    DOEpatents

    Smith, Barbara F.; Jarvinen, Gordon D.; Ryan, Robert R.

    1989-01-01

    An organic extracting solution and an extraction method useful for separating elements of the actinide series of the periodic table from elements of the lanthanide series, where both are in trivalent form. The extracting solution consists of a primary ligand and a secondary ligand, preferably in an organic solvent. The primary ligand is a substituted monothio-1,3-dicarbonyl, which includes a substituted 4-acyl-2-pyrazolin-5-thione, such as 4-benzoyl-2,4-dihydro-5-methyl-2-phenyl-3H-pyrazol-3-thione (BMPPT). The secondary ligand is a substituted phosphine oxide, such as trioctylphosphine oxide (TOPO).

  5. Theoretical Studies of the Electronic Structure of the Compounds of the Actinide Elements

    SciTech Connect

    Kaltsoyannis, Nikolas; Hay, P. Jeffrey; Li, Jun; Blaudeau, Jean-Philippe; Bursten, Bruce E.

    2006-02-02

    In this chapter, we will present an overview of the theoretical and computational developments that have increased our understanding of the electronic structure of actinide-containing molecules and ions. The application of modern electronic structure methodologies to actinide systems remains one of the great challenges in quantum chemistry; indeed, as will be discussed below, there is no other portion of the periodic table that leads to the confluence of complexity with respect to the calculation of ground- and excited-state energies, bonding descriptions, and molecular properties. But there is also no place in the periodic table in which effective computational modeling of electronic structure can be more useful. The difficulties in creating, isolating, and handling many of the actinide elements provide an opportunity for computational chemistry to be an unusually important partner in developing the chemistry of these elements. The importance of actinide electronic structure begins with the earliest studies of uranium chemistry and predates the discovery of quantum mechanics. The fluorescence of uranyl compounds was observed as early as 1833 (Jørgensen and Reisfeld, 1983), a presage of the development of actinometry as a tool for measuring photochemical quantum yields. Interest in nuclear fuels has stimulated tremendous interest in understanding the properties, including electronic properties, of small actinide-containing molecules and ions, especially the oxides and halides of uranium and plutonium. The synthesis of uranocene in 1968 (Streitwieser and Mu¨ ller-Westerhoff, 1968) led to the flurry of activity in the organometallic chemistry of the actinides that continues today. Actinide organometallics (or organoactinides) are nearly always molecular systems and are often volatile, which makes them amenable to an arsenal of experimental probes of molecular and electronic structure (Marks and Fischer, 1979). Theoretical and computational studies of the electronic

  6. Actinide ion sensor for pyroprocess monitoring

    DOEpatents

    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.

  7. Exploring actinide materials through synchrotron radiation techniques.

    PubMed

    Shi, Wei-Qun; Yuan, Li-Yong; Wang, Cong-Zhi; Wang, Lin; Mei, Lei; Xiao, Cheng-Liang; Zhang, Li; Li, Zi-Jie; Zhao, Yu-Liang; Chai, Zhi-Fang

    2014-12-10

    Synchrotron radiation (SR) based techniques have been utilized with increasing frequency in the past decade to explore the brilliant and challenging sciences of actinide-based materials. This trend is partially driven by the basic needs for multi-scale actinide speciation and bonding information and also the realistic needs for nuclear energy research. In this review, recent research progresses on actinide related materials by means of various SR techniques were selectively highlighted and summarized, with the emphasis on X-ray absorption spectroscopy, X-ray diffraction and scattering spectroscopy, which are powerful tools to characterize actinide materials. In addition, advanced SR techniques for exploring future advanced nuclear fuel cycles dealing with actinides are illustrated as well.

  8. 237Np Mössbauer studies on actinide superconductors and related materials

    NASA Astrophysics Data System (ADS)

    Colineau, Eric; Gaczyński, Piotr; Griveau, Jean-Christophe; Eloirdi, Rachel; Caciuffo, Roberto

    2012-03-01

    Actinide materials play a special role in condensed matter physics, spanning behaviours of itinerant d-electron and localized 4f-electron materials. This duality of the 5f electrons confer to actinide-based intermetallic compounds a broad variety of physical properties such as magnetic or multipolar ordering, heavy fermion behaviour, quantum criticality, unconventional superconductivity... 237Np Mössbauer spectroscopy is a unique microscopic tool for gaining information on the electronic and magnetic properties of Np systems.

  9. Extraction of trivalent lanthanides and actinides by ``CMPO-like`` calixarenes

    SciTech Connect

    Delmau, L.H.; Simon, N.; Schwing-Weill, M.J.

    1999-04-01

    Extractive properties of calix[4]arenes bearing carbamoylmethylphosphine oxide moieties on their upper rim toward trivalent lanthanide and actinide cations were investigated. The study revealed that these molecules selectively extract light lanthanides and actinides from heavy lanthanides. All parameters present in the extraction system were varied to determine the origin of the selectivity. It was found that this selectivity requires a calix[4]arene platform and acetamidophosphine oxide groups containing phenyl substituents on the four phosphorus atoms.

  10. Development of a remote bushing for actinide vitrification

    SciTech Connect

    Schumacher, R.F.; Ramsey, W.G.; Johnson, F.M.

    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.

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

    NASA Astrophysics Data System (ADS)

    Karahan, Aydın

    2011-07-01

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

  12. Separation of actinides using capillary extraction chromatography-inductively coupled plasma mass spectrometry

    SciTech Connect

    Peterson, Dominic S

    2008-01-01

    Trace levels of actinides have been separated on extraction chromatography columns. Detection of the actinides was achieved using an inductively coupled plasma mass spectrometer (ICP-MS), which was coupled with the extraction chromatography system. In this study we compare 30 cm long, 4.6 mm ID columns to capillary columns (750 {micro}m ID) with lengths from 30 cm up to 150 cm. The columns that were tested were packed with TRU resin. We were able to separate a mixture of five actinides ({sup 232}Th, {sup 238}U, {sup 237}Np, {sup 239}pU, {sup 241}Am). This work has application to rapid bioassay as well as for automated separations of actinide materials.

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

    NASA Astrophysics Data System (ADS)

    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

  14. Evaluation of Homogeneous Options: Effects of Minor Actinide Exclusion from Single and Double Tier Recycle in Sodium Fast Reactors

    SciTech Connect

    R. M. Ferrer; S. Bays; M. Pope

    2008-03-01

    The Systems Analysis Campaign under the Global Nuclear Energy Partnership (GNEP) has requested the fuel cycle analysis group at the Idaho National Laboratory (INL) to analyze and provide isotopic data for four scenarios in which different strategies for Minor Actinides (MA) management are investigated. A 1000 MWth commercial-scale Sodium Fast Reactor (SFR) design was selected as the baseline in this scenario study. Two transuranic (TRU) conversion ratios, defined as the ratio of the amount of TRU produced over the TRU destroyed in the reactor core, along with different fuel-types were investigated.

  15. Electrochemical separation of actinides and fission products in molten salt electrolyte

    SciTech Connect

    Gay, R. L.; Grantham, L. F.; Fusselman, S. P.; Grimmett, D. L.; Roy, J. J.

    1995-09-15

    Molten salt electrochemical separation may be applied to accelerator-based conversion (ABC) and transmutation systems by dissolving the fluoride transport salt in LiCl-KCl eutectic solvent. The resulting fluoride-chloride mixture will contain small concentrations of fission product rare earths (La, Nd, Gd, Pr, Ce, Eu, Sm, and Y) and actinides (U, Np, Pu, Am, and Cm). The Gibbs free energies of formation of the metal chlorides are grouped advantageously such that the actinides can be deposited on a solid cathode with the majority of the rare earths remaining in the electrolyte. Thus, the actinides are recycled for further transmutation. Rockwell and its partners have measured the thermodynamic properties of the metal chlorides of interest (rare earths and actinides) and demonstrated separation of actinides from rare earths in laboratory studies. A model is being developed to predict the performance of a commercial electrochemical cell for separations starting with PUREX compositions. This model predicts excellent separation of plutonium and other actinides from the rare earths in metal-salt systems.

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

    NASA Astrophysics Data System (ADS)

    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

  17. BATSE spectroscopy analysis system

    NASA Technical Reports Server (NTRS)

    Schaefer, Bradley E.; Bansal, Sandhia; Basu, Anju; Brisco, Phil; Cline, Thomas L.; Friend, Elliott; Laubenthal, Nancy; Panduranga, E. S.; Parkar, Nuru; Rust, Brad

    1992-01-01

    The Burst and Transient Source Experiment (BATSE) Spectroscopy Analysis System (BSAS) is the software system which is the primary tool for the analysis of spectral data from BATSE. As such, Guest Investigators and the community as a whole need to know its basic properties and characteristics. Described here are the characteristics of the BATSE spectroscopy detectors and the BSAS.

  18. Experimental studies of actinides in molten salts

    SciTech Connect

    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.

  19. Decontamination of matrices containing actinide oxides

    SciTech Connect

    Villarreal, Robert

    1997-12-01

    There is provided a method for removing actinides and actinide oxides, particularly fired actinides, from soil and other contaminated matrices, comprising: (a) contacting a contaminated material with a solution of at least one inhibited fluoride and an acid to form a mixture; (b) heating the mixture of contaminated material and solution to a temperature in the range from about 30 C to about 90 C while stirring; (c) separating the solution from any undissolved matrix material in the mixture; (d) washing the undissolved matrix material to remove any residual materials; and (e) drying and returning the treated matrix material to the environment.

  20. Investigating Actinide Molecular Adducts From Absorption Edge Spectroscopy

    SciTech Connect

    Den Auwer, C.; Conradson, S.D.; Guilbaud, P.; Moisy, P.; Mustre de Leon, J.; Simoni, E.; /SLAC, SSRL

    2006-10-27

    Although Absorption Edge Spectroscopy has been widely applied to the speciation of actinide elements, specifically at the L{sub III} edge, understanding and interpretation of actinide edge spectra are not complete. In that sense, semi-quantitative analysis is scarce. In this paper, different aspects of edge simulation are presented, including semi-quantitative approaches. Comparison is made between various actinyl (U, Np) aquo or hydroxy compounds. An excursion into transition metal osmium chemistry allows us to compare the structurally related osmyl and uranyl hydroxides. The edge shape and characteristic features are discussed within the multiple scattering picture and the role of the first coordination sphere as well as contributions from the water solvent are described.

  1. Actinides in the Source of Cosmic Rays and the Present Interstellar Medium

    NASA Technical Reports Server (NTRS)

    Lingenfelter, R. E.; Higdon, J. C.; Kratz, K. -L.

    2003-01-01

    The abundances of the actinide elements in the cosmic rays can provide critical constraints on the major sites of their acceleration. Using recent calculations of the r-process yields in core collapse supernovae, we have determined the actinide abundances averaged over various assumed time intervals for their supernova generation and their cosmic-ray acceleration. Using standard Galactic chemical evolution models, we have also determined the expected actinide abundances in the present interstellar medium. From these two components, we have calculated the U/Th and other actinide abundances expected in the supernova-active cores of superbubbles, as a function of their ages and mean metallicity resulting from dilution with interstellar cloud debris. Then, using observations of the fractions of Galactic supernovae that occur in superbubbles and in the rest of the interstellar medium, we calculate the expected actinide abundances in cosmic rays accelerated by Galactic supernovae. We find that the current measurements of actinide/Pt-group and preliminary estimates of the UPuCm/Th ratio in cosmic rays are all consistent with the expected values if superbubble cores have mean metallicities of around 3 times solar. Such metallicities are quite comparable to the superbubble core metallicities inferred from other cosmic-ray observations. Future, more precise measurements of these ratios with experiments such as ECCO are needed to provide a better measure of the mean source metallicity sampled by the local Galactic cosmic rays. Measurements of the cosmic- ray actinide abundances have been favorably compared with the protosolar ratio, inferred from present solar system abundances, to infer that the cosmic rays are accelerated from the general interstellar medium. We suggest, however, that such an inference is not valid because the expected actinide abundances in the present interstellar medium are very different from the protosolar values, which sampled the interstellar medium

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

    SciTech Connect

    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.

  3. Actinide removal from spent salts

    DOEpatents

    Hsu, Peter C.; von Holtz, Erica H.; Hipple, David L.; Summers, Leslie J.; Adamson, Martyn G.

    2002-01-01

    A method for removing actinide contaminants (uranium and thorium) from the spent salt of a molten salt oxidation (MSO) reactor is described. Spent salt is removed from the reactor and analyzed to determine the contaminants present and the carbonate concentration. The salt is dissolved in water, and one or more reagents are added to precipitate the thorium as thorium oxide and/or the uranium as either uranium oxide or as a diuranate salt. The precipitated materials are filtered, dried and packaged for disposal as radioactive waste. About 90% of the thorium and/or uranium present is removed by filtration. After filtration, salt solutions having a carbonate concentration >20% can be dried and returned to the reactor for re-use. Salt solutions containing a carbonate concentration <20% require further clean-up using an ion exchange column, which yields salt solutions that contain less than 0.1 ppm of thorium or uranium.

  4. Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME

    SciTech Connect

    Johnson, Aaron T.; Nash, Kenneth L.

    2015-08-20

    The basic features of an f-element extraction process based on a solvent composed of equimolar mixtures of Cyanex-923 (a mixed trialkyl phosphine oxide) and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) extractants in n-dodecane are investigated in this report. This system, which combines features of the TRPO and TALSPEAK processes, is based on co-extraction of trivalent lanthanides and actinides from 0.1 to 1.0 M HNO3 followed by application of a buffered aminopolycarboxylate solution strip to accomplish a Reverse TALSPEAK selective removal of actinides. This mixed-extractant medium could enable a simplified approach to selective trivalent f-element extraction and actinide partitioning in a single process. As compared with other combined process applications in development for more compact actinide partitioning processes (DIAMEX-SANEX, GANEX, TRUSPEAK, ALSEP), this combination features only monofunctional extractants with high solubility limits and comparatively low molar mass. Selective actinide stripping from the loaded extractant phase is done using a glycine-buffered solution containing N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA) or triethylenetetramine-N,N,N',N'',N''',N'''-hexaacetic acid (TTHA). Lastly, the results reported provide evidence for simplified interactions between the two extractants and demonstrate a pathway toward using mixed monofunctional extractants to separate trivalent actinides (An) from fission product lanthanides (Ln).

  5. Mixed monofunctional extractants for trivalent actinide/lanthanide separations: TALSPEAK-MME

    DOE PAGES

    Johnson, Aaron T.; Nash, Kenneth L.

    2015-08-20

    The basic features of an f-element extraction process based on a solvent composed of equimolar mixtures of Cyanex-923 (a mixed trialkyl phosphine oxide) and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) extractants in n-dodecane are investigated in this report. This system, which combines features of the TRPO and TALSPEAK processes, is based on co-extraction of trivalent lanthanides and actinides from 0.1 to 1.0 M HNO3 followed by application of a buffered aminopolycarboxylate solution strip to accomplish a Reverse TALSPEAK selective removal of actinides. This mixed-extractant medium could enable a simplified approach to selective trivalent f-element extraction and actinide partitioning in a singlemore » process. As compared with other combined process applications in development for more compact actinide partitioning processes (DIAMEX-SANEX, GANEX, TRUSPEAK, ALSEP), this combination features only monofunctional extractants with high solubility limits and comparatively low molar mass. Selective actinide stripping from the loaded extractant phase is done using a glycine-buffered solution containing N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA) or triethylenetetramine-N,N,N',N'',N''',N'''-hexaacetic acid (TTHA). Lastly, the results reported provide evidence for simplified interactions between the two extractants and demonstrate a pathway toward using mixed monofunctional extractants to separate trivalent actinides (An) from fission product lanthanides (Ln).« less

  6. Actinide-Catalyzed Intermolecular Addition of Alcohols to Carbodiimides.

    PubMed

    Batrice, Rami J; Kefalidis, Christos E; Maron, Laurent; Eisen, Moris S

    2016-02-24

    The unprecedented actinide-catalyzed addition of alcohols to carbodiimides is presented. This represents a rare example of thorium-catalyzed transformations of an alcoholic substrate and the first example of uranium complexes showing catalytic reactivity with alcohols. Using the uranium and thorium amides U[N(SiMe3)2]3 and [(Me3Si)2N]2An[κ(2)-(N,C)-CH2Si(CH3)2N(SiMe3)] (An = Th or U), alcohol additions to unsaturated carbon-nitrogen bonds are achieved in short reaction times with excellent selectivities and high to excellent yields. Computational studies, supported by experimental thermodynamic data, suggest plausible models of the profile of the reaction which allow the system to overcome the high barrier of scission of the actinide-oxygen bond. Accompanied by experimentally determined kinetic parameters, a plausible mechanism is proposed for the catalytic cycle. PMID:26844823

  7. Accuracy Improvement of Neutron Nuclear Data on Minor Actinides

    NASA Astrophysics Data System (ADS)

    Harada, Hideo; Iwamoto, Osamu; Iwamoto, Nobuyuki; Kimura, Atsushi; Terada, Kazushi; Nakao, Taro; Nakamura, Shoji; Mizuyama, Kazuhito; Igashira, Masayuki; Katabuchi, Tatsuya; Sano, Tadafumi; Takahashi, Yoshiyuki; Takamiya, Koichi; Pyeon, Cheol Ho; Fukutani, Satoshi; Fujii, Toshiyuki; Hori, Jun-ichi; Yagi, Takahiro; Yashima, Hiroshi

    2015-05-01

    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.

  8. A literature review of actinide-carbonate mineral interactions

    SciTech Connect

    Stout, D.L.; Carroll, S.A.

    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.

  9. Joint Actinide Shock Physics Experimental Research - JASPER

    ScienceCinema

    None

    2016-07-12

    Commonly known as JASPER the Joint Actinide Shock Physics Experimental Research facility is a two stage light gas gun used to study the behavior of plutonium and other materials under high pressures, temperatures, and strain rates.

  10. BWR Assembly Optimization for Minor Actinide Recycling

    SciTech Connect

    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).

  11. Joint Actinide Shock Physics Experimental Research - JASPER

    SciTech Connect

    2014-10-31

    Commonly known as JASPER the Joint Actinide Shock Physics Experimental Research facility is a two stage light gas gun used to study the behavior of plutonium and other materials under high pressures, temperatures, and strain rates.

  12. Preparation of actinide targets by electrodeposition

    NASA Astrophysics Data System (ADS)

    Trautmann, N.; Folger, H.

    1989-10-01

    Actinide targets with varying thicknesses on different substrates have been prepared by electrodeposition either from aqueous solutions or from solutions of their nitrates in isopropyl alcohol. With these techniques the actinides can be deposited almost quantitatively on various backing materials within 15 to 30 min. Targets of thorium, uranium, neptunium, plutonium, americium, curium and californium with areal densities from almost carrier-free up to 1.4 mg/cm 2 on thin beryllium, carbon, titanium, tantalum and platinum foils have been prepared. In most cases, prior to the deposition, the actinides had to be purified chemically and for some of them, due to the limited amount of material available, recycling procedures were required. Applications of actinide targets in heavy-ion reactions are briefly discussed.

  13. PREPARATION OF ACTINIDE-ALUMINUM ALLOYS

    DOEpatents

    Moore, R.H.

    1962-09-01

    BS>A process is given for preparing alloys of aluminum with plutonium, uranium, and/or thorium by chlorinating actinide oxide dissolved in molten alkali metal chloride with hydrochloric acid, chlorine, and/or phosgene, adding aluminum metal, and passing air and/or water vapor through the mass. Actinide metal is formed and alloyed with the aluminum. After cooling to solidification, the alloy is separated from the salt. (AEC)

  14. Transmutation of actinides in power reactors.

    PubMed

    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.

  15. The Actinide Transition Revisited by Gutzwiller Approximation

    NASA Astrophysics Data System (ADS)

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

    2015-03-01

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

  16. Transmutation of actinides in power reactors.

    PubMed

    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. PMID:16604724

  17. Recent progress in actinide borate chemistry

    SciTech Connect

    Wang, Shuao; Alekseev, Evgeny V.; Depmeier, Wulf; Albrecht-Schmitt, Thomas E.

    2011-01-01

    The use of molten boric acid as a reactive flux for synthesizing actinide borates has been developed in the past two years providing access to a remarkable array of exotic materials with both unusual structures and unprecedented properties. [ThB₅O₆(OH)₆][BO(OH)₂]·2.5H₂O possesses a cationic supertetrahedral structure and displays remarkable anion exchange properties with high selectivity for TcO4- Uranyl borates form noncentrosymmetric structures with extraordinarily rich topological relationships. Neptunium borates are often mixed-valent and yield rare examples of compounds with one metal in three different oxidation states. Plutonium borates display new coordination chemistry for trivalent actinides. Finally, americium borates show a dramatic departure from plutonium borates, and there are scant examples of families of actinides compounds that extend past plutonium to examine the bonding of later actinides. There are several grand challenges that this work addresses. The foremost of these challenges is the development of structure-property relationships in transuranium materials. A deep understanding of the materials chemistry of actinides will likely lead to the development of advanced waste forms for radionuclides present in nuclear waste that prevent their transport in the environment. This work may have also uncovered the solubility-limiting phases of actinides in some repositories, and allows for measurements on the stability of these materials.

  18. Recent progress in actinide borate chemistry.

    PubMed

    Wang, Shuao; Alekseev, Evgeny V; Depmeier, Wulf; Albrecht-Schmitt, Thomas E

    2011-10-21

    The use of molten boric acid as a reactive flux for synthesizing actinide borates has been developed in the past two years providing access to a remarkable array of exotic materials with both unusual structures and unprecedented properties. [ThB(5)O(6)(OH)(6)][BO(OH)(2)]·2.5H(2)O possesses a cationic supertetrahedral structure and displays remarkable anion exchange properties with high selectivity for TcO(4)(-). Uranyl borates form noncentrosymmetric structures with extraordinarily rich topological relationships. Neptunium borates are often mixed-valent and yield rare examples of compounds with one metal in three different oxidation states. Plutonium borates display new coordination chemistry for trivalent actinides. Finally, americium borates show a dramatic departure from plutonium borates, and there are scant examples of families of actinides compounds that extend past plutonium to examine the bonding of later actinides. There are several grand challenges that this work addresses. The foremost of these challenges is the development of structure-property relationships in transuranium materials. A deep understanding of the materials chemistry of actinides will likely lead to the development of advanced waste forms for radionuclides present in nuclear waste that prevent their transport in the environment. This work may have also uncovered the solubility-limiting phases of actinides in some repositories, and allows for measurements on the stability of these materials.

  19. Systems Analysis Sub site

    SciTech Connect

    EERE

    2012-03-16

    Systems analysis provides direction, focus, and support for the development and introduction of hydrogen production, storage, and end-use technologies, and provides a basis for recommendations on a balanced portfolio of activities.

  20. Enhanced techniques for the measurement of ultra-low level (pg and fg) actinide analysis by ICP-MS for forensic and geologic applications

    NASA Astrophysics Data System (ADS)

    Pollington, A. D.; Kinman, W.; Hanson, S. K.

    2014-12-01

    and accuracy of actinide isotope measurements and what procedures can be applied to minimize interferences.

  1. Magnetic measurements of the transuranium elements and charge state characterization of actinides in monazite. Progress report

    SciTech Connect

    Huray, P. G.

    1980-01-01

    A micromagnetic susceptometer for the purpose of measuring extremely small sample quantities (on the microgram level) was designed, constructed, and calibrated in previous years. (The 1979 progress report gives details of its operation.) This device has operated without significant downtime in this funding period, and much progress has been made in the magnetic characterization of elements beyond Am in the periodic table. This program has roughly doubled man's knowledge of magnetism in Cm, Bk, and Cf, and includes the only Es magnetic measurements to date. The incorporation of an automatic data collection system in this period has made analysis much more accurate, and has allowed quicker turnaround of compounds and metals for study. Results obtained for the compounds and metals studied this year are summarized. The lanthanide orthophosphates are being investigated as an alternate means of primary containment for high-level actinide wastes. Researchers at the Oak Ridge National Laboratory are involved in preparation of actinide-doped compounds for all of the lanthanide transition series (La through Lu) for a study of leaching characteristics and E.S.R. classification. To aid this study the charge state of /sup 237/Np or /sup 57/Fe has been identified, either in the as-prepared compounds or following radioactive decay of /sup 241/Am via the Moessbauer Effect. The final charge state will be an influential variable in the immobilization characteristics of the waste products stored in this synthetic monazite form. 10 figures, 1 table. (RWR)

  2. Design of an electrochemically assisted radiation sensor for α-spectrometry of actinides traces in water.

    PubMed

    de Sanoit, Jacques; Quang Tran, Thuan; Pomorski, Michal; Pierre, Sylvie; Mer-Calfati, Christine; Bergonzo, Philippe

    2013-10-01

    We describe a new approach for the detection and identification of actinides at low activity levels directly in aqueous solution. The measurement consists initially, in immobilizing alpha emitters in the form of insoluble hydroxides onto the entrance window of an immersed alpha particles detector. For this, a boron doped diamond detector window is negatively polarized to produce a basic layer on its surface by water decomposition. Actinides elements that are known to be very sensitive to hydrolysis are precipitated as solid hydroxides onto the entrance window of the sensor. Due to the absence of an air layer between the radioactive source and the detector, there is no need for vacuum during the alpha spectrometry measurement. After analysis, the detector can be easily cleaned by anodization in the aqueous medium to be reused at once. The minimum detectable activity concentration (MDA) of the system has been evaluated with (241)Am at 0.5 Bq/L for a 0.33 cm(2) area Si PIN diode. PMID:23816879

  3. Multidisciplinary System Reliability Analysis

    NASA Technical Reports Server (NTRS)

    Mahadevan, Sankaran; Han, Song; Chamis, Christos C. (Technical Monitor)

    2001-01-01

    The objective of this study is to develop a new methodology for estimating the reliability of engineering systems that encompass multiple disciplines. The methodology is formulated in the context of the NESSUS probabilistic structural analysis code, developed under the leadership of NASA Glenn Research Center. The NESSUS code has been successfully applied to the reliability estimation of a variety of structural engineering systems. This study examines whether the features of NESSUS could be used to investigate the reliability of systems in other disciplines such as heat transfer, fluid mechanics, electrical circuits etc., without considerable programming effort specific to each discipline. In this study, the mechanical equivalence between system behavior models in different disciplines are investigated to achieve this objective. A new methodology is presented for the analysis of heat transfer, fluid flow, and electrical circuit problems using the structural analysis routines within NESSUS, by utilizing the equivalence between the computational quantities in different disciplines. This technique is integrated with the fast probability integration and system reliability techniques within the NESSUS code, to successfully compute the system reliability of multidisciplinary systems. Traditional as well as progressive failure analysis methods for system reliability estimation are demonstrated, through a numerical example of a heat exchanger system involving failure modes in structural, heat transfer and fluid flow disciplines.

  4. Redox response of actinide materials to highly ionizing radiation.

    PubMed

    Tracy, Cameron L; Lang, Maik; Pray, John M; Zhang, Fuxiang; Popov, Dmitry; Park, Changyong; Trautmann, Christina; Bender, Markus; Severin, Daniel; Skuratov, Vladimir A; Ewing, Rodney C

    2015-01-01

    Energetic radiation can cause dramatic changes in the physical and chemical properties of actinide materials, degrading their performance in fission-based energy systems. As advanced nuclear fuels and wasteforms are developed, fundamental understanding of the processes controlling radiation damage accumulation is necessary. Here we report oxidation state reduction of actinide and analogue elements caused by high-energy, heavy ion irradiation and demonstrate coupling of this redox behaviour with structural modifications. ThO2, in which thorium is stable only in a tetravalent state, exhibits damage accumulation processes distinct from those of multivalent cation compounds CeO2 (Ce(3+) and Ce(4+)) and UO3 (U(4+), U(5+) and U(6+)). The radiation tolerance of these materials depends on the efficiency of this redox reaction, such that damage can be inhibited by altering grain size and cation valence variability. Thus, the redox behaviour of actinide materials is important for the design of nuclear fuels and the prediction of their performance.

  5. ORIGEN2 simulation of the Los Alamos accelerator-driven transmutation system

    SciTech Connect

    Landeyro, P.A. ); Buccafurni, A.; Orazi, A. )

    1992-01-01

    This work aims at analyzing different actinide-burning systems to evaluate their performance and verify the possibility of eliminating, or at least reducing, the storage time for nuclear wastes in the final repository. To achieve these goals, two steps are added to the normal fuel cycle: partitioning and transmutation. In the partitioning step, the actinides are extracted from the high-level wastes produced in reprocessing plants, while during the transmutation step, the actinides are burned. To evaluate the potential performance of the different systems suitable for actinide transmutation, it is necessary to determine and analyze the parameters that influence actinide burning as well as to compare the potential risk due to the waste produced by each system with that associated with radioactive materials existing in nature. Another important parameter to consider is the ratio between the transmutation and generation rates, which shows how fast the system burns actinides. For these considerations, an analysis of the parameters that influence actinide burning are followed by an evaluation by means of the ORIGEN2 generation and depletion code that is as accurate as possible.

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

    PubMed

    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.

  7. Applicability of RELAP5-3D for Thermal-Hydraulic Analyses of a Sodium-Cooled Actinide Burner Test Reactor

    SciTech Connect

    C. B. Davis

    2006-07-01

    The Actinide Burner Test Reactor (ABTR) is envisioned as a sodium-cooled, fast reactor that will burn the actinides generated in light water reactors to reduce nuclear waste and ease proliferation concerns. The RELAP5-3D computer code is being considered as the thermal-hydraulic system code to support the development of the ABTR. An evaluation was performed to determine the applicability of RELAP5-3D for the analysis of a sodium-cooled fast reactor. The applicability evaluation consisted of several steps, including identifying the important transients and phenomena expected in the ABTR, identifying the models and correlations that affect the code’s calculation of the important phenomena, and evaluating the applicability of the important models and correlations for calculating the important phenomena expected in the ABTR. The applicability evaluation identified code improvements and additional models needed to simulate the ABTR. The accuracy of the calculated thermodynamic and transport properties for sodium was also evaluated.

  8. Space lab system analysis

    NASA Technical Reports Server (NTRS)

    Rives, T. B.; Ingels, F. M.

    1988-01-01

    An analysis of the Automated Booster Assembly Checkout System (ABACS) has been conducted. A computer simulation of the ETHERNET LAN has been written. The simulation allows one to investigate different structures of the ABACS system. The simulation code is in PASCAL and is VAX compatible.

  9. Data analysis systems.

    NASA Astrophysics Data System (ADS)

    Wells, Donald C.

    The following sections are included: * INTRODUCTION * WHY SYSTEMS? * PROJECT MANAGEMENT REASONS * TECHNICAL REASONS * THE TIME-SCALE PROBLEM * WHAT END-USERS WANT * DATA INTERCHANGE FORMATS * PROJECT MANAGEMENT ISSUES * THE EXPORT POLICY * GROUP PROGRAMMING PSYCHOLOGY * THE CASE FOR SYSTEM PORTABILITY * HOW TO BUILD PORTABLE DATA ANALYSIS SYSTEMS * ON THE DESIGN OF COMMAND LANGUAGES * LAYERED VIRTUAL INTERFACES IN AIPS * STATUS REPORT ON NRAO'S AIPS PROJECT * AIPS DEVELOPMENT PLANS * CONCLUSION * DISCUSSION * REFERENCES * BIBLIOGRAPHY—FOR FURTHER READING

  10. CONVEYOR SYSTEM SAFETY ANALYSIS

    SciTech Connect

    M. Salem

    1995-06-23

    The purpose and objective of this analysis is to systematically identify and evaluate hazards related to the Yucca Mountain Project Exploratory Studies Facility (ESF) surface and subsurface conveyor system (for a list of conveyor subsystems see section 3). This process is an integral part of the systems engineering process; whereby safety is considered during planning, design, testing, and construction. A largely qualitative approach was used since a radiological System Safety Analysis is not required. The risk assessment in this analysis characterizes the accident scenarios associated with the conveyor structures/systems/components in terms of relative risk and includes recommendations for mitigating all identified risks. The priority for recommending and implementing mitigation control features is: (1) Incorporate measures to reduce risks and hazards into the structure/system/component (S/S/C) design, (2) add safety devices and capabilities to the designs that reduce risk, (3) provide devices that detect and warn personnel of hazardous conditions, and (4) develop procedures and conduct training to increase worker awareness of potential hazards, on methods to reduce exposure to hazards, and on the actions required to avoid accidents or correct hazardous conditions. The scope of this analysis is limited to the hazards related to the design of conveyor structures/systems/components (S/S/Cs) that occur during normal operation. Hazards occurring during assembly, test and maintenance or ''off normal'' operations have not been included in this analysis. Construction related work activities are specifically excluded per DOE Order 5481.1B section 4. c.

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

    SciTech Connect

    Greenspan, Ehud; Todreas, Neil; Taiwo, Temitope

    2009-03-10

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

  12. Coal systems analysis

    SciTech Connect

    Warwick, P.D.

    2005-07-01

    This collection of papers provides an introduction to the concept of coal systems analysis and contains examples of how coal systems analysis can be used to understand, characterize, and evaluate coal and coal gas resources. Chapter are: Coal systems analysis: A new approach to the understanding of coal formation, coal quality and environmental considerations, and coal as a source rock for hydrocarbons by Peter D. Warwick. Appalachian coal assessment: Defining the coal systems of the Appalachian Basin by Robert C. Milici. Subtle structural influences on coal thickness and distribution: Examples from the Lower Broas-Stockton coal (Middle Pennsylvanian), Eastern Kentucky Coal Field, USA by Stephen F. Greb, Cortland F. Eble, and J.C. Hower. Palynology in coal systems analysis The key to floras, climate, and stratigraphy of coal-forming environments by Douglas J. Nichols. A comparison of late Paleocene and late Eocene lignite depositional systems using palynology, upper Wilcox and upper Jackson Groups, east-central Texas by Jennifer M.K. O'Keefe, Recep H. Sancay, Anne L. Raymond, and Thomas E. Yancey. New insights on the hydrocarbon system of the Fruitland Formation coal beds, northern San Juan Basin, Colorado and New Mexico, USA by W.C. Riese, William L. Pelzmann, and Glen T. Snyder.

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

    SciTech Connect

    Judge, Elizabeth J.; Berg, John M.; Le, Loan A.; Lopez, Leon N.; Barefield, James E.

    2012-06-18

    interactions occurring within the plasma, such as collisional energy transfer, that might be a factor in the reduction in neptunium emission lines. Neptunium has to be analyzed alone using LIBS to further understand the dynamics that may be occurring in the plasma of the mixed actinide fuel pellet sample. The LIBS data suggests that the emission spectrum for the mixed actinide fuel pellet is not simply the sum of the emission spectra of the pure samples but is dependent on the species present in the plasma and the interactions and reactions that occur within the plasma. Finally, many of the neptunium lines are in the near infrared region which is drastically reduced in intensity by the current optical setup and possibly the sensitivity of the emission detector in the spectral region. Once the optics are replaced and the optical collection system is modified and optimized, the probability of observing emission lines for neptunium might be increased significantly. The mixed actinide fuel pellet was analyzed under the experimental conditions listed in Table 1. The LIBS spectra of the fuel pellet are shown in Figures 1-49. The spectra are labeled with the observed wavelength and atomic species (both neutral (I) and ionic (II)). Table 2 is a complete list of the observed and literature based emission wavelengths. The literature wavelengths have references including NIST Atomic Spectra Database (NIST), B.A. Palmer et al. 'An Atlas of Uranium Emission Intensities in a Hollow Cathode Discharge' taken at the Kitt Peak National Observatory (KPNO), R.L. Kurucz 1995 Atomic Line Data from the Smithsonian Astrophysical Observatory (SAO), J. Blaise et al. 'The Atomic Spectrum of Plutonium' from Argonne National Laboratory (BFG), and M. Fred and F.S. Tomkins, 'Preliminary Term Analysis of Am I and Am II Spectra' (FT). The dash (-) shown under Ionic State indicates that the ionic state of the transition was not available. In the spectra, the dash (-) is replaced with a question mark (?). Peaks

  14. Actinide production in /sup 136/Xe bombardments of /sup 249/Cf

    SciTech Connect

    Gregorich, K.E.

    1985-08-01

    The production cross sections for the actinide products from /sup 136/Xe bombardments of /sup 249/Cf at energies 1.02, 1.09, and 1.16 times the Coulomb barrier were determined. Fractions of the individual actinide elements were chemically separated from recoil catcher foils. The production cross sections of the actinide products were determined by measuring the radiations emitted from the nuclides within the chemical fractions. The chemical separation techniques used in this work are described in detail, and a description of the data analysis procedure is included. The actinide production cross section distributions from these /sup 136/Xe + /sup 249/Cf bombardments are compared with the production cross section distributions from other heavy ion bombardments of actinide targets, with emphasis on the comparison with the /sup 136/Xe + /sup 248/Cm reaction. A technique for modeling the final actinide cross section distributions has been developed and is presented. In this model, the initial (before deexcitation) cross section distribution with respect to the separation energy of a dinuclear complex and with respect to the Z of the target-like fragment is given by an empirical procedure. It is then assumed that the N/Z equilibration in the dinuclear complex occurs by the transfer of neutrons between the two participants in the dinuclear complex. The neutrons and the excitation energy are statistically distributed between the two fragments using a simple Fermi gas level density formalism. The resulting target-like fragment initial cross section distribution with respect to Z, N, and excitation energy is then allowed to deexcite by emission of neutrons in competition with fission. The result is a final cross section distribution with respect to Z and N for the actinide products. 68 refs., 33 figs., 6 tabs.

  15. Biomedical systems analysis program

    NASA Technical Reports Server (NTRS)

    1979-01-01

    Biomedical monitoring programs which were developed to provide a system analysis context for a unified hypothesis for adaptation to space flight are presented and discussed. A real-time system of data analysis and decision making to assure the greatest possible crew safety and mission success is described. Information about man's abilities, limitations, and characteristic reactions to weightless space flight was analyzed and simulation models were developed. The predictive capabilities of simulation models for fluid-electrolyte regulation, erythropoiesis regulation, and calcium regulation are discussed.

  16. Nonaqueous method for dissolving lanthanide and actinide metals

    DOEpatents

    Crisler, L.R.

    1975-11-11

    Lanthanide and actinide beta-diketonate complex molecular compounds are produced by reacting a beta-diketone compound with a lanthanide or actinide element in the elemental metallic state in a mixture of carbon tetrachloride and methanol.

  17. Actinides AMS at CIRCE in Caserta (Italy)

    NASA Astrophysics Data System (ADS)

    De Cesare, M.; Gialanella, L.; Rogalla, D.; Petraglia, A.; Guan, Y.; De Cesare, N.; D'Onofrio, A.; Quinto, F.; Roca, V.; Sabbarese, C.; Terrasi, F.

    2010-04-01

    The operation of Nuclear Power Plants and atmospheric tests of nuclear weapons performed in the past, together with production, transport and reprocessing of nuclear fuel, lead to the release into the environment of a wide range of radioactive nuclides, such as uranium, plutonium, fission and activation products. These nuclides are present in the environment at ultra trace levels. Their detection requires sensitive techniques like AMS (Accelerator Mass Spectrometry). In order to perform isotopic ratio measurements of the longer-lived actinides, e.g., of 236U relative to the primary 238U and various Pu isotopes relative to 239Pu, an upgrade of the CIRCE accelerator (Center for Isotopic Research on Cultural and Environmental Heritage) in Caserta, Italy, is underway. In this paper we report on the results of simulations aiming to define the best ion optics and to understand the origin of possible measurement background. The design of a high resolution TOF- E (Time of Flight-Energy) detector system is described, which will be used to identify the rare isotopes among interfering background signals.

  18. Correlation and relativistic effects in actinide ions

    SciTech Connect

    Safronova, U. I.; Safronova, M. S.

    2011-11-15

    Wavelengths, line strengths, and transition rates are calculated for the multipole (E1, M1, E2, M2, E3, and M3) transitions between the excited 6s{sup 2}6p{sup 5}nl and 6s6p{sup 6}nl states and the ground 6s{sup 2}6p{sup 6} state in Ac{sup 3+}, Th{sup 4+}, and U{sup 6+} Rn-like ions. Relativistic many-body perturbation theory (RMBPT), including the Breit interaction, is used to evaluate energies and transition rates for multipole transitions in these hole-particle systems. The RMBPT method agrees with multiconfigurational Dirac-Fock (MCDF) calculations in lowest order, includes all second-order correlation corrections, and includes corrections from negative-energy states. The calculations start from a [Xe]4f{sup 14}5d{sup 10}6s{sup 2}6p{sup 6} Dirac-Fock potential. First-order perturbation theory is used to obtain intermediate-coupling coefficients, and second-order RMBPT is used to determine the matrix elements. Evaluated multipole matrix elements for transitions from excited states to the ground states are used to determine the line strengths, transition rates, and multipole polarizabilities. This work provides a number of yet unmeasured properties of these actinide ions for various applications and for benchmark tests of theory and experiment.

  19. Microcomputer log analysis system

    SciTech Connect

    Ostrander, C.

    1984-04-01

    A comprehensive friendly log analysis system for use on a microcomputer requires only average log analysis skills. Most systems require both log analysis and computer professional for operation. This one has many capabilities: (1) data entry is handled by office personnel after minimal training; (2) entered data is filed and cataloged for future retrieval and analysis; (3) the system can handle more than 9,000,000 ft (2700 km) of log data in over 60,000 files; (4) all data can be edited; (5) searches and listings can be made using factors such as formation names; (6) facsimile reproductions can be made of any log on file; (7) a screening program turns the system into a sophisticated hand calculator to quickly determine zones of interest; and (8) up to 1100 ft (335 m) of contiguous data from a well can be analyzed in one run. Innovative features include: (1) a discriminating factor to separate reservoirs for individual attention concerning rock type, fluid content and potential reserves; and (2) a written report of each reservoir using artificial intelligence. The report discusses, among other things, the rock type and its consistency, comparing the system finding with the geologist's opinion. Differences between the two will elicit alternative analyses.

  20. Prediction of dissolved actinide concentrations in concentrated electrolyte solutions: a conceptual model and model results for the Waste Isolation Pilot Plant (WIPP)

    SciTech Connect

    Novak, C.F.; Moore, R.C.; Bynum, R.V.

    1996-10-25

    The conceptual model for WIPP dissolved concentrations is a description of the complex natural and artificial chemical conditions expected to influence dissolved actinide concentrations in the repository. By a set of physical and chemical assumptions regarding chemical kinetics, sorption substrates, and waste-brine interactions, the system was simplified to be amenable to mathematical description. The analysis indicated that an equilibrium thermodynamic model for describing actinide solubilities in brines would be tractable and scientifically supportable. This paper summarizes the conceptualization and modeling approach and the computational results as used in the WIPP application for certification of compliance with relevant regulations for nuclear waste repositories. The WIPP site contains complex natural brines ranging from sea water to 10x more concentrated than sea water. Data bases for predicting solubility of Am(III) (as well as Pu(III) and Nd(III)), Th(IV), and Np(V) in these brines under potential repository conditions have been developed, focusing on chemical interactions with Na, K, Mg, Cl, SO{sub 4}, and CO{sub 3} ions, and the organic acid anions acetate, citrate, EDTA, and oxalate. The laboratory and modeling effort augmented the Harvie et al. parameterization of the Pitzer activity coefficient model so that it could be applied to the actinides and oxidation states important to the WIPP system.

  1. Application of chemical structure and bonding of actinide oxide materials for forensic science

    SciTech Connect

    Wilkerson, Marianne Perry

    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.

  2. Vitrification of actinide solutions in SRS separations facilities

    SciTech Connect

    Minichan, R.L.; Ramsey, W.G.

    1995-09-01

    The actinide vitrification system being developed at SRS provides the capability to convert specialized or unique forms of nuclear material into a stable solid glass product that can be safely shipped, stored or reprocessed according to the DOE complex mission. This project is an application of technology developed through funds from the Office of Technology Development (OTD). This technology is ideally suited for vitrifying relatively small quantities of fissile or special nuclear material since it is designed to be critically safe. Successful demonstration of this system to safely vitrify radioactive material could open up numerous opportunities for transferring this technology to applications throughout the DOE complex.

  3. Digital Systems Analysis

    ERIC Educational Resources Information Center

    Martin, Vance S.

    2009-01-01

    There have been many attempts to understand how the Internet affects our modern world. There have also been numerous attempts to understand specific areas of the Internet. This article applies Immanuel Wallerstein's World Systems Analysis to our informationalist society. Understanding this world as divided among individual core, semi-periphery,…

  4. VENTILATION TECHNOLOGY SYSTEMS ANALYSIS

    EPA Science Inventory

    The report gives results of a project to develop a systems analysis of ventilation technology and provide a state-of-the-art assessment of ventilation and indoor air quality (IAQ) research needs. (NOTE: Ventilation technology is defined as the hardware necessary to bring outdoor ...

  5. Complexation of Actinides in Solution: Thermodynamic Measurementsand Structural Characterization

    SciTech Connect

    Rao, L.

    2007-02-01

    This paper presents a brief introduction of the studies of actinide complexation in solution at Lawrence Berkeley National Laboratory. An integrated approach of thermodynamic measurements and structural characterization is taken to obtain fundamental understanding of actinide complexation in solution that is of importance in predicting the behavior of actinides in separation processes and environmental transport.

  6. The Actinide-Lanthanide Separation Process

    SciTech Connect

    Lumetta, Gregg J.; Gelis, Artem V.; Carter, Jennifer C.; Niver, Cynthia M.; Smoot, Margaret R.

    2014-02-21

    The Actinide-Lanthanide SEParation (ALSEP) process is described. The process uses an extractant phase consisting of either N,N,N',N'-tetraoctyldiglycolamide (TODGA) or N,N,N',N'-tetra(2 ethylhexyl)diglycolamide (T2EHDGA) combined with 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]). The neutral TODGA or T2EHDGA serves to co-extract the trivalent actinide and lanthanide ions from nitric acid media. Switching the aqueous phase chemistry to a citrate buffered diethylenetriaminepentaacetic acid (DTPA) solution at pH 2.5 to 4 results in selective transfer of the actinides to the aqueous phase, thus resulting in separation of these two groups of elements.

  7. THEORY FOR THE XPS OF ACTINIDES

    SciTech Connect

    Bagus, Paul S.; Ilton, Eugene S.

    2013-08-01

    Two aspects of the electronic structure of actinide oxides that significantly affect the XPS spectra are described; these aspects are also important for the materials properties of the oxides. The two aspects considered are: (1) The spin-orbit coupling of the open 5f shell electrons in actinide cations and how this coupling affects the electronic structure. And, (2) the covalent character of the metal oxygen interaction in actinide compounds. Because of this covalent character, there are strong departures from the nominal oxidation states that are significantly larger in core-hole states than in the ground state. The consequences for the XPS of this covalent character are examined. A proper understanding of the way in which they influence the XPS makes it possible to use the XPS to correctly characterize the electronic structure of the oxides.

  8. Actinide separations by supported liquid membranes

    SciTech Connect

    Danesi, P.R.; Horwitz, E.P.; Rickert, P.; Chiarizia, R.

    1984-01-01

    The work has demonstrated that actinide removal from synthetic waste solutions using both flat-sheet and hollow-fiber SLM's is a feasible chemical process at the laboratory scale level. The process is characterized by the typical features of SLM's processes: very small quantities of extractant required; the potential for operations with high feed/strip volume ratios, resulting in a corresponding concentration factor of the actinides; and simplicity of operation. Major obstacles to the implementation of the SLM technology to the decontamination of liquid nuclear wastes are the probable low resistance of polypropylene supports to high radiation fields, which may prevent the application to high-level nuclear wastes; the unknown lifetime of the SLM; and the high Na content of the separated actinide solution.

  9. Probing the population of the spin-orbit split levels in the actinide 5f states.

    PubMed

    Moore, K T; van der Laan, G; Tobin, J G; Chung, B W; Wall, M A; Schwartz, A J

    2006-03-01

    Spin-orbit interaction in the 5f states is believed to strongly influence exotic behaviors observed in actinide metals and compounds. Understanding these interactions and how they relate to the actinide series is of considerable importance. To address this issue, the branching ratio of the white-line peaks of the N4,5 edge for the light actinide metals, alpha-Th, alpha-U, and alpha-Pu were recorded using electron energy-loss spectroscopy (EELS) in a transmission electron microscope (TEM) and synchrotron-radiation-based X-ray absorption spectroscopy (XAS). Using the spin-orbit sum rule and the branching ratios from both experimental spectra and many-electron atomic spectral calculations, accurate values of the spin-orbit interaction, and thus the relative occupation of the j = 5/2 and 7/2 levels, are determined for the actinide 5f states. Results show that the spin-orbit sum rule works very well with both EELS and XAS spectra, needing little or no correction. This is important, since the high spatial resolution of a TEM can be used to overcome the problems of single-crystal growth often encountered with actinide metals, allowing acquisition of EELS spectra, and subsequent spin-orbit analysis, from nm-sized regions. The relative occupation numbers obtained by our method have been compared with recent theoretical results and they show a good agreement in their trend.

  10. Plutonium and minor actinide utilisation in a pebble-bed high temperature reactor

    SciTech Connect

    Petrov, B. Y.; Kuijper, J. C.; Oppe, J.; De Haas, J. B. M.

    2012-07-01

    This paper contains results of the analysis of the pebble-bed high temperature gas-cooled PUMA reactor loaded with plutonium and minor actinide (Pu/MA) fuel. Starting from knowledge and experience gained in the Euratom FP5 projects HTR-N and HTR-N1, this study aims at demonstrating the potential of high temperature reactors to utilize or transmute Pu/MA fuel. The work has been performed within the Euratom FP6 project PUMA. A number of different fuel types and fuel configurations have been analyzed and compared with respect to incineration performance and safety-related reactor parameters. The results show the excellent plutonium and minor actinide burning capabilities of the high temperature reactor. The largest degree of incineration is attained in the case of an HTR fuelled by pure plutonium fuel as it remains critical at very deep burnup of the discharged pebbles. Addition of minor actinides to the fuel leads to decrease of the achievable discharge burnup and therefore smaller fraction of actinides incinerated during reactor operation. The inert-matrix fuel design improves the transmutation performance of the reactor, while the 'wallpaper' fuel does not have advantage over the standard fuel design in this respect. After 100 years of decay following the fuel discharge, the total amount of actinides remains almost unchanged for all of the fuel types considered. Among the plutonium isotopes, only the amount of Pu-241 is reduced significantly due to its relatively short half-life. (authors)

  11. Experimental and simulated assay of actinides in a real waste package

    NASA Astrophysics Data System (ADS)

    Saurel, N.; Capdevila, J. M.; Huot, N.; Gmar, M.

    2005-09-01

    The non-destructive control of nuclear wastes is important for their management and the non-proliferation. Among the methods using the nuclear radiation as an investigation, the Instrumental Photon Activation Analysis (IPAA) seems to be a promising way to quantify the masses of actinides present in bulky packages of nuclear waste. The IPAA method consists in irradiating actinides with photons of high energy to produce photofission reactions. The counting of the delayed neutrons, produced by these photofission reactions, allows to locate and to quantify the mass of actinides by tomography. At this end, we use a simulation tool named OPERA to obtain the information necessary for the tomographic restitution and an experimental installation based on a LINear ACcelerator (LINAC) to perform the measurements. The high-energy photons (11 MeV) are produced by Bremsstrahlung, thanks to a tungsten target placed in front of the LINAC. In this paper, we present the first experimental results obtained on a real package of nuclear waste. We establish that, for this waste package, the limit of detection, in terms of mass of actinides, is about 1 g. Furthermore, these results show the good agreement between the experiment and the simulation that provides a localization of actinides by tomography.

  12. Neptune Aerocapture Systems Analysis

    NASA Technical Reports Server (NTRS)

    Lockwood, Mary Kae

    2004-01-01

    A Neptune Aerocapture Systems Analysis is completed to determine the feasibility, benefit and risk of an aeroshell aerocapture system for Neptune and to identify technology gaps and technology performance goals. The high fidelity systems analysis is completed by a five center NASA team and includes the following disciplines and analyses: science; mission design; aeroshell configuration screening and definition; interplanetary navigation analyses; atmosphere modeling; computational fluid dynamics for aerodynamic performance and database definition; initial stability analyses; guidance development; atmospheric flight simulation; computational fluid dynamics and radiation analyses for aeroheating environment definition; thermal protection system design, concepts and sizing; mass properties; structures; spacecraft design and packaging; and mass sensitivities. Results show that aerocapture can deliver 1.4 times more mass to Neptune orbit than an all-propulsive system for the same launch vehicle. In addition aerocapture results in a 3-4 year reduction in trip time compared to all-propulsive systems. Aerocapture is feasible and performance is adequate for the Neptune aerocapture mission. Monte Carlo simulation results show 100% successful capture for all cases including conservative assumptions on atmosphere and navigation. Enabling technologies for this mission include TPS manufacturing; and aerothermodynamic methods and validation for determining coupled 3-D convection, radiation and ablation aeroheating rates and loads, and the effects on surface recession.

  13. The gastrointestinal absorption of the actinide elements.

    PubMed

    Harrison, J D

    1991-03-01

    The greatest uncertainty in dose estimates for the ingestion of long-lived, alpha-emitting isotopes of the actinide elements is in the values used for their fractional absorption from the gastrointestinal tract (f1 values). Recent years have seen a large increase in the available data on actinide absorption. Human data are reviewed here, together with animal data, to illustrate the effect on absorption of chemical form, incorporation into food materials, fasting and other dietary factors, and age at ingestion. The f1 values recommended by the International Commission on Radiological Protection, by an Expert Group of the Nuclear Energy Agency and by the National Radiological Protection Board are discussed.

  14. Elevated concentrations of actinides in mono lake.

    PubMed

    Anderson, R F; Bacon, M P; Brewer, P G

    1982-04-30

    Tetravalent thorium, pentavalent protactinium, hexavalent uranium, and plutonium (oxidation state uncertain) are present in much higher concentrations in Mono Lake, a saline, alkaline lake in eastern central California, than in seawater. Low ratios of actinium to protactinium and of americium to plutonium indicate that the concentrations of trivalent actinides are not similarly enhanced. The elevated concentrations of the ordinarily very insoluble actinides are maintained in solution by natural ligands, which inhibit their chemical removal from the water column, rather than by an unusually large rate of supply.

  15. Elevated concentrations of actinides in mono lake.

    PubMed

    Anderson, R F; Bacon, M P; Brewer, P G

    1982-04-30

    Tetravalent thorium, pentavalent protactinium, hexavalent uranium, and plutonium (oxidation state uncertain) are present in much higher concentrations in Mono Lake, a saline, alkaline lake in eastern central California, than in seawater. Low ratios of actinium to protactinium and of americium to plutonium indicate that the concentrations of trivalent actinides are not similarly enhanced. The elevated concentrations of the ordinarily very insoluble actinides are maintained in solution by natural ligands, which inhibit their chemical removal from the water column, rather than by an unusually large rate of supply. PMID:17735740

  16. Strong correlations in actinide redox reactions.

    PubMed

    Horowitz, S E; Marston, J B

    2011-02-14

    Reduction-oxidation (redox) reactions of the redox couples An(VI)/An(V), An(V)/An(IV), and An(IV)/An(III), where An is an element in the family of early actinides (U, Np, and Pu), as well as Am(VI)/Am(V) and Am(V)/Am(III), are modeled by combining density functional theory with a generalized Anderson impurity model that accounts for the strong correlations between the 5f electrons. Diagonalization of the Anderson impurity model yields improved estimates for the redox potentials and the propensity of the actinide complexes to disproportionate.

  17. Strong correlations in actinide redox reactions

    NASA Astrophysics Data System (ADS)

    Horowitz, S. E.; Marston, J. B.

    2011-02-01

    Reduction-oxidation (redox) reactions of the redox couples An(VI)/An(V), An(V)/An(IV), and An(IV)/An(III), where An is an element in the family of early actinides (U, Np, and Pu), as well as Am(VI)/Am(V) and Am(V)/Am(III), are modeled by combining density functional theory with a generalized Anderson impurity model that accounts for the strong correlations between the 5f electrons. Diagonalization of the Anderson impurity model yields improved estimates for the redox potentials and the propensity of the actinide complexes to disproportionate.

  18. Stability of tetravalent actinides in perovskites

    SciTech Connect

    Williams, C.W.; Morss, L.R.; Choi, I.K.

    1983-01-01

    This paper reports the first determination of the enthalpy of formation of a complex actinide(IV) oxide: ..delta..H/sup 0//sub f/ (BaUO/sub 3/, s, 298 K) = -1690 +- 10 kJ mol/sup -1/. The preparation and properties of this and other actinide(IV) complex oxides are described and are compared with other perovskites BaMO/sub 3/. The relative stabilities of tetravalent and hexavalent uranium in various environments are compared in terms of the oxidation-reduction behavior of uranium in geological nuclear waste storage media; in perovskite, uranium(IV) is very unstable in comparison with uranium(VI).

  19. Pyrochlore based glass-ceramics for the immobilization of actinide-rich nuclear wastes: From concept to reality

    NASA Astrophysics Data System (ADS)

    Zhang, Y.; Zhang, Z.; Thorogood, G.; Vance, E. R.

    2013-01-01

    Pyrochlore based glass-ceramics have been developed, from concept to reality, for the immobilization of actinide-rich nuclear wastes. Compared with zirconolite based glass-ceramics, they are less sensitive to the processing redox conditions and can double actinide waste loadings thus decreasing volumes of the consolidated waste forms, and subsequently reducing the interim storage and disposal costs. More importantly, they provide an alternative flexible system to tackle radioactive wastes arising from the advanced nuclear reactors.

  20. Research in actinide chemistry. Final report, March 1, 1993--February 28, 1996

    SciTech Connect

    Choppin, G R

    1997-01-01

    The present three-year grant period has been a fruitful one for the laboratory as research entered some new areas while continuing in others in which the group has been successful. As in past grant periods, the principal focus has been on complexation of actinide elements with inorganic and organic ligands. The ligands to study have been chosen for their value (known or potential) in actinide separations or for their potential role in environmental behavior of the actinides. Since the radioactivity of some actinides limits the variety of techniques which can be used in their study, we have used {open_quotes}oxidation state analogs{close_quotes}. These analogs have the same oxidation state and very similar chemical behavior but are stable or very long-lived. Also, the analogs are chosen for their redox stability to avoid uncertainties in interpretation of systems in which several oxidations may coexist (e.g., in the case of Pu). Examples of such analogs which we have used are: Nd(III), Eu(III) for Pu(III), Am(III), Cm(III); Th(IV) for U(IV), Pu(IV); NpO{sub 2}{sup +} for PuO{sub 2}{sup +}; UO{sub 2}{sup 2+} for NpO{sub 2}{sup 2+}, PuO{sub 2}{sup 2+}. These analogs have allowed use of techniques which can increase significantly our understanding of actinide complexation.

  1. A System Analysis Tool

    SciTech Connect

    CAMPBELL,PHILIP L.; ESPINOZA,JUAN

    2000-06-01

    In this paper we describe a tool for analyzing systems. The analysis is based on program slicing. It answers the following question for the software: if the value of a particular variable changes, what other variable values also change, and what is the path in between? program slicing was developed based on intra-procedure control and data flow. It has been expanded commercially to inter-procedure flow. However, we extend slicing to collections of programs and non-program entities, which we term multi-domain systems. The value of our tool is that an analyst can model the entirety of a system, not just the software, and we believe that this makes for a significant increase in power. We are building a prototype system.

  2. Network systems security analysis

    NASA Astrophysics Data System (ADS)

    Yilmaz, Ä.°smail

    2015-05-01

    Network Systems Security Analysis has utmost importance in today's world. Many companies, like banks which give priority to data management, test their own data security systems with "Penetration Tests" by time to time. In this context, companies must also test their own network/server systems and take precautions, as the data security draws attention. Based on this idea, the study cyber-attacks are researched throughoutly and Penetration Test technics are examined. With these information on, classification is made for the cyber-attacks and later network systems' security is tested systematically. After the testing period, all data is reported and filed for future reference. Consequently, it is found out that human beings are the weakest circle of the chain and simple mistakes may unintentionally cause huge problems. Thus, it is clear that some precautions must be taken to avoid such threats like updating the security software.

  3. Synthesis of Coordinatively Unsaturated Tetravalent Actinide Complexes with η(5) Coordination of Pyrrole.

    PubMed

    Batrice, Rami J; Fridman, Natalia; Eisen, Moris S

    2016-03-21

    The synthesis of new actinide complexes utilizing bridged α-alkyl-pyrrolyl ligands is presented. Lithiation of the ligands followed by treatment with 1 equiv of actinide tetrachloride (uranium or thorium) produces the desired complex in good yield. X-ray diffraction studies reveal unique η(5):η(5) coordination of the pyrrolyl moieties; when the nonsterically demanding methylated ligand is used, rapid addition of the lithiated ligand solution to the metal precursor forms a bis-ligated complex that reveals η(5):η(1) coordination as determined by crystallographic analysis. PMID:26950463

  4. Plutonium and minor actinides utilization in Thorium molten salt reactor

    NASA Astrophysics Data System (ADS)

    Waris, Abdul; Aji, Indarta K.; Novitrian, Kurniadi, Rizal; Su'ud, Zaki

    2012-06-01

    FUJI-12 reactor is one of MSR systems that proposed by Japan. The original FUJI-12 design considers Th/233U or Th/Pu as main fuel. In accordance with the currently suggestion to stay away from the separation of Pu and minor actinides (MA), in this study we evaluated the utilization of Pu and MA in FUJI-12. The reactor grade Pu was employed in the present study as a small effort of supporting THORIMS-NES scenario. The result shows that the reactor can achieve its criticality with the Pu & MA composition in the fuel of 5.96% or more.

  5. Plutonium and minor actinides utilization in Thorium molten salt reactor

    SciTech Connect

    Waris, Abdul; Aji, Indarta K.; Novitrian,; Kurniadi, Rizal; Su'ud, Zaki

    2012-06-06

    FUJI-12 reactor is one of MSR systems that proposed by Japan. The original FUJI-12 design considers Th/{sup 233}U or Th/Pu as main fuel. In accordance with the currently suggestion to stay away from the separation of Pu and minor actinides (MA), in this study we evaluated the utilization of Pu and MA in FUJI-12. The reactor grade Pu was employed in the present study as a small effort of supporting THORIMS-NES scenario. The result shows that the reactor can achieve its criticality with the Pu and MA composition in the fuel of 5.96% or more.

  6. DART system analysis.

    SciTech Connect

    Boggs, Paul T.; Althsuler, Alan; Larzelere, Alex R.; Walsh, Edward J.; Clay, Ruuobert L.; Hardwick, Michael F. (Sandia National Laboratories, Livermore, CA)

    2005-08-01

    The Design-through-Analysis Realization Team (DART) is chartered with reducing the time Sandia analysts require to complete the engineering analysis process. The DART system analysis team studied the engineering analysis processes employed by analysts in Centers 9100 and 8700 at Sandia to identify opportunities for reducing overall design-through-analysis process time. The team created and implemented a rigorous analysis methodology based on a generic process flow model parameterized by information obtained from analysts. They also collected data from analysis department managers to quantify the problem type and complexity distribution throughout Sandia's analyst community. They then used this information to develop a community model, which enables a simple characterization of processes that span the analyst community. The results indicate that equal opportunity for reducing analysis process time is available both by reducing the ''once-through'' time required to complete a process step and by reducing the probability of backward iteration. In addition, reducing the rework fraction (i.e., improving the engineering efficiency of subsequent iterations) offers approximately 40% to 80% of the benefit of reducing the ''once-through'' time or iteration probability, depending upon the process step being considered. Further, the results indicate that geometry manipulation and meshing is the largest portion of an analyst's effort, especially for structural problems, and offers significant opportunity for overall time reduction. Iteration loops initiated late in the process are more costly than others because they increase ''inner loop'' iterations. Identifying and correcting problems as early as possible in the process offers significant opportunity for time savings.

  7. Preparation of minor actinides targets or blankets by means of ionic exchange resin

    NASA Astrophysics Data System (ADS)

    Picart, S.; Mokhtari, H.; Ramière, I.; Jobelin, I.

    2010-03-01

    The conversion of minor actinides to fuel starting materials for transmutation in a closed nuclear cycle is a big challenge for the next decades and the development of Gen(IV) nuclear systems. Conversion routes are numerous, but one needs to prove that they can be adapted to handle minor actinides. One of them is called the resin process and is particularly attractive because it stands for a "dustless" process as it produces microspheres of oxide or carbide after thermal treatment of the loaded resin. The study presented herein focuses on the experiments and tests which enable us to optimize the fixation of minor actinides onto ionic exchange resin and their carbonization into oxide type materials.

  8. The abundance of the actinides in the cosmic radiation as measured on HEAO 3

    NASA Technical Reports Server (NTRS)

    Binns, W. R.; Israel, M. H.; Klarmann, J.; Fickle, R. K.; Waddington, C. J.; Garrard, T. L.; Stone, E. C.

    1982-01-01

    The HEAO 3 detector of heavy cosmic-ray nuclei has observed one possible actinide nucleus and some 100 nuclei of the platinum-lead group of elements. The resulting upper limit of 3% for the abundance ratio of actinides to platinum-lead nuclides is significantly lower than previous results from other observations. This new limit is inconsistent with freshly synthesized, pure r-process sources for cosmic-ray nuclei in this charge interval but is consistent with a source having a composition similar to the solar system, or to aged r-process material. We observe no events with a charge greater than 96.

  9. Density Functional Theory Studies of the Electronic Structure of Solid State Actinide Oxides

    SciTech Connect

    Wen, Xiaodong; Martin, Richard L.; Henderson, Thomas M.; Scuseria, Gustavo E.

    2013-02-13

    The actinide oxides have been extensively studied in the context of the nuclear fuel cycle. They are also of fundamental interest as members of a class of strongly correlated materials, the Mott insulators. Their complex physical and chemical properties make them challenging systems to characterize, both experimentally and theoretically. Chiefly, this is because actinide oxides can exhibit both electronic localization and electronic delocalization and have partially occupied f orbitals, which can lead to multiple possibilities for ground states. Of particular concern for theoretical work is that the large number of competing states display strong correlations which are dffcult to capture with computationally tractable methods.

  10. Actinide Targets for Neutron Cross Section Measurements

    SciTech Connect

    John D. Baker; Christopher A. McGrath

    2006-10-01

    The Advanced Fuel Cycle Initiative (AFCI) and the Generation IV Reactor Initiative have demonstrated a lack of detailed neutron cross-sections for certain "minor" actinides, those other than the most common (235U, 238U, and 239Pu). For some closed-fuel-cycle reactor designs more than 50% of reactivity will, at some point, be derived from "minor" actinides that currently have poorly known or in some cases not measured (n,?) and (n,f) cross sections. A program of measurements under AFCI has begun to correct this. One of the initial hurdles has been to produce well-characterized, highly isotopically enriched, and chemically pure actinide targets on thin backings. Using a combination of resurrected techniques and new developments, we have made a series of targets including highly enriched 239Pu, 240Pu, and 242Pu. Thus far, we have electrodeposited these actinide targets. In the future, we plan to study reductive distillation to achieve homogeneous, adherent targets on thin metal foils and polymer backings. As we move forward, separated isotopes become scarcer, and safety concerns become greater. The chemical purification and electodeposition techniques will be described.

  11. Actinide valences in xenotime and monazite

    NASA Astrophysics Data System (ADS)

    Vance, E. R.; Zhang, Y.; McLeod, T.; Davis, J.

    2011-02-01

    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 3+ and Np 3+ can be incorporated in xenotime samples fired in a reducing atmosphere.

  12. 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

    SciTech Connect

    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.

  13. An expanded porphyrin approach toward transactinium chelation and the development of porphyrin-coated optical fibers as potential actinide sensors

    SciTech Connect

    Klunder, G.; Silva, R.

    1994-12-01

    Characterization of the contamination at DOE waste sites and facilities is necessary during environmental restoration. Characterization of toxic waste in containers and storage tanks is needed for effective waste management. Therefore, analytical and monitoring systems are needed for real-time analysis and feedback. The development of in-situ methods to measure chemical properties by specialized instrumentation capable of real-time analysis, without sacrificing sensitivity, has been identified as an area of needed development. Absorption spectroscopy is widely used and considered to be one of the most reliable techniques available for the qualitative and quantitative determination of sample composition. With the advancements in fiber optic technology, using light for remote in-situ sensing of groundwater contaminants has become practical. Significant progress has been made in the area of fiber-optic chemical sensors as can be seen by the number of recent review articles. The objective of this work is to develop a remote sensor for real-time measurement of actinides and concentrations in environmental or process waters based on absorption spectroscopy using internal reflection spectroscopy. Porphyrin coated silica wafers were prepared and the sensitivity and selectivity to actinides was determined.

  14. Launch Vehicle Systems Analysis

    NASA Technical Reports Server (NTRS)

    Olds, John R.

    1999-01-01

    This report summaries the key accomplishments of Georgia Tech's Space Systems Design Laboratory (SSDL) under NASA Grant NAG8-1302 from NASA - Marshall Space Flight Center. The report consists of this summary white paper, copies of technical papers written under this grant, and several viewgraph-style presentations. During the course of this grant four main tasks were completed: (1)Simulated Combined-Cycle Rocket Engine Analysis Module (SCCREAM), a computer analysis tool for predicting the performance of various RBCC engine configurations; (2) Hyperion, a single stage to orbit vehicle capable of delivering 25,000 pound payloads to the International Space Station Orbit; (3) Bantam-X Support - a small payload mission; (4) International Trajectory Support for interplanetary human Mars missions.

  15. Neutron activation analysis system

    DOEpatents

    Taylor, M.C.; Rhodes, J.R.

    1973-12-25

    A neutron activation analysis system for monitoring a generally fluid media, such as slurries, solutions, and fluidized powders, including two separate conduit loops for circulating fluid samples within the range of radiation sources and detectors is described. Associated with the first loop is a neutron source that emits s high flux of slow and thermal neutrons. The second loop employs a fast neutron source, the flux from which is substantially free of thermal neutrons. Adjacent to both loops are gamma counters for spectrographic determination of the fluid constituents. Other gsmma sources and detectors are arranged across a portion of each loop for deterMining the fluid density. (Official Gazette)

  16. Beta systems error analysis

    NASA Technical Reports Server (NTRS)

    1984-01-01

    The atmospheric backscatter coefficient, beta, measured with an airborne CO Laser Doppler Velocimeter (LDV) system operating in a continuous wave, focussed model is discussed. The Single Particle Mode (SPM) algorithm, was developed from concept through analysis of an extensive amount of data obtained with the system on board a NASA aircraft. The SPM algorithm is intended to be employed in situations where one particle at a time appears in the sensitive volume of the LDV. In addition to giving the backscatter coefficient, the SPM algorithm also produces as intermediate results the aerosol density and the aerosol backscatter cross section distribution. A second method, which measures only the atmospheric backscatter coefficient, is called the Volume Mode (VM) and was simultaneously employed. The results of these two methods differed by slightly less than an order of magnitude. The measurement uncertainties or other errors in the results of the two methods are examined.

  17. Heavy actinide production from the interactions of sup 40 Ar with sup 248 Cm and a comparison with the sup 44 Ca- sup 248 Cm system

    SciTech Connect

    Leyba, J.D.; Henderson, R.A.; Hall, H.L.; Gannett, C.M.; Chadwick, R.B.; Czerwinski, K.R.; Kadkhodayan, B.A.; Kreek, S.A.; Haynes, G.R.; Gregorich, K.E.; Lee, D.M.; Nurmia, M.J.; Hoffman, D.C. Nuclear Science Division, Lawrence Berkeley Laboratory, University of California, Berkeley, Berkeley, California 94720)

    1990-05-01

    Excitation functions have been measured for isotopes of Bk, Cf, Es, and Fm produced from the interactions of 207- to 286-MeV {sup 40}Ar ions with {sup 248}Cm. The measured isotopic distributions were found to be essentially symmetric with full widths at half maximum between 2.0 and 3.5 mass units. These results are comparable to those obtained in previous studies using {sup 40,44,48}Ca with {sup 248}Cm. The maxima of the isotopic distributions from the {sup 40}Ar-{sup 248}Cm system show shifts, to both heavier and lighter mass numbers, of 0 to 2 mass units relative to the corresponding maxima of the isotopic distributions from the {sup 40,44,48}Ca-{sup 248}Cm systems.

  18. IUPAC-NIST Solubility Data Series. 74. Actinide Carbon Compounds

    NASA Astrophysics Data System (ADS)

    Hála, Jiri; Hála, Jiri; Navratil, James D.

    2001-03-01

    This volume presents solubility data of the carbonates, salts of carboxylic acids, and other carbon containing compounds of actinides. Covered are compounds of thorium, uranium, neptunium, plutonium, americium, and one system for curium. No solubility data on carbonates or other carbon containing compounds have been found for other actinide elements. The literature has been covered up to the end of 1999, and there was a great effort to have the literature survey as complete as possible. Only those published results that report meaningful data were considered for the volume. Papers that reported qualitative results with statements like "sparingly soluble" or "insoluble," etc. were not considered. In addition to papers that published numerical data, some papers that presented data in graphical form only were considered as well. They were considered for the volume either if no other data were available for the system, if the data were published in difficult to obtain older literature, or if the data were considered to be of importance for other reasons. For many compounds it was not possible to provide the Chemical Abstracts Registry Numbers since these have not yet been assigned. For this reason, the Registry Number index is incomplete.

  19. System of systems modeling and analysis.

    SciTech Connect

    Campbell, James E.; Anderson, Dennis James; Longsine, Dennis E.; Shirah, Donald N.

    2005-01-01

    This report documents the results of an LDRD program entitled 'System of Systems Modeling and Analysis' that was conducted during FY 2003 and FY 2004. Systems that themselves consist of multiple systems (referred to here as System of Systems or SoS) introduce a level of complexity to systems performance analysis and optimization that is not readily addressable by existing capabilities. The objective of the 'System of Systems Modeling and Analysis' project was to develop an integrated modeling and simulation environment that addresses the complex SoS modeling and analysis needs. The approach to meeting this objective involved two key efforts. First, a static analysis approach, called state modeling, has been developed that is useful for analyzing the average performance of systems over defined use conditions. The state modeling capability supports analysis and optimization of multiple systems and multiple performance measures or measures of effectiveness. The second effort involves time simulation which represents every system in the simulation using an encapsulated state model (State Model Object or SMO). The time simulation can analyze any number of systems including cross-platform dependencies and a detailed treatment of the logistics required to support the systems in a defined mission.

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

    SciTech Connect

    Van Der Sluys, W.G.; Burns, C.J.; Smith, D.C.

    1991-04-02

    This invention is comprised of 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 effective 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.

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

    DOEpatents

    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.

  2. Electrorecovery of actinides at room temperature

    SciTech Connect

    Stoll, Michael E; Oldham, Warren J; Costa, David A

    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

  3. Laboratory actinide partitioning - Whitlockite/liquid and influence of actinide concentration levels

    NASA Technical Reports Server (NTRS)

    Benjamin, T. M.; Jones, J. H.; Heuser, W. R.; Burnett, D. S.

    1983-01-01

    The partition coefficients between synthetic whitlockite (beta Ca-phosphate) and coexisting silicate melts are determined for the actinide elements Th, U and Pu. Experiments were performed at 1 bar pressure and 1250 C at oxygen fugacities from 10 to the -8.5 to 10 to the -0.7 bars, and partitioning was determined from trace element radiography combined with conventional electron microprobe analysis. Results show Pu to be more readily incorporated into crystalline phases than U or Th under reducing conditions, which is attributed to the observation that Pu exists primarily in the trivalent state, while U and Th are tetravalent. Corrected partition coefficients for whitlockite of 3.6, less than or equal to 0.6, 1.2, 0.5 and less than or equal to 0.002 are estimated for Pu(+3), Pu(+4), Th(+4), U(+4) and U(+6), respectively. Experiments performed at trace levels and percent levels of UO2 indicate that Si is involved in U substitution in whitlockite, and show a reduced partition coefficient at higher concentrations of U that can be explained by effects on melt structure or the fraction of tetravalent U.

  4. Actinide production from xenon bombardments of curium-248

    SciTech Connect

    Welch, R.B.

    1985-01-01

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

  5. Integrated fluorescence analysis system

    DOEpatents

    Buican, Tudor N.; Yoshida, Thomas M.

    1992-01-01

    An integrated fluorescence analysis system enables a component part of a sample to be virtually sorted within a sample volume after a spectrum of the component part has been identified from a fluorescence spectrum of the entire sample in a flow cytometer. Birefringent optics enables the entire spectrum to be resolved into a set of numbers representing the intensity of spectral components of the spectrum. One or more spectral components are selected to program a scanning laser microscope, preferably a confocal microscope, whereby the spectrum from individual pixels or voxels in the sample can be compared. Individual pixels or voxels containing the selected spectral components are identified and an image may be formed to show the morphology of the sample with respect to only those components having the selected spectral components. There is no need for any physical sorting of the sample components to obtain the morphological information.

  6. Microbial Transformations of Actinides and Other Radionuclides

    SciTech Connect

    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.

  7. Actinide phosphonate complexes in aqueous solutions

    SciTech Connect

    Nash, K.L.

    1993-10-01

    Complexes formed by actinides with carboxylic acids, polycarboxylic acids, and aminopolycarboxylic acids play a central role in both the basic and process chemistry of the actinides. Recent studies of f-element complexes with phosphonic acid ligands indicate that new ligands incorporating doubly ionizable phosphonate groups (-PO{sub 3}H{sub 2}) have many properties which are unique chemically, and promise more efficient separation processes for waste cleanup and environmental restoration. Simple diphosphonate ligands form much stronger complexes than isostructural carboxylates, often exhibiting higher solubility as well. In this manuscript recent studies of the thermodynamics and kinetics of f-element complexation by 1,1 and 1,2 diphosphonic acid ligands are described.

  8. Separation of Californium from other Actinides

    DOEpatents

    Mailen, J C; Ferris, L M

    1973-09-25

    A method is provided for separating californium from a fused fluoride composition containing californium and at least one element selected from the group consisting of plutonium, americium, curium, uranium, thorium, and protactinium which comprises contacting said fluoride composition with a liquid bismuth phase containing sufficient lithium or thorium to effect transfer of said actinides to the bismuth phase and then contacting the liquid bismuth phase with molten LiCl to effect selective transfer of californium to the chloride phase.

  9. In vitro removal of actinide (IV) ions

    DOEpatents

    Weitl, Frederick L.; Raymond, Kenneth N.

    1982-01-01

    A compound of the formula: ##STR1## wherein X is hydrogen or a conventional electron-withdrawing group, particularly --SO.sub.3 H or a salt thereof; n is 2, 3, or 4; m is 2, 3, or 4; and p is 2 or 3. The present compounds are useful as specific sequestering agents for actinide (IV) ions. Also described is a method for the 2,3-dihydroxybenzamidation of azaalkanes.

  10. Surrogate Reactions in the Actinide Region

    SciTech Connect

    Burke, J T; Bernstein, L A; Scielzo, N D; Bleuel, D L; Lesher, S R; Escher, J; Ahle, L; Dietrich, F S; Hoffman, R D; Norman, E B; Sheets, S A; Phair, L; Fallon, P; Clark, R M; Gibelin, J; Jewett, C; Lee, I Y; Macchiavelli, A O; McMahan, M A; Moretto, L G; Rodriguez-Vieitez, E; Wiedeking, M; Lyles, B F; Beausang, C W; Allmond, J M; Ai, H; Cizewski, J A; Hatarik, R; O'Malley, P D; Swan, T

    2008-01-30

    Over the past three years we have studied various surrogate reactions (d,p), ({sup 3}He,t), ({alpha},{alpha}{prime}) on several uranium isotopes {sup 234}U, {sup 235}U, {sup 236}U, and {sup 238}U. An overview of the STARS/LIBERACE surrogate research program as it pertains to the actinides is discussed. A summary of results to date will be presented along with a discussion of experimental difficulties encountered in surrogate experiments and future research directions.

  11. Performance Characteristics of Actinide-Burning Fusion Power Plants

    SciTech Connect

    Cheng, E.T

    2005-05-15

    Performance characteristics were summarized of two molten salt based fusion power plants. One of them is to burn spent fuel actinides, the other is to burn U{sup 238}. Both power plants produce output energy larger than a fusion power plant would normally produce without including actinides. Additional features, obtainable by design for these actinide burning power plants, are adequate tritium breeding, sub-critical condition, and stable power output.

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

    SciTech Connect

    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.

  13. Actinide and lanthanide separation process (ALSEP)

    SciTech Connect

    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).

  14. Value of burnup credit beyond actinides

    SciTech Connect

    Lancaster, D.; Fuentes, E.; Kang, Chi

    1997-12-01

    DOE has submitted a topical report to the NRC justifying burnup credit based only on actinide isotopes (U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, and Am-241). When this topical report is approved, it will allow a great deal of the commercial spent nuclear fuel to be transported in significantly higher capacity casks. A cost savings estimate for shipping fuel in 32 assembly (burnup credit) casks as opposed to 24 assembly (non-burnup credit) casks was previously presented. Since that time, more detailed calculations have been performed using the methodology presented in the Actinide-Only Burnup Credit Topical Report. Loading curves for derated casks have been generated using actinide-only burnup credit and are presented in this paper. The estimates of cost savings due to burnup credit for shipping fuel utilizing 32, 30, 28, and 24 assembly casks where only the 24 assembly cask does not burnup credit have been created and are discussed. 4 refs., 2 figs.

  15. Actinide behavior in a freshwater pond

    SciTech Connect

    Trabalka, J.R.; Bogle, M.A.; Scott, T.G.

    1983-01-01

    Long-term investigations of solution chemistry in an alkaline freshwater pond have revealed that actinide oxidation state behavior, particularly that of plutonium, is complex. The Pu(V,VI) fraction was predominant in solution, but it varied over the entire range reported from other natural aquatic environments, in this case, as a result of intrinsic biological and chemical cycles (redox and pH-dependent phenomena). A strong positive correlation between plutonium (Pu), but not uranium (U), and hydroxyl ion over the observation period, especially when both were known to be in higher oxidation states, was particularly notable. Coupled with other examples of divergent U and Pu behavior, this result suggests that Pu(V), or perhaps a mixture of Pu(V,VI), was the prevalent oxidation state in solution. Observations of trivalent actinide sorption behavior during an algal bloom, coupled with the association with a high-molecular weight (nominally 6000 to 10,000 mol wt) organic fraction in solution, indicate that solution-detritus cycling of organic carbon, in turn, may be the primary mechanism in amercium-curium (Am-Cm) cycling. Sorption by sedimentary materials appears to predominate over other factors controlling effective actinide solubility and may explain, at least partially, the absence of an expected strong positive correlation between carbonate and dissolved U. 49 references, 6 figures, 12 tables.

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

    NASA Astrophysics Data System (ADS)

    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.

  17. Bidentate organophosphorus solvent extraction process for actinide recovery and partition

    DOEpatents

    Schulz, Wallace W.

    1976-01-01

    A liquid-liquid extraction process for the recovery and partitioning of actinide values from acidic nuclear waste aqueous solutions, the actinide values including trivalent, tetravalent and hexavalent oxidation states is provided and includes the steps of contacting the aqueous solution with a bidentate organophosphorous extractant to extract essentially all of the actinide values into the organic phase. Thereafter the respective actinide fractions are selectively partitioned into separate aqueous solutions by contact with dilute nitric or nitric-hydrofluoric acid solutions. The hexavalent uranium is finally removed from the organic phase by contact with a dilute sodium carbonate solution.

  18. Impact of Including Higher Actinides in Fast Reactor Transmutation Analyses

    SciTech Connect

    B. Forget; M. Asgari; R. Ferrer; S. Bays

    2007-09-01

    Previous fast reactor transmutation studies generally disregarded higher mass minor actinides beyond Cm-246 due to various considerations including deficiencies in nuclear cross-section data. Although omission of these higher mass actinides does not significantly impact the neutronic calculations and fuel cycle performance parameters follow-on neutron dose calculations related to fuel recycling, transportation and handling are significantly impacted. This report shows that including the minor actinides in the equilibrium fast reactor calculations will increase the predicted neutron emission by about 30%. In addition a sensitivity study was initiated by comparing the impact of different cross-section evaluation file for representing these minor actinides.

  19. NEW METHOD FOR DETERMINATION OF ACTINIDES AND STRONTIUM IN ANIMAL TISSUE

    SciTech Connect

    Maxwell, S; Jay Hutchison, J; Don Faison, D

    2007-05-07

    The analysis of actinides in animal tissue samples is very important for environmental monitoring. There is a need to measure actinide isotopes with very low detection limits in animal tissue samples, including fish, deer, hogs, beef and shellfish. A new, rapid actinide separation method has been developed and implemented that allows the measurement of plutonium, neptunium, uranium, americium, curium and strontium isotopes in large animal tissue samples (100-200 g) with high chemical recoveries and effective removal of matrix interferences. This method uses stacked TEVA Resin{reg_sign}, TRU Resin{reg_sign} and DGA-Resin{reg_sign} cartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium (Pu), neptunium (Np), uranium (U), americium (Am), and curium (Cm) using a single multi-stage column combined with alpha spectrometry. Sr-90 is collected on Sr Resin{reg_sign} from Eichrom Technologies (Darien, IL, USA). After acid digestion and furnace heating of the animal tissue samples, the actinides and Sr-89/90 are separated using column extraction chromatography. This method has been shown to be effective over a wide range of animal tissue matrices. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized.

  20. Performance Comparison of Metallic, Actinide Burning Fuel in Lead-Bismuth and Sodium Cooled Fast Reactors

    SciTech Connect

    Weaver, Kevan Dean; Herring, James Stephen; Mac Donald, Philip Elsworth

    2001-04-01

    Various methods have been proposed to “incinerate” or “transmutate” the current inventory of trans-uranic waste (TRU) that exits in spent light-water-reactor (LWR) fuel, and weapons plutonium. These methods include both critical (e.g., fast reactors) and non-critical (e.g., accelerator transmutation) systems. The work discussed here is part of a larger effort at the Idaho National Engineering and Environmental Laboratory (INEEL) and at the Massachusetts Institute of Technology (MIT) to investigate the suitability of lead and lead-alloy cooled fast reactors for producing low-cost electricity as well as for actinide burning. The neutronics of non-fertile fuel loaded with 20 or 30-wt% light water reactor (LWR) plutonium plus minor actinides for use in a lead-bismuth cooled fast reactor are discussed in this paper, with an emphasis on the fuel cycle life and isotopic content. Calculations show that the average actinide burn rate is similar for both the sodium and lead-bismuth cooled cases ranging from -1.02 to -1.16 g/MWd, compared to a typical LWR actinide generation rate of 0.303 g/MWd. However, when using the same parameters, the sodium-cooled case went subcritical after 0.2 to 0.8 effective full power years, and the lead-bismuth cooled case ranged from 1.5 to 4.5 effective full power years.

  1. ENHANCING ADVANCED CANDU PROLIFERATION RESISTANCE FUEL WITH MINOR ACTINIDES

    SciTech Connect

    Gray S. Chang

    2010-05-01

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

  2. Advanced Extraction Methods for Actinide/Lanthanide Separations

    SciTech Connect

    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

  3. DANDE: a linked code system for core neutronics/depletion analysis

    SciTech Connect

    LaBauve, R.J.; England, T.R.; George, D.C.; MacFarlane, R.E.; Wilson, W.B.

    1985-06-01

    This report describes DANDE - a modular neutronics, depletion code system for reactor analysis. It consists of nuclear data processing, core physics, and fuel depletion modules, and allows one to use diffusion and transport methods interchangeably in core neutronics calculations. This latter capability is especially important in the design of small modular cores. Additional unique features include the capability of updating the nuclear data file during a calculation; a detailed treatment of depletion, burnable poisons as well as fuel; and the ability to make geometric changes such as control rod repositioning and fuel relocation in the course of a calculation. The detailed treatment of reactor fuel burnup, fission-product creation and decay, as well as inventories of higher-order actinides is a necessity when predicting the behavior of reactor fuel under increased burn conditions. The operation of the code system is made clear in this report by following a sample problem.

  4. The role of actinide burning and the Integral Fast Reactor in the future of nuclear power

    SciTech Connect

    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.

  5. Delayed Neutron and Delayed Photon Characteristics from Photofission of Actinides

    SciTech Connect

    Dore, D.; Berthoumieux, E.; Leprince, A.; Ridikas, D.

    2011-12-13

    Delayed neutron (DN) and delayed photon (DP) emissions from photofission reactions play an important role for applications involving nuclear material detection and characterization. To provide new, accurate, basic nuclear data for evaluations and data libraries, an experimental programme of DN and DP measurements has been undertaken for actinides with bremsstrahlung endpoint energy in the giant resonance region ({approx}15 MeV). In this paper, the experimental setup and the data analysis method will be described. Experimental results for DN and DP characteristics will be presented for {sup 232}Th, {sup 235,238}U, {sup 237}Np, and {sup 239}Pu. Finally, an example of an application to study the contents of nuclear waste packages will be briefly discussed.

  6. Neutron capture by fissile and fertile actinide targets

    SciTech Connect

    Maslov, Vladimir M.

    2009-01-28

    For fissile actinide targets {sup 233}U, {sup 235}U and {sup 239}Pu the capture cross sections are strongly influenced by the target spin, fission transition states spectroscopy and fission/{gamma}-emission competition of the compound nuclides. The capture cross sections were obtained via a consistent description of fission and elastic/inelastic scattering, (n,{gamma}f) reaction being included.For neutron capture reactions on even-even U, Pu and Cm nuclei the methods, proven in case of {sup 232}Th(n,{gamma}) and {sup 238}U(n,{gamma}) data analysis are used. Calculated {sup 240}Pu(n,{gamma}) and {sup 244}Cm(n,{gamma}) reaction cross sections shapes are much similar to that, observed for the {sup 238}U(n,{gamma}) and {sup 232}Th(n,{gamma}) reactions. Differences are due to fission and neutron emission competition, which depends on the (Z,N)-composition of the compound nucleus.

  7. Study of actinide chemistry in saturated potassium fluoride solution

    NASA Technical Reports Server (NTRS)

    Cohen, D.; Thalmayer, C. E.

    1969-01-01

    Study concerning the chemistry of actinides in saturated KF solution included work with neptunium, uranium, and americium. Solubilities, absorption spectra, oxidation-reduction reactions, and solid compounds which can be produced in KF solution were examined. The information is used for preparation of various materials from salts of the actinides.

  8. Process for Making a Ceramic Composition for Immobilization of Actinides

    SciTech Connect

    Ebbinghaus, Bartley B.; Van Konynenburg, Richard A.; Vance, Eric R.; Stewart, Martin W.; Walls, Philip A.; Brummond, William Allen; Armantrout, Guy A.; Curtis, Paul G.; Hobson, Beverly F.; Farmer, Joseph; Herman, Connie Cicero; Herman, David Thomas

    1999-06-22

    Disclosed is a process for making a ceramic composition for the immobilization of actinides, particularly uranium and plutonium. The ceramic is a titanate material comprising pyrochlore, brannerite and rutile. The process comprises oxidizing the actinides, milling the oxides to a powder, blending them with ceramic precursors, cold pressing the blend and sintering the pressed material.

  9. Process for making a ceramic composition for immobilization of actinides

    DOEpatents

    Ebbinghaus, Bartley B.; Van Konynenburg, Richard A.; Vance, Eric R.; Stewart, Martin W.; Walls, Philip A.; Brummond, William Allen; Armantrout, Guy A.; Herman, Connie Cicero; Hobson, Beverly F.; Herman, David Thomas; Curtis, Paul G.; Farmer, Joseph

    2001-01-01

    Disclosed is a process for making a ceramic composition for the immobilization of actinides, particularly uranium and plutonium. The ceramic is a titanate material comprising pyrochlore, brannerite and rutile. The process comprises oxidizing the actinides, milling the oxides to a powder, blending them with ceramic precursors, cold pressing the blend and sintering the pressed material.

  10. Improved method for extracting lanthanides and actinides from acid solutions

    DOEpatents

    Horwitz, E.P.; Kalina, D.G.; Kaplan, L.; Mason, G.W.

    1983-07-26

    A process for the recovery of actinide and lanthanide values from aqueous acidic solutions uses a new series of neutral bi-functional extractants, the alkyl(phenyl)-N,N-dialkylcarbamoylmethylphosphine oxides. The process is suitable for the separation of actinide and lanthanide values from fission product values found together in high-level nuclear reprocessing waste solutions.

  11. POTENTIAL BENCHMARKS FOR ACTINIDE PRODUCTION IN HANFORD REACTORS

    SciTech Connect

    PUIGH RJ; TOFFER H

    2011-10-19

    A significant experimental program was conducted in the early Hanford reactors to understand the reactor production of actinides. These experiments were conducted with sufficient rigor, in some cases, to provide useful information that can be utilized today in development of benchmark experiments that may be used for the validation of present computer codes for the production of these actinides in low enriched uranium fuel.

  12. Detailed calculations of minor actinide transmutation in a fast reactor

    SciTech Connect

    Takeda, Toshikazu

    2015-12-31

    The transmutation of minor actinides in a fast reactor is investigated by a new method to investigate the transmutation behavior of individual minor actinides. It is found that Np-237 and Am-241 mainly contributes to the transmutation rate though the transmutation behaviors are very different.

  13. FY2011 Annual Report for the Actinide Isomer Detection Project

    SciTech Connect

    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

  14. Sigma Team for Advanced Actinide Recycle FY2015 Accomplishments and Directions

    SciTech Connect

    Moyer, Bruce A.

    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

  15. Actinide management with commercial fast reactors

    NASA Astrophysics Data System (ADS)

    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.

  16. Multicoordinate ligands for actinide/lanthanide separations.

    PubMed

    Dam, Henk H; Reinhoudt, David N; Verboom, Willem

    2007-02-01

    In nuclear waste treatment processes there is a need for improved ligands for the separation of actinides (An(III)) and lanthanides (Ln(III)). Several research groups are involved in the design and synthesis of new An(III) ligands and in the confinement of these and existing An(III) ligands onto molecular platforms giving multicoordinate ligands. The preorganization of ligands considerably improves the An(III) extraction properties, which are largely dependent on the solubility and rigidity of the platform. This tutorial review summarizes the most important An(III) ligands with emphasis on the preorganization strategy using (macrocyclic) platforms.

  17. Radiation chemistry of aqueous solutions of actinides

    NASA Astrophysics Data System (ADS)

    Pikaev, Alexei K.; Shilov, Vladimir P.; Gogolev, Andrei V.

    1997-09-01

    The data on radiolytic transformations of ions of uranium, neptunium, plutonium, americium, curium and transcurium elements in aqueous solutions are generalised. The results of studies on the kinetics of fast reactions of these ions with primary products of water radiolysis (hydrated electron e-aq, H, OH, and O- radicals and H2O2), many inorganic (Cl2-, NO3, SO4-, CO3-, O3- etc.) and organic free radicals are analysed. The mechanism of γ- and α-radiolysis of solutions of actinide ions is discussed. The bibliography includes 183 references.

  18. Actinide management with commercial fast reactors

    SciTech Connect

    Ohki, Shigeo

    2015-12-31

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

  19. Site preferences of actinide cations in [NZP] compounds

    NASA Astrophysics Data System (ADS)

    Hawkins, H. T.; Spearing, D. R.; Smith, D. M.; Hampel, F. G.; Veirs, D. K.; Scheetz, B. E.

    2000-07-01

    Compounds adopting the sodium dizirconium tris(phosphate) (NaZr2(PO4)3) structure type belong to the [NZP] structural family of compounds. [NZP] compounds possess desirable properties that would permit their application as hosts for the actinides. These properties include compositional flexibility (i.e., three structural sites that can accommodate a variety of different cations), high thermal stability, negligible thermal expansion, and resistance to radiation damage. Experimental data indicate that [NZP] compounds resist dissolution and release of constituents over a wide range of experimental conditions. Moreover, [NZP] compounds may be synthesized by both conventional and novel methods and may be heat treated or sintered at modest temperatures (800 °C-1350 °C) in open or restricted systems.

  20. Actinides in Solution: Disproportionation, Strong Correlations, and Emergence

    NASA Astrophysics Data System (ADS)

    Marston, Brad; Horowitz, Steven

    2010-03-01

    Plutonium in acid solutions can be found in oxidation states III through VI. There is a striking near perfect degeneracy of the reduction-oxidation (redox) potentials, each being about 1 volt. Neptunium is the only other element that approaches this degree of degeneracy. One consequence of the redox degeneracy is a marked tendency of plutonium ions to disproportionate; up to four different oxidation states can coexist simultaneously in the same solution, greatly complicating the environmental chemistry of the element. While the degeneracy could simply be a coincidence, it could also be the manifestation of a higher-level organizing principle at work. Other systems that exhibit disproportionation raise the possibility of an emergent negative-U attractive interaction. The hypothesis is tested by combining first-principles relativistic density-functional calculations using the Amsterdam Density Functional (ADF) package with exact diagonalizations of Hubbard-like models of the strong correlations between the actinide 5f electrons.

  1. Actinides and Rare Earths Topical Conference (Code AC)

    SciTech Connect

    Tobin, J G

    2009-11-24

    Actinide and the Rare Earth materials exhibit many unique and diverse physical, chemical and magnetic properties, in large part because of the complexity of their f electronic structure. This Topical Conference will focus upon the chemistry, physics and materials science in Lanthanide and Actinide materials, driven by 4f and 5f electronic structure. Particular emphasis will be placed upon 4f/5f magnetic structure, surface science and thin film properties. For the actinides, fundamental actinide science and its role in resolving technical challenges posed by actinide materials will be stressed. Both basic and applied experimental approaches, including synchrotron-radiation-based investigations, as well as theoretical modeling and computational simulations, are planned to be part of the Topical Conference. Of particular importance are the issues related to the potential renaissance in Nuclear Fuels, including synthesis, oxidation, corrosion, intermixing, stability in extreme environments, prediction of properties via benchmarked simulations, separation science, environmental impact and disposal of waste products.

  2. Actinide-Aluminate Speciation in Alkaline Radioactive Waste

    SciTech Connect

    Dr. David L. Clark; Dr. Alexander M. Fedosseev

    2001-12-21

    Investigation of behavior of actinides in alkaline media containing AL(III) showed that no aluminate complexes of actinides in oxidation states (IIII-VIII) were formed in alkaline solutions. At alkaline precipitation IPH (10-14) of actinides in presence of AL(III) formation of aluminate compounds is not observed. However, in precipitates contained actinides (IIV)<(VI), and to a lesser degree actinides (III), some interference of components takes place that is reflected in change of solid phase properties in comparison with pure components or their mechanical mixture. The interference decreases with rise of precipitation PH and at PH 14 is exhibited very feebly. In the case of NP(VII) the individual compound with AL(III) is obtained, however it is not aluminate of neptunium(VII), but neptunate of aluminium(III) similar to neptunates of other metals obtained earlier.

  3. Research in actinide chemistry. Progress report, 1990--1993

    SciTech Connect

    Choppin, G.R.

    1993-04-01

    This research studies the behavior of the actinide elements in aqueous solution. The high radioactivity of the transuranium actinides limits the concentrations which can be studied and, consequently, limits the experimental techniques. However, oxidation state analogs (trivalent lanthanides, tetravalent thorium, and hexavalent uranium) do not suffer from these limitations. Behavior of actinides in the environment are a major USDOE concern, whether in connection with long-term releases from a repository, releases from stored defense wastes or accidental releases in reprocessing, etc. Principal goal of our research was expand the thermodynamic data base on complexation of actinides by natural ligands (e.g., OH{sup {minus}}, CO{sub 3}{sup 2{minus}}, PO{sub 4}{sup 3{minus}}, humates). The research undertakes fundamental studies of actinide complexes which can increase understanding of the environmental behavior of these elements.

  4. Separation of actinides from lanthanides utilizing molten salt electrorefining

    SciTech Connect

    Grimmett, D.L.; Fusselman, S.P.; Roy, J.J.; Gay, R.L.; Krueger, C.L.; Storvick, T.S.; Inoue, T.; Hijikata, T.; Takahashi, N.

    1996-10-01

    TRUMP-S (TRansUranic Management through Pyropartitioning Separation) is a pyrochemical process being developed to separate actinides form fission products in nuclear waste. A key process step involving molten salt electrorefining to separate actinides from lanthanides has been studied on a laboratory scale. Electrorefining of U, Np, Pu, Am, and lanthanide mixtures from molten cadmium at 450 C to a solid cathode utilizing a molten chloride electrolyte resulted in > 99% removal of actinides from the molten cadmium and salt phases. Removal of the last few percent of actinides is accompanied by lowered cathodic current efficiency and some lanthanide codeposition. Actinide/lanthanide separation ratios on the cathode are ordered U > Np > Pu > Am and are consistent with predictions based on equilibrium potentials.

  5. Comparative Photoemission Study of Actinide (Am, Pu, Np and U) Metals, Nitrides, and Hydrides

    SciTech Connect

    Gouder, Thomas; Seibert, Alice; Rebizant, Jean; Huber, Frank; Havela, Ladislav

    2007-07-01

    Core-level and valence-band spectra of Pu and the other early actinide compounds show remarkable systematics, which can be understood in the framework of final state screening. We compare the early actinide (U, Np, Pu and Am) metals, nitrides and hydrides and a few other specific compounds (PuSe, PuS, PuCx, PuSix) prepared as thin films by sputter deposition. In choosing these systems, we combine inherent 5f band narrowing, due to 5f orbital contraction throughout the actinide series, with variations of the chemical environment in the compounds. Goal of this work was to learn more on the electronic structure of the early actinide systems and to achieve the correct interpretation of their photoemission spectra. The highly correlated nature of the 5f states in systems, which are on the verge to localization, makes this a challenging task, because of the peculiar interplay between ground state DOS and final-state effects. Their influence can be estimated by doing systematic studies on systems with different (5f) bandwidths. We conclude on the basis of such systematic experiments that final-state effects due to strong e-e correlations in narrow 5f-band systems lead to multiplet like structures, analogous to those observed in the case of systems with localized electron states. Such observations in essentially band-like 5f-systems was first surprising, but the astonishing similarity of photoemission spectra of very different chemical systems (e.g. PuSe, Pu{sub 2}C{sub 3}..) points to a common origin, relating them to atomic features rather than material dependent density of states (DOS) features. (authors)

  6. The use of Diphonix{sup {trademark}} ion exchange resin as a preconcentration step for the lanthanides and actinides in analytical applications

    SciTech Connect

    Rollins, A.N.; Thakkar, A.H.; Fern, M.J.

    1995-12-01

    Diphonix ion exchange resin is a chelating ion exchange resin containing sulfonic and gemdiphosphonic acid groups. This resin has a high specificity for the lanthanides and actinides, especially at acidities below pH = 3. Currently, we are investigating new ways to use Diphonix resin as a preconcentration step to separate the lanthanides and actinides from interfering elements present in a variety of environmental matrices. Once the lanthanides and actinides have been separated from the interfering matrix constituents, the elements are removed from the resin and passed through subsequent separation schemes. This presentation will outline the use of Diphonix resin with a variety of problem matrices, and demonstrate its usefulness for analysis of the lanthanides and actinides.

  7. A cholesterol and actinide dependent shadow biosphere of archaea and viroids in autoimmune diseases.

    PubMed

    Kurup, Ravikumar; Kurup, Parameswara Achutha

    2012-03-01

    Endogenous digoxin has been related to the pathogenesis of multiple sclerosis and other autoimmune diseases like systemic lupus erythematosis and rheumatoid arthritis. The possibility of endogenous digoxin synthesis by archaea with a mevalonate pathway and cholesterol catabolism was considered. 10 cases each of multiple sclerosis and other autoimmune diseases like systemic lupus erythematosis and rheumatoid arthritis before starting treatment and 10 age and sex matched healthy controls from general population were chosen for the study. Cholesterol substrate was added to the plasma of the patients and the generation of cytochrome F420, free RNA, free DNA, polycyclic aromatic hydrocarbon, hydrogen peroxide, serotonin, pyruvate, ammonia, glutamate, cytochrome C, hexokinase, ATP synthase, HMG CoA reductase, digoxin and bile acids were studied. The changes with the addition of antibiotics and cerium to the patient's plasma were also studied. The statistical analysis was done by ANOVA. The parameters mentioned above were increased the patient's plasma with addition of cholesterol substrate. The addition of antibiotics to the patient's plasma caused a decrease in all the parameters while addition of cerium increased their levels. An actinide dependent shadow biosphere of archaea and viroids is described in multiple sclerosis and other autoimmune diseases like systemic lupus erythematosis and rheumatoid arthritis contributing to their pathogenesis.

  8. Laser rocket system analysis

    NASA Technical Reports Server (NTRS)

    Jones, W. S.; Forsyth, J. B.; Skratt, J. P.

    1979-01-01

    The laser rocket systems investigated in this study were for orbital transportation using space-based, ground-based and airborne laser transmitters. The propulsion unit of these systems utilizes a continuous wave (CW) laser beam focused into a thrust chamber which initiates a plasma in the hydrogen propellant, thus heating the propellant and providing thrust through a suitably designed nozzle and expansion skirt. The specific impulse is limited only by the ability to adequately cool the thruster and the amount of laser energy entering the engine. The results of the study showed that, with advanced technology, laser rocket systems with either a space- or ground-based laser transmitter could reduce the national budget allocated to space transportation by 10 to 345 billion dollars over a 10-year life cycle when compared to advanced chemical propulsion systems (LO2-LH2) of equal capability. The variation in savings depends upon the projected mission model.

  9. Power Plant Systems Analysis

    NASA Technical Reports Server (NTRS)

    Williams, J. R.; Yang, Y. Y.

    1973-01-01

    Three basic thermodynamic cycles of advanced nuclear MHD power plant systems are studied. The effect of reactor exit temperature and space radiator temperature on the overall thermal efficiency of a regenerative turbine compressor power plant system is shown. The effect of MHD pressure ratio on plant efficiency is also described, along with the dependence of MHD power output, compressor power requirement, turbine power output, mass flow rate of H2, and overall plant efficiency on the reactor exit temperature for a specific configuration.

  10. Electrodeposition of actinide compounds from an aqueous ammonium acetate matrix. Experimental development and optimization

    DOE PAGES

    Boll, Rose Ann; Matos, Milan; Torrico, Matthew N.

    2015-03-27

    Electrodeposition is a technique that is routinely employed in nuclear research for the preparation of thin solid films of actinide materials which can be used in accelerator beam bombardments, irradiation studies, or as radioactive sources. The present study investigates the deposition of both lanthanides and actinides from an aqueous ammonium acetate electrolyte matrix. Electrodepositions were performed primarily on stainless steel disks; with yield analysis evaluated using -spectroscopy. Experimental parameters were studied and modified in order to optimize the uniformity and adherence of the deposition while maximizing the yield. The initial development utilized samarium as the plating material, with and withoutmore » a radioactive tracer. As a result, surface characterization studies were performed by scanning electron microscopy, electron microprobe analysis, radiographic imaging, and x-ray diffraction.« less

  11. Electrodeposition of actinide compounds from an aqueous ammonium acetate matrix. Experimental development and optimization

    SciTech Connect

    Boll, Rose Ann; Matos, Milan; Torrico, Matthew N.

    2015-03-27

    Electrodeposition is a technique that is routinely employed in nuclear research for the preparation of thin solid films of actinide materials which can be used in accelerator beam bombardments, irradiation studies, or as radioactive sources. The present study investigates the deposition of both lanthanides and actinides from an aqueous ammonium acetate electrolyte matrix. Electrodepositions were performed primarily on stainless steel disks; with yield analysis evaluated using -spectroscopy. Experimental parameters were studied and modified in order to optimize the uniformity and adherence of the deposition while maximizing the yield. The initial development utilized samarium as the plating material, with and without a radioactive tracer. As a result, surface characterization studies were performed by scanning electron microscopy, electron microprobe analysis, radiographic imaging, and x-ray diffraction.

  12. Land Analysis System (LAS)

    NASA Technical Reports Server (NTRS)

    Pease, P. B.

    1989-01-01

    Version 4.1 of LAS provides flexible framework for algorithm development and processing and analysis of image data. Over 500,000 lines of code enable image repair, clustering, classification, film processing, geometric registration, radiometric correction, and manipulation of image statistics.

  13. Exergy Analysis of Rocket Systems

    NASA Technical Reports Server (NTRS)

    Gilbert, Andrew; Mesmer, Bryan; Watson, Michael D.

    2015-01-01

    Exergy is defined as the useful work available from a system in a specified environment. Exergy analysis allows for comparison between different system designs, and allows for comparison of subsystem efficiencies within system designs. The proposed paper explores the relationship between the fundamental rocket equation and an exergy balance equation. A previously derived exergy equation related to rocket systems is investigated, and a higher fidelity analysis will be derived. The exergy assessments will enable informed, value-based decision making when comparing alternative rocket system designs, and will allow the most efficient configuration among candidate configurations to be determined.

  14. Actinide Solubility and Speciation in the WIPP

    SciTech Connect

    Reed, Donald T.

    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.

  15. Miniaturized flow injection analysis system

    DOEpatents

    Folta, James A.

    1997-01-01

    A chemical analysis technique known as flow injection analysis, wherein small quantities of chemical reagents and sample are intermixed and reacted within a capillary flow system and the reaction products are detected optically, electrochemically, or by other means. A highly miniaturized version of a flow injection analysis system has been fabricated utilizing microfabrication techniques common to the microelectronics industry. The microflow system uses flow capillaries formed by etching microchannels in a silicon or glass wafer followed by bonding to another wafer, commercially available microvalves bonded directly to the microflow channels, and an optical absorption detector cell formed near the capillary outlet, with light being both delivered and collected with fiber optics. The microflow system is designed mainly for analysis of liquids and currently measures 38.times.25.times.3 mm, but can be designed for gas analysis and be substantially smaller in construction.

  16. Miniaturized flow injection analysis system

    DOEpatents

    Folta, J.A.

    1997-07-01

    A chemical analysis technique known as flow injection analysis is described, wherein small quantities of chemical reagents and sample are intermixed and reacted within a capillary flow system and the reaction products are detected optically, electrochemically, or by other means. A highly miniaturized version of a flow injection analysis system has been fabricated utilizing microfabrication techniques common to the microelectronics industry. The microflow system uses flow capillaries formed by etching microchannels in a silicon or glass wafer followed by bonding to another wafer, commercially available microvalves bonded directly to the microflow channels, and an optical absorption detector cell formed near the capillary outlet, with light being both delivered and collected with fiber optics. The microflow system is designed mainly for analysis of liquids and currently measures 38{times}25{times}3 mm, but can be designed for gas analysis and be substantially smaller in construction. 9 figs.

  17. Canister Model, Systems Analysis

    1993-09-29

    This packges provides a computer simulation of a systems model for packaging nuclear waste and spent nuclear fuel in canisters. The canister model calculates overall programmatic cost, number of canisters, and fuel and waste inventories for the Idaho Chemical Processing Plant (other initial conditions can be entered).

  18. WASTE COMBUSTION SYSTEM ANALYSIS

    EPA Science Inventory

    The report gives results of a study of biomass combustion alternatives. The objective was to evaluate the thermal performance and costs of available and developing biomass systems. The characteristics of available biomass fuels were reviewed, and the performance parameters of alt...

  19. A new incorporation mechanism for trivalent actinides into bioapatite: a TRLFS and EXAFS study.

    PubMed

    Holliday, Kiel; Handley-Sidhu, Stephanie; Dardenne, Kathy; Renshaw, Joanna; Macaskie, Lynne; Walther, Clemens; Stumpf, Thorsten

    2012-02-28

    One of the most toxic byproducts of nuclear power and weapons production is the transuranics, which have a high radiotoxicity and long biological half-life due to their tendency to accumulate in the skeletal system. This accumulation is inhomogeneous and has been associated with the chemical properties and structure of the bone material rather than its location or function. This suggests a chemical driving force to incorporation and requires an atomic scale mechanistic understanding of the incorporation process. Here we propose a new incorporation mechanism for trivalent actinides and lanthanides into synthetic and biologically produced hydroxyapatite. Time-resolved laser fluorescence spectroscopy and extended X-ray absorption fine structure have been used to demonstrate that trivalent actinides and lanthanides incorporate into the amorphous grain boundaries of apatite. This incorporation site can be used to explain patterns in uptake and distribution of radionuclides in the mammalian skeletal system. PMID:22313032

  20. A new incorporation mechanism for trivalent actinides into bioapatite: a TRLFS and EXAFS study.

    PubMed

    Holliday, Kiel; Handley-Sidhu, Stephanie; Dardenne, Kathy; Renshaw, Joanna; Macaskie, Lynne; Walther, Clemens; Stumpf, Thorsten

    2012-02-28

    One of the most toxic byproducts of nuclear power and weapons production is the transuranics, which have a high radiotoxicity and long biological half-life due to their tendency to accumulate in the skeletal system. This accumulation is inhomogeneous and has been associated with the chemical properties and structure of the bone material rather than its location or function. This suggests a chemical driving force to incorporation and requires an atomic scale mechanistic understanding of the incorporation process. Here we propose a new incorporation mechanism for trivalent actinides and lanthanides into synthetic and biologically produced hydroxyapatite. Time-resolved laser fluorescence spectroscopy and extended X-ray absorption fine structure have been used to demonstrate that trivalent actinides and lanthanides incorporate into the amorphous grain boundaries of apatite. This incorporation site can be used to explain patterns in uptake and distribution of radionuclides in the mammalian skeletal system.

  1. Evaluation of Fluid Conduction and Mixing within a Subassembly of the Actinide Burner Test Reactor

    SciTech Connect

    Cliff B. Davis

    2007-09-01

    The RELAP5-3D code is being considered as a thermal-hydraulic system code to support the development of the sodium-cooled Actinide Burner Test Reactor as part of the Global Nuclear Energy Partnership. An evaluation was performed to determine whether the control system could be used to simulate the effects of non-convective mechanisms of heat transport in the fluid, including axial and radial heat conduction and subchannel mixing, that are not currently represented with internal code models. The evaluation also determined the relative importance of axial and radial heat conduction and fluid mixing on peak cladding temperature for a wide range of steady conditions and during a representative loss-of-flow transient. The evaluation was performed using a RELAP5-3D model of a subassembly in the Experimental Breeder Reactor-II, which was used as a surrogate for the Actinide Burner Test Reactor.

  2. Systems analysis-independent analysis and verification

    SciTech Connect

    Badin, J.S.; DiPietro, J.P.

    1995-09-01

    The DOE Hydrogen Program is supporting research, development, and demonstration activities to overcome the barriers to the integration of hydrogen into the Nation`s energy infrastructure. Much work is required to gain acceptance of hydrogen energy system concepts and to develop them for implementation. A systems analysis database has been created that includes a formal documentation of technology characterization profiles and cost and performance information. Through a systematic and quantitative approach, system developers can understand and address important issues and thereby assure effective and timely commercial implementation. This project builds upon and expands the previously developed and tested pathway model and provides the basis for a consistent and objective analysis of all hydrogen energy concepts considered by the DOE Hydrogen Program Manager. This project can greatly accelerate the development of a system by minimizing the risk of costly design evolutions, and by stimulating discussions, feedback, and coordination of key players and allows them to assess the analysis, evaluate the trade-offs, and to address any emerging problem areas. Specific analytical studies will result in the validation of the competitive feasibility of the proposed system and identify system development needs. Systems that are investigated include hydrogen bromine electrolysis, municipal solid waste gasification, electro-farming (biomass gasifier and PEM fuel cell), wind/hydrogen hybrid system for remote sites, home electrolysis and alternate infrastructure options, renewable-based electrolysis to fuel PEM fuel cell vehicle fleet, and geothermal energy used to produce hydrogen. These systems are compared to conventional and benchmark technologies. Interim results and findings are presented. Independent analyses emphasize quality, integrity, objectivity, a long-term perspective, corporate memory, and the merging of technical, economic, operational, and programmatic expertise.

  3. Arctic Climate Systems Analysis

    SciTech Connect

    Ivey, Mark D.; Robinson, David G.; Boslough, Mark B.; Backus, George A.; Peterson, Kara J.; van Bloemen Waanders, Bart G.; Swiler, Laura Painton; Desilets, Darin Maurice; Reinert, Rhonda Karen

    2015-03-01

    This study began with a challenge from program area managers at Sandia National Laboratories to technical staff in the energy, climate, and infrastructure security areas: apply a systems-level perspective to existing science and technology program areas in order to determine technology gaps, identify new technical capabilities at Sandia that could be applied to these areas, and identify opportunities for innovation. The Arctic was selected as one of these areas for systems level analyses, and this report documents the results. In this study, an emphasis was placed on the arctic atmosphere since Sandia has been active in atmospheric research in the Arctic since 1997. This study begins with a discussion of the challenges and benefits of analyzing the Arctic as a system. It goes on to discuss current and future needs of the defense, scientific, energy, and intelligence communities for more comprehensive data products related to the Arctic; assess the current state of atmospheric measurement resources available for the Arctic; and explain how the capabilities at Sandia National Laboratories can be used to address the identified technological, data, and modeling needs of the defense, scientific, energy, and intelligence communities for Arctic support.

  4. Energy-Systems Economic Analysis

    NASA Technical Reports Server (NTRS)

    Doane, J.; Slonski, M. L.; Borden, C. S.

    1982-01-01

    Energy Systems Economic Analysis (ESEA) program is flexible analytical tool for rank ordering of alternative energy systems. Basic ESEA approach derives an estimate of those costs incurred as result of purchasing, installing and operating an energy system. These costs, suitably aggregated into yearly costs over lifetime of system, are divided by expected yearly energy output to determine busbar energy costs. ESEA, developed in 1979, is written in FORTRAN IV for batch execution.

  5. End point control of an actinide precipitation reactor

    SciTech Connect

    Muske, K.R.; Palmer, M.J.

    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.

  6. On the Suitability of Lanthanides as Actinide Analogs

    SciTech Connect

    Szigethy, Geza; Raymond, Kenneth N.

    2008-04-11

    With the current level of actinide materials used in civilian power generation and the need for safe and efficient methods for the chemical separation of these species from their daughter products and for long-term storage requirements, a detailed understanding of actinide chemistry is of great importance. Due to the unique bonding properties of the f-elements, the lanthanides are commonly used as structural and chemical models for the actinides, but differences in the bonding between these 4f and 5f elements has become a question of immediate applicability to separations technology. This brief overview of actinide coordination chemistry in the Raymond group at UC Berkeley/LBNL examines the validity of using lanthanide analogs as structural models for the actinides, with particular attention paid to single crystal X-ray diffraction structures. Although lanthanides are commonly accepted as reasonable analogs for the actinides, these comparisons suggest the careful study of actinide materials independent of their lanthanide analogs to be of utmost importance to present and future efforts in nuclear industries.

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

    PubMed

    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.

  8. Gas core reactors for actinide transmutation. [uranium hexafluoride

    NASA Technical Reports Server (NTRS)

    Clement, J. D.; Rust, J. H.; Wan, P. T.; Chow, S.

    1979-01-01

    The preliminary design of a uranium hexafluoride actinide transmutation reactor to convert long-lived actinide wastes to shorter-lived fission product wastes was analyzed. It is shown that externally moderated gas core reactors are ideal radiators. They provide an abundant supply of thermal neutrons and are insensitive to composition changes in the blanket. For the present reactor, an initial load of 6 metric tons of actinides is loaded. This is equivalent to the quantity produced by 300 LWR-years of operation. At the beginning, the core produces 2000 MWt while the blanket generates only 239 MWt. After four years of irradiation, the actinide mass is reduced to 3.9 metric tonnes. During this time, the blanket is becoming more fissile and its power rapidly approaches 1600 MWt. At the end of four years, continuous refueling of actinides is carried out and the actinide mass is held constant. Equilibrium is essentially achieved at the end of eight years. At equilibrium, the core is producing 1400 MWt and the blanket 1600 MWt. At this power level, the actinide destruction rate is equal to the production rate from 32 LWRs.

  9. Plutonium and ''minor'' actinides: safe sequestration [rapid communication

    NASA Astrophysics Data System (ADS)

    Ewing, Rodney C.

    2005-01-01

    The actinides exhibit a number of unique chemical and nuclear properties. Of particular interest are the man-made actinides (Np, Pu, Cm and Am) that are produced in significant enough quantities that they are a source of energy in fission reactions, a source of fissile material for nuclear weapons and of environmental concern because of their long half-lives and radiotoxicity. During the past 50 yr, over 1400 mT of Pu and substantial quantities of the "minor" actinides, such as Np, Am and Cm, have been generated in nuclear reactors. There are two basic strategies for the disposition of these elements: (1) to "burn" or transmute the actinides using nuclear reactors or accelerators; (2) to "sequester" the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of isometric pyrochlore, A 2B 2O 7 (A=rare earths; B=Ti, Zr, Sn and Hf), for the immobilization of actinides, particularly plutonium. Systematic studies of rare-earth pyrochlores have led to the discovery that certain compositions (B=Zr, Hf) are stable to very high doses of α-decay event damage. The radiation stability of these compositions is closely related to the structural distortions that occur for specific pyrochlore compositions and the electronic structure of the B-site cation. This understanding provides the basis for designing materials for the safe, long-term immobilization and sequestration of actinides.

  10. Surface Complexation of Actinides with Iron Oxides: Implications for Radionuclide Transport in Near-Surface Aquifers

    NASA Astrophysics Data System (ADS)

    Jerden, J. L.; Kropf, A. J.; Tsai, Y.

    2005-12-01

    The surface complexation of actinides with iron oxides plays a key role in actinide transport and retardation in geosphere-biosphere systems. The development of accurate actinide transport models therefore requires a mechanistic understanding of surface complexation reactions (i.e. knowledge of chemical speciation at mineral/fluid interfaces). Iron oxides are particularly important actinide sorbents due to their pH dependent surface charges, relatively high surface areas and ubiquity in oxic and suboxic near-surface systems. In this paper we present results from field and laboratory investigations that elucidate the mechanisms involved in binding uranium and neptunium to iron oxide mineral substrates in near neutral groundwaters. The field study involved sampling and characterizing uranium-bearing groundwaters and solids from a saprolite aquifer overlying an unmined uranium deposit in the Virginia Piedmont. The groundwaters were analyzed by inductively coupled mass spectrometry and ion chromatography and the aquifer solids were analyzed by electron microprobe. The laboratory study involved a series of batch sorption tests in which U(VI) and Np(V) were reacted with goethite, hematite and magnetite in simulated groundwaters. The pH, ionic strength, aging time, and sorbent/sorbate ratios were varied in these experiments. The oxidation state and coordination environment of neptunium in solutions and sorbents from the batch tests were characterized by X-ray absorption spectroscopy (XAS) at the Advanced Photon Source, Argonne National Laboratory. Results from this work indicate that, in oxidizing near-surface aquifers, the dissolved concentration of uranium may be limited to less than 30 parts per billion due to uptake by iron oxide mineral coatings and the precipitation of sparingly soluble U(VI) phosphate minerals. Results from the batch adsorption tests showed that, in near neutral groundwaters, a significant fraction of the uranium and neptunium adsorbed as strongly

  11. SURFACE COMPLEXATION OF ACTINIDES WITH IRON OXIDES: IMPLICATIONS FOR RADIONUCLIDE TRANSPORT IN NEAR-SURFACE AQUIFERS

    SciTech Connect

    J.L. Jerden Jr.; A.J. Kropf; Y. Tsai

    2005-08-25

    The surface complexation of actinides with iron oxides plays a key role in actinide transport and retardation in geosphere-biosphere systems. The development of accurate actinide transport models therefore requires a mechanistic understanding of surface complexation reactions (i.e. knowledge of chemical speciation at mineral/fluid interfaces). Iron oxides are particularly important actinide sorbents due to their pH dependent surface charges, relatively high surface areas and ubiquity in oxic and suboxic near-surface systems. In this paper we present results from field and laboratory investigations that elucidate the mechanisms involved in binding uranium and neptunium to iron oxide mineral substrates in near neutral groundwaters. The field study involved sampling and characterizing uranium-bearing groundwaters and solids from a saprolite aquifer overlying an unmined uranium deposit in the Virginia Piedmont. The groundwaters were analyzed by inductively coupled mass spectrometry and ion chromatography and the aquifer solids were analyzed by electron microprobe. The laboratory study involved a series of batch sorption tests in which U(VI) and Np(V) were reacted with goethite, hematite and magnetite in simulated groundwaters. The pH, ionic strength, aging time, and sorbent/sorbate ratios were varied in these experiments. The oxidation state and coordination environment of neptunium in solutions and sorbents from the batch tests were characterized by X-ray absorption spectroscopy (XAS) at the Advanced Photon Source, Argonne National Laboratory. Results from this work indicate that, in oxidizing near-surface aquifers, the dissolved concentration of uranium may be limited to less than 30 parts per billion due to uptake by iron oxide mineral coatings and the precipitation of sparingly soluble U(VI) phosphate minerals. Results from the batch adsorption tests showed that, in near neutral groundwaters, a significant fraction of the uranium and neptunium adsorbed as strongly

  12. Human factors and safety issues associated with actinide retrieval from spent light water reactor fuel assemblies

    SciTech Connect

    Spelt, P.F.

    1992-01-01

    A major problem in environmental restoration and waste management is the disposition of used fuel assemblies from the many light water reactors in the United States, which present a radiation hazard to those whose job is to dispose of them, with a similar threat to the general environment associated with long-term storage in fuel repositories around the country. Actinides resident in the fuel pins as a result of their use in reactor cores constitute a significant component of this hazard. Recently, the Department of Energy has initiated an Actinide Recycle Program to study the feasibility of using pyrochemical (molten salt) processes to recover actinides from the spent fuel assemblies of commercial reactors. This project concerns the application of robotics technology to the operation and maintenance functions of a plant whose objective is to recover actinides from spent fuel assemblies, and to dispose of the resulting hardware and chemical components from this process. Such a procedure involves a number of safety and human factors issues. The purpose of the project is to explore the use of robotics and artificial intelligence to facilitate accomplishment of the program goals while maintaining the safety of the humans doing the work and the integrity of the environment. This project will result in a graphic simulation on a Silicon Graphics workstation as a proof of principle demonstration of the feasibility of using robotics along with an intelligent operator interface. A major component of the operator-system interface is a hybrid artificial intelligence system developed at Oak Ridge National Laboratory, which combines artificial neural networks and an expert system into a hybrid, self-improving computer-based system interface. 10 refs.

  13. Human factors and safety issues associated with actinide retrieval from spent light water reactor fuel assemblies

    SciTech Connect

    Spelt, P.F.

    1992-08-01

    A major problem in environmental restoration and waste management is the disposition of used fuel assemblies from the many light water reactors in the United States, which present a radiation hazard to those whose job is to dispose of them, with a similar threat to the general environment associated with long-term storage in fuel repositories around the country. Actinides resident in the fuel pins as a result of their use in reactor cores constitute a significant component of this hazard. Recently, the Department of Energy has initiated an Actinide Recycle Program to study the feasibility of using pyrochemical (molten salt) processes to recover actinides from the spent fuel assemblies of commercial reactors. This project concerns the application of robotics technology to the operation and maintenance functions of a plant whose objective is to recover actinides from spent fuel assemblies, and to dispose of the resulting hardware and chemical components from this process. Such a procedure involves a number of safety and human factors issues. The purpose of the project is to explore the use of robotics and artificial intelligence to facilitate accomplishment of the program goals while maintaining the safety of the humans doing the work and the integrity of the environment. This project will result in a graphic simulation on a Silicon Graphics workstation as a proof of principle demonstration of the feasibility of using robotics along with an intelligent operator interface. A major component of the operator-system interface is a hybrid artificial intelligence system developed at Oak Ridge National Laboratory, which combines artificial neural networks and an expert system into a hybrid, self-improving computer-based system interface. 10 refs.

  14. SUBSURFACE VISUAL ALARM SYSTEM ANALYSIS

    SciTech Connect

    D.W. Markman

    2001-08-06

    The ''Subsurface Fire Hazard Analysis'' (CRWMS M&O 1998, page 61), and the document, ''Title III Evaluation Report for the Surface and Subsurface Communication System'', (CRWMS M&O 1999a, pages 21 and 23), both indicate the installed communication system is adequate to support Exploratory Studies Facility (ESF) activities with the exception of the mine phone system for emergency notification purposes. They recommend the installation of a visual alarm system to supplement the page/party phone system The purpose of this analysis is to identify data communication highway design approaches, and provide justification for the selected or recommended alternatives for the data communication of the subsurface visual alarm system. This analysis is being prepared to document a basis for the design selection of the data communication method. This analysis will briefly describe existing data or voice communication or monitoring systems within the ESF, and look at how these may be revised or adapted to support the needed data highway of the subsurface visual alarm. system. The existing PLC communication system installed in subsurface is providing data communication for alcove No.5 ventilation fans, south portal ventilation fans, bulkhead doors and generator monitoring system. It is given that the data communication of the subsurface visual alarm system will be a digital based system. It is also given that it is most feasible to take advantage of existing systems and equipment and not consider an entirely new data communication system design and installation. The scope and primary objectives of this analysis are to: (1) Briefly review and describe existing available data communication highways or systems within the ESF. (2) Examine technical characteristics of an existing system to disqualify a design alternative is paramount in minimizing the number of and depth of a system review. (3) Apply general engineering design practices or criteria such as relative cost, and degree of

  15. Complex System Ensemble Analysis

    NASA Astrophysics Data System (ADS)

    Pearson, Carl A.

    A new measure for interaction network ensembles and their dynamics is presented: the ensemble transition matrix, T, the proportions of networks in an ensemble that support particular transitions. That presentation begins with generation of the ensemble and application of constraint perturbations to compute T, including estimating alternatives to accommodate cases where the problem size becomes computationally intractable. Then, T is used to predict ensemble dynamics properties in expected-value like calculations. Finally, analyses from the two complementary assumptions about T - that it represents uncertainty about a unique system or that it represents stochasticity around a unique constraint - are presented: entropy-based experiment selection and generalized potentials/heat dissipation of the system, respectively. Extension of these techniques to more general graph models is described, but not demonstrated. Future directions for research using T are proposed in the summary chapter. Throughout this work, the presentation of various calculations involving T are motivated by the Budding Yeast Cell Cycle example, with argument for the generality of the approaches presented by the results of their application to a database of pseudo-randomly generated dynamic constraints.

  16. 5f-electron localization in the actinide metals: thorides, actinides and the Mott transition

    NASA Astrophysics Data System (ADS)

    Lawson, A. C.

    2016-03-01

    For the light actinides Ac-Cm, the numbers of localized and itinerant 5f-electrons are determined by comparing various estimates of the f-electron counts. At least one itinerant f-electron is found for each element, Pa-Cm. These results resolve certain disagreements among electron counts determined by different methods and are consistent with the Mott transition model and with the picture of the 5f-electrons' dual nature.

  17. Information systems vulnerability: A systems analysis perspective

    SciTech Connect

    Wyss, G.D.; Daniel, S.L.; Schriner, H.K.; Gaylor, T.R.

    1996-07-01

    Vulnerability analyses for information systems are complicated because the systems are often geographically distributed. Sandia National Laboratories has assembled an interdisciplinary team to explore the applicability of probabilistic logic modeling (PLM) techniques (including vulnerability and vital area analysis) to examine the risks associated with networked information systems. The authors have found that the reliability and failure modes of many network technologies can be effectively assessed using fault trees and other PLM methods. The results of these models are compatible with an expanded set of vital area analysis techniques that can model both physical locations and virtual (logical) locations to identify both categories of vital areas simultaneously. These results can also be used with optimization techniques to direct the analyst toward the most cost-effective security solution.

  18. Chemistry of tetravalent actinide phosphates-Part I

    SciTech Connect

    Brandel, V. . E-mail: vbrandel@neuf.fr; Dacheux, N. . E-mail: dacheux@ipno.in2p3.fr

    2004-12-01

    The chemistry and crystal structure of phosphates of tetravalent cations, including that of actinides was reviewed several times up to 1985. Later, new compounds were synthesized and characterized. In more recent studies, it was found that some of previously reported phases, especially those of thorium, uranium and neptunium, were wrongly identified. In the light of these new facts an update review and classification of the tetravalent actinide phosphates is proposed in the two parts of this paper. Their crystal structure and some chemical properties are also compared to non-actinide cation phosphates.

  19. Engineering-Scale Distillation of Cadmium for Actinide Recovery

    SciTech Connect

    J.C. Price; D. Vaden; R.W. Benedict

    2007-10-01

    During the recovery of actinide products from spent nuclear fuel, cadmium is separated from the actinide products by a distillation process. Distillation occurs in an induction-heated furnace called a cathode processor capable of processing kilogram quantities of cadmium. Operating parameters have been established for sufficient recovery of the cadmium based on mass balance and product purity. A cadmium distillation rate similar to previous investigators has also been determined. The development of cadmium distillation for spent fuel treatment enhances the capabilities for actinide recovery processes.

  20. Process to remove actinides from soil using magnetic separation

    DOEpatents

    Avens, Larry R.; Hill, Dallas D.; Prenger, F. Coyne; Stewart, Walter F.; Tolt, Thomas L.; Worl, Laura A.

    1996-01-01

    A process of separating actinide-containing components from an admixture including forming a slurry including actinide-containing components within an admixture, said slurry including a dispersion-promoting surfactant, adjusting the pH of the slurry to within a desired range, and, passing said slurry through a pretreated matrix material, said matrix material adapted to generate high magnetic field gradients upon the application of a strong magnetic field exceeding about 0.1 Tesla whereupon a portion of said actinide-containing components are separated from said slurry and remain adhered upon said matrix material is provided.

  1. An emergency bioassay method for actinides in urine.

    PubMed

    Dai, Xiongxin; Kramer-Tremblay, Sheila

    2011-08-01

    A rapid bioassay method has been developed for the sequential measurements of actinides in human urine samples. The method involves actinide separation from a urine matrix by co-precipitation with hydrous titanium oxide (HTiO), followed by anion exchange and extraction chromatography column purification, and final counting by alpha spectrometry after cerium fluoride micro-precipitation. The minimal detectable activities for the method were determined to be 20 mBq L(-1) or less for plutonium, uranium, americium and curium isotopes, with an 8-h sample turn-around time. Spike tests showed that this method would meet the requirements for actinide bioassay following a radiation emergency.

  2. Hydrothermal Synthesis and Crystal Structures of Actinide Compounds

    NASA Astrophysics Data System (ADS)

    Runde, Wolfgang; Neu, Mary P.

    Since the 1950s actinides have been used to benefit industry, science, health, and national security. The largest industrial application, electricity generation from uranium and thorium fuels, is growing worldwide. Thus, more actinides are being mined, produced, used and processed than ever before. The future of nuclear energy hinges on how these increasing amounts of actinides are contained in each stage of the fuel cycle, including disposition. In addition, uranium and plutonium were built up during the Cold War between the United States and the Former Soviet Union for defense purposes and nuclear energy. These stockpiles have been significantly reduced in the last decade.

  3. Separations and Actinide Science -- 2005 Roadmap

    SciTech Connect

    Not Available

    2005-09-01

    The Separations and Actinide Science Roadmap presents a vision to establish a separations and actinide science research (SASR) base composed of people, facilities, and collaborations and provides new and innovative nuclear fuel cycle solutions to nuclear technology issues that preclude nuclear proliferation. This enabling science base will play a key role in ensuring that Idaho National Laboratory (INL) achieves its long-term vision of revitalizing nuclear energy by providing needed technologies to ensure our nation's energy sustainability and security. To that end, this roadmap suggests a 10-year journey to build a strong SASR technical capability with a clear mission to support nuclear technology development. If nuclear technology is to be used to satisfy the expected growth in U.S. electrical energy demand, the once-through fuel cycle currently in use should be reconsidered. Although the once-through fuel cycle is cost-effective and uranium is inexpensive, a once-through fuel cycle requires long-term disposal to protect the environment and public from long-lived radioactive species. The lack of a current disposal option (i.e., a licensed repository) has resulted in accumulation of more than 50,000 metric tons of spent nuclear fuel. The process required to transition the current once-through fuel cycle to full-recycle will require considerable time and significant technical advancement. INL's extensive expertise in aqueous separations will be used to develop advanced separations processes. Computational chemistry will be expanded to support development of future processing options. In the intermediate stage of this transition, reprocessing options will be deployed, waste forms with higher loading densities and greater stability will be developed, and transmutation of long-lived fission products will be explored. SASR will support these activities using its actinide science and aqueous separations expertise. In the final stage, full recycle will be enabled by

  4. Thermal Analysis System

    NASA Technical Reports Server (NTRS)

    DiStefano, III, Frank James (Inventor); Wobick, Craig A. (Inventor); Chapman, Kirt Auldwin (Inventor); McCloud, Peter L. (Inventor)

    2014-01-01

    A thermal fluid system modeler including a plurality of individual components. A solution vector is configured and ordered as a function of one or more inlet dependencies of the plurality of individual components. A fluid flow simulator simulates thermal energy being communicated with the flowing fluid and between first and second components of the plurality of individual components. The simulation extends from an initial time to a later time step and bounds heat transfer to be substantially between the flowing fluid, walls of tubes formed in each of the individual components of the plurality, and between adjacent tubes. Component parameters of the solution vector are updated with simulation results for each of the plurality of individual components of the simulation.

  5. Detailed studies of Minor Actinide transmutation-incineration in high-intensity neutron fluxes

    SciTech Connect

    Bringer, O.; Blandin, C.; Oriol, L.

    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)

  6. Dounreay PFR irradiation history for the joint US/UK actinide sample exposures

    SciTech Connect

    Raman, S.; Murphy, B.D.; Nestor, C.W. Jr.

    1995-07-01

    The operating history of the Dounreay Prototype Fast Reactor is presented to the extent that it is relevant to the irradiation of actinide specimens that were subsequently analyzed at Oak Ridge National Laboratory (ORNL). Three fuel pins with actinide samples were irradiated from July 1982 to July 1988 and returned to ORNL for analysis. They contained isotopes of elements from thorium to curium. The times when each of these fuel pins were in the reactor core are described as are the operating power levels and neutron spectra. The appendices give daily power levels of the reactor as well as six-group neutron energy spectra for various times and axial positions in the core.

  7. End effect K{sub eff} bias curve for actinide-only burnup credit casks

    SciTech Connect

    Kang, C.H.; Lancaster, D.B.

    1997-03-01

    A conservative end effect k{sub eff} bias curve for actinide-only burnup credit for spent fuel casks is presented in this paper. The k{sub eff} bias values can be added to the uniform axial burnup analysis to conservatively bound the actinide-only end effect. A normalized axial burnup distribution for the standard Westinghouse 17 x 17 assembly design is used for calculating k{sub eff}. The end effect calculated is a strong function of burnup, and increases as cask size size decreases. The presence of poison plates increases the end effect. The bias curve presented is based on the most limiting cask configuration of a single PWR assembly with completely black poison plates. Therefore, axially uniform criticality calculations with application of the proposed k{sub eff} could eliminate the need for axially burnup dependent analyses. 7 refs., 1 fig.

  8. Engineering test plan for US/UK higher actinides irradiations tests

    SciTech Connect

    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.

  9. System safety engineering analysis handbook

    NASA Technical Reports Server (NTRS)

    Ijams, T. E.

    1972-01-01

    The basic requirements and guidelines for the preparation of System Safety Engineering Analysis are presented. The philosophy of System Safety and the various analytic methods available to the engineering profession are discussed. A text-book description of each of the methods is included.

  10. Speech Analysis Systems: An Evaluation.

    ERIC Educational Resources Information Center

    Read, Charles; And Others

    1992-01-01

    Performance characteristics are reviewed for seven computerized systems marketed for acoustic speech analysis: CSpeech, CSRE, ILS-PC, Kay Elemetrics model 550 Sona-Graph, MacSpeech Lab II, MSL, and Signalyze. Characteristics reviewed include system components, basic capabilities, documentation, user interface, data formats and journaling, and…

  11. Theoretical atomic volumes of the light actinides

    SciTech Connect

    Jones, M. D.; Boettger, J. C.; Albers, R. C.; Singh, D. J.

    2000-02-15

    The zero-pressure zero-temperature equilibrium volumes and bulk moduli are calculated for the light actinides Th through Pu using two independent all-electron, full-potential, electronic-structure methods: the full-potential linear augmented-plane-wave method and the linear combinations of Gaussian-type orbitals-fitting function method. The results produced by these two distinctly different electronic-structure techniques are in good agreement with each other, but differ significantly from previously published calculations using the full-potential linear muffin-tin-orbital (FP-LMTO) method. The theoretically calculated equilibrium volumes are in some cases nearly 10% larger than the previous FP-LMTO calculations, bringing them much closer to the experimentally observed volumes. We also discuss the anomalous upturn in equilibrium volume seen experimentally for {alpha}-Pu. (c) 2000 The American Physical Society.

  12. Complexation of actinides with derivatives of oxydiaceticacid

    SciTech Connect

    Rao, Linfeng; Tian, Guoxin

    2006-01-04

    Complexation of Np(V), U(VI) and Nd(III) with dimethyl-3-oxa-glutaramic acid (DMOGA) and tetramethyl-3-oxa-glutaramide (TMOGA) was studied in comparison with the complexation with oxydiacetic acid (ODA). Stability constants and enthalpy of complexation were determined by potentiometry, spectrophotometry and calorimetry. Thermodynamic parameters, in conjunction with structural information of solid compounds, indicate that DMOGA and TMOGA form tridentate complexes with the ether-oxygen participating in bonding with actinide/lanthanide ions. The trends in the stability constants, enthalpy and entropy of complexation are discussed in terms of the difference in the hydration of the amide groups and carboxylate groups and the difference in the charge density of the metal ions.

  13. Microfabricated Genomic Analysis System

    NASA Technical Reports Server (NTRS)

    Gonda, Steve; Elms, Rene

    2005-01-01

    Genetic sequencing and many genetic tests and assays require electrophoretic separation of DNA. In this technique, DNA fragments are separated by size as they migrate through a sieving gel under the influence of an applied electric field. In order to conduct these analyses on-orbit, it is essential to acquire the capability to efficiently perform electrophoresis in a microgravity environment. Conventional bench top electrophoresis equipment is large and cumbersome and does not lead itself to on-orbit utilization. Much of the previous research regarding on-orbit electrophoresis involved altering conventional electrophoresis equipment for bioprocessing, purification, and/or separation technology applications. A new and more efficient approach to on-orbit electrophoresis is the use of a microfabricated electrophoresis platform. These platforms are much smaller, less expensive to produce and operate, use less power, require smaller sample sizes (nanoliters), and achieve separation in a much shorter distance (a few centimeters instead of 10 s or 100 s of centimeters.) In contrast to previous applications, this platform would be utilized as an analytical tool for life science/medical research, environmental monitoring, and medical diagnoses. Identification of infectious agents as well as radiation related damage are significant to NASA s efforts to maintain, study, and monitor crew health during and in support of near-Earth and interplanetary missions. The capability to perform genetic assays on-orbit is imperative to conduct relevant and insightful biological and medical research, as well as continuing NASA s search for life elsewhere. This technology would provide an essential analytical tool for research conducted in a microgravity environment (Shuttle, ISS, long duration/interplanetary missions.) In addition, this technology could serve as a critical and invaluable component of a biosentinel system to monitor space environment genotoxic insults to include radiation.

  14. Actinide cross section program at ORELA

    SciTech Connect

    Dabbs, J. W.T.

    1980-01-01

    The actinide cross section program at ORELA, the Oak Ridge Electron Linear Accelerator, is aimed at obtaining accurate neutron cross sections (primarily fission, capture, and total) for actinide nuclides which occur in fission reactors. Such cross sections, measured as a function of neutron energy over as wide a range of energies as feasible, comprise a data base that permits calculated predictions of the formation and removal of these nuclides in reactors. The present program is funded by the Division of Basic Energy Sciences of DOE, and has components in several divisions at ORNL. For intensively ..cap alpha..-active nuclides, many of the existing fission cross section data have been provided by underground explosions. New measurement techniques, developed at ORELA, now permit linac measurements on fissionable nuclides with alpha half-lives as short as 28 years. Capture and capture-plus-fission measurements utilize scintillation detectors (of capture ..gamma.. rays and fission neutrons) in which pulse shape discrimination plays an important role. Total cross sections can be measured at ORELA on samples of only a few milligrams. A simultaneous program of chemical and isotopic analyses of samples irradiated in EBR-II is in progress to provide benchmarks for the existing differential measurements. These analyses are being studied with updated versions of ORIGEN and with sensitivity determinations. Calculations of the sensitivity to cross section changes of various aspects of the nuclear fuel cycle are also being made. Even in this relatively mature field, many cross sections still require improvements to provide an adequate data base. Examples of recent techniques and measurements are presented. 12 figures, 3 tables.

  15. Space elevator systems level analysis

    SciTech Connect

    Laubscher, B. E.

    2004-01-01

    The Space Elevator (SE) represents a major paradigm shift in space access. It involves new, untried technologies in most of its subsystems. Thus the successful construction of the SE requires a significant amount of development, This in turn implies a high level of risk for the SE. This paper will present a systems level analysis of the SE by subdividing its components into their subsystems to determine their level of technological maturity. such a high-risk endeavor is to follow a disciplined approach to the challenges. A systems level analysis informs this process and is the guide to where resources should be applied in the development processes. It is an efficient path that, if followed, minimizes the overall risk of the system's development. systems level analysis is that the overall system is divided naturally into its subsystems, and those subsystems are further subdivided as appropriate for the analysis. By dealing with the complex system in layers, the parameter space of decisions is kept manageable. Moreover, A rational way to manage One key aspect of a resources are not expended capriciously; rather, resources are put toward the biggest challenges and most promising solutions. This overall graded approach is a proven road to success. The analysis includes topics such as nanotube technology, deployment scenario, power beaming technology, ground-based hardware and operations, ribbon maintenance and repair and climber technology.

  16. Collection of Lanthanides and Actinides from Natural Waters with Conventional and Nanoporous Sorbents

    SciTech Connect

    Johnson, Bryce E.; Santschi, Peter H.; Chuang, Chia-Ying; Otosaka, Shigeyoshi; Addleman, Raymond S.; Douglas, Matthew; Rutledge, Ryan D.; Chouyyok, Wilaiwan; Davidson, Joseph D.; Fryxell, Glen E.; Schwantes, Jon M.

    2012-10-16

    Effective collection of trace-level lanthanides and actinides is advantageous for recovery and recycling of valuable resources, environmental remediation, chemical separations and in-situ monitoring. Using isotopic tracers, we have evaluated a number of conventional and nanoporous sorbent materials for their ability to capture and remove selected lanthanides (Ce and Eu) and actinides (Th, Pa, U, and Np) from fresh and salt water systems. In general, the nanostructured materials demonstrated a higher level of performance and consistency. Nanoporous silica surface modified with 3,4- hydroxypyridinone provided excellent collection and consistency in both river water and seawater. The MnO2 materials, particular the high surface area small particle material also demonstrated good performance. Other conventional sorbents typically performed at the levels below the nanostructured sorbents and demonstrate a larger variability and matrix dependency.

  17. Collection of lanthanides and actinides from natural waters with conventional and nanoporous sorbents.

    PubMed

    Johnson, Bryce E; Santschi, Peter H; Chuang, Chia-Ying; Otosaka, Shigeyoshi; Addleman, Raymond Shane; Douglas, Matt; Rutledge, Ryan D; Chouyyok, Wilaiwan; Davidson, Joseph D; Fryxell, Glen E; Schwantes, Jon M

    2012-10-16

    Effective collection of trace-level lanthanides and actinides is advantageous for recovery and recycling of valuable resources, environmental remediation, chemical separations, and in situ monitoring. Using isotopic tracers, we have evaluated a number of conventional and nanoporous sorbent materials for their ability to capture and remove selected lanthanides (Ce and Eu) and actinides (Th, Pa, U, and Np) from fresh and salt water systems. In general, the nanostructured materials demonstrated a higher level of performance and consistency. Nanoporous silica surface modified with 3,4-hydroxypyridinone provided excellent collection and consistency in both river water and seawater. The MnO(2) materials, in particular the high surface area small particle material, also demonstrated good performance. Other conventional sorbents typically performed at levels below the nanostructured sorbents and demonstrate a larger variability and matrix dependency.

  18. A many-body potential approach to modelling the thermomechanical properties of actinide oxides.

    PubMed

    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.

  19. RELATIVISTIC EFFECTS ON THE EQUATION OF STATE OF THE LIGHT ACTINIDES

    SciTech Connect

    Landa, A; Soderlind, P

    2005-11-04

    The effect of the relativistic spin-orbit (SO) interaction on the bonding in the early actinides has been investigated by means of electronic-structure calculations. Specifically, the equation of state (EOS) for the face-centered cubic (fcc) model systems of these metals have been calculated from the first-principles density-functional theory (DFT). Traditionally, the SO interaction in electronic-structure methods is implemented as a perturbation to the Hamiltonian that is solved for basis functions that explicitly do not depend on SO coupling. Here this approximation is shown to compare well with the fully relativistic Dirac treatment. It is further shown that SO coupling has a gradually increasing effect on the EOS as one proceeds through the actinides and the effect is diminished as density increases.

  20. Occlusion and ion exchange in the molten (lithium chloride + potassium chloride + alkaline earth chloride) salt + zeolite 4A system with alkaline earth chlorides of calcium and strontium, and in the molten (lithium chloride + potassium chloride + actinide chloride) salt + zeolite 4A system with the actinide chloride of uranium.

    SciTech Connect

    Lexa, D.; Chemical Engineering

    2003-04-01

    The interaction between molten salts of the type LiCl-KCl-MeCl n (Me=Ca, Sr, U; x{sub MeCLn} $$ = to 0.45; and x {sub KCl}/x LiCl=0.69) and zeolite 4A have been studied at 823 K. The main interactions between these salts and zeolite are molten salt occlusion to form salt-loaded zeolite and ion exchange between the molten salt and salt-loaded zeolite. An irreversible chemical reaction has been observed in the LiCl-KCl-UCl{sup 3+}zeolite system. The extent of occlusion is a function of the concentration of MeCl n in the zeolite and is equal to 10{+-}1 Cl- per zeolite unit cell, (AlSiO{sub 4}){sub 12}, at infinite MeCl n dilution. The ion-exchange mole-fraction equilibrium constants (separation factors) with respect to Li are decreasing functions of the concentration of SrCl{sub 2} and UCl{sub 3}, but an increasing function of the concentration of CaCl{sub 2} in the zeolite. At infinite MeCl n dilution, they are equal to 0.9, 11.9, and 13 for CaCl{sub 2}, SrCl{sub 2}, and UCl{sub 3}, respectively. The standard ion-exchange chemical potentials are equal to -50.0, -84, and -101.1 kJ x mol-1 for Ca{sup 2+}, Sr{sup 2+}, and U{sup 3+}, respectively.

  1. Actinide targets for the synthesis of super-heavy elements

    DOE PAGES

    Roberto, J.; Alexander, Charles W.; Boll, Rose Ann; Ezold, Julie G.; Felker, Leslie Kevin; Rykaczewski, Krzysztof Piotr; Hogle, Susan L.

    2015-06-18

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing themore » production of rare actinides including 249Bk, 251Cf, and 254Es are described.« less

  2. Actinide targets for the synthesis of super-heavy elements

    SciTech Connect

    Roberto, J.; Alexander, Charles W.; Boll, Rose Ann; Ezold, Julie G.; Felker, Leslie Kevin; Rykaczewski, Krzysztof Piotr; Hogle, Susan L.

    2015-06-18

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing the production of rare actinides including 249Bk, 251Cf, and 254Es are described.

  3. Separation of Minor Actinides from Lanthanides by Dithiophosphinic Acid Extractants

    SciTech Connect

    D. R. Peterman; M. R. Greenhalgh; R. D. Tillotson; J. R. Klaehn; M. K. Harrup; T. A. Luther; J. D. Law; L. M. Daniels

    2008-09-01

    The selective extraction of the minor actinides (Am(III) and Cm(III)) from the lanthanides is an important part of advanced reprocessing of spent nuclear fuel. This separation would allow the Am/Cm to be fabricated into targets and recycled to a reactor and the lanthanides to be dispositioned. This separation is difficult to accomplish due to the similarities in the chemical properties of the trivalent actinides and lanthanides. Research efforts at the Idaho National Laboratory have identified an innovative synthetic pathway yielding new regiospecific dithiophosphinic acid (DPAH) extractants. The synthesis provides DPAH derivatives that can address the issues concerning minor actinide separation and extractant stability. For this work, two new symmetric DPAH extractants have been prepared. The use of these extractants for the separation of minor actinides from lanthanides will be discussed.

  4. Actinide targets for the synthesis of super-heavy elements

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

    Since 2000, six new super-heavy elements with atomic numbers 113 through 118 have been synthesized in hot fusion reactions of 48Ca beams on actinide targets. These target materials, including 242Pu, 244Pu, 243Am, 245Cm, 248Cm, 249Cf, and 249Bk, are available in very limited quantities and require specialized production and processing facilities resident in only a few research centers worldwide. This report describes the production and chemical processing of heavy actinide materials for super-heavy element research, current availabilities of these materials, and related target fabrication techniques. The impact of actinide materials in super-heavy element discovery is reviewed, and strategies for enhancing the production of rare actinides including 249Bk, 251Cf, and 254Es are described.

  5. Influence of microorganisms on the oxidation state distribution of multivalent actinides under anoxic conditions

    SciTech Connect

    Reed, Donald Timothy; Borkowski, Marian; Lucchini, Jean - Francois; Ams, David; Richmann, M. K.; Khaing, H.; Swanson, J. S.

    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.

  6. Environmental impact of a teratogenic actinide: a case study of americium-241

    SciTech Connect

    Wang, J.; Yang, J.Y.

    1985-10-16

    Americium-241 is widely used as a radiation source, but it also has some potential risk if taken into the body. Although the radiotoxicity of americium-241 is small compared to other transuranic actinides, its effects on the reproductive system and on development of the placenta are more damaging than the effects of plutonium-239. A previous report based on a worst-case scenario involving a hypothetical fire accident in a contaminated facility indicated that there could have been a significant impact on nearby residents from a unit release of americium-241 via atmospheric dispersion. However, because the facility is located in a rural region where most drinking water supplies are drawn from private wells, it is believed that deposition of americium-241 from the atmosphere might also have impacts via the groundwater pathway by infiltration of rainwater. In this analysis, a three-dimensional analytical mathematical model is used to assess several aspects of americium-241 contamination of groundwater, including radioactive transformation, advection, dispersion, and soil sorption. Simulation results indicate that no significant radiological impacts would occur to the nearby residents via the groundwater pathway. 15 refs., 2 figs., 2 tabs.

  7. Enhancing BWR proliferation resistance fuel with minor actinides

    NASA Astrophysics Data System (ADS)

    Chang, Gray S.

    2009-03-01

    To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced light water reactor- LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides ( 237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu/Pu. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO 2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate-term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm 3) to the top (0.35 g/cm 3) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. The concept of MARA, which involves the use of transuranic nuclides ( 237Np and/or 241Am), significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in

  8. Weld analysis and control system

    NASA Technical Reports Server (NTRS)

    Kennedy, Larry Z. (Inventor); Rodgers, Michael H. (Inventor); Powell, Bradley W. (Inventor); Burroughs, Ivan A. (Inventor); Goode, K. Wayne (Inventor)

    1994-01-01

    The invention is a Weld Analysis and Control System developed for active weld system control through real time weld data acquisition. Closed-loop control is based on analysis of weld system parameters and weld geometry. The system is adapted for use with automated welding apparatus having a weld controller which is capable of active electronic control of all aspects of a welding operation. Enhanced graphics and data displays are provided for post-weld analysis. The system provides parameter acquisition, including seam location which is acquired for active torch cross-seam positioning. Torch stand-off is also monitored for control. Weld bead and parent surface geometrical parameters are acquired as an indication of weld quality. These parameters include mismatch, peaking, undercut, underfill, crown height, weld width, puddle diameter, and other measurable information about the weld puddle regions, such as puddle symmetry, etc. These parameters provide a basis for active control as well as post-weld quality analysis and verification. Weld system parameters, such as voltage, current and wire feed rate, are also monitored and archived for correlation with quality parameters.

  9. Method for adding additional isotopes to actinide-only burnup credit

    SciTech Connect

    Lancaster, D.B.; Fuentes, E.; Kang, C.

    1998-01-01

    The Topical Report on Actinide-Only Burnup Credit for Pressurized Water Reactor Spent Nuclear Fuel Packages requires computer code validation to be performed against a benchmark set of chemical assays for isotopic concentration and against a benchmark set of critical experiments for package criticality. Both sets contain all the isotopes included in the methodology. The chemical assays used include the uranium and plutonium isotopes, while the critical experiments were composed of UO{sub 2} or MOX rods, covering the isotopes in the actinide only approach. Since other isotopes are not included in the validation benchmark sets, it would be necessary to justify both the content and worth of any additional isotope for which burnup credit is to be taken (i.e., both the concentration and criticality effect of each particular isotope must be validated). A method is proposed here that can be used for any number of additional isotopes. As does the actinide-only burnup credit methodology, this method makes use of chemical assay data to establish the conservatism in the prediction of each isotope`s concentration. Criticality validation is also performed using a benchmark set of UO{sub 2} and MOX critical experiments, where the additional isotopes are validated using worth experiments to conservatively account for any uncertainty in their cross sections. The remaining requirements (analysis and modeling parameters, loading criteria generation, and physical implementation and controls) are performed exactly as described in the actinide-only burnup credit methodology. This report provides insight into each particular requirement in the new methodology.

  10. Comparative studies of actinide and sub-actinide fission cross section calculation from MCNP6 and TALYS

    SciTech Connect

    Perkasa, Y. S.; Waris, A. Kurniadi, R. Su'ud, Z.

    2014-09-30

    Comparative studies of actinide and sub-actinide fission cross section calculation from MCNP6 and TALYS have been conducted. In this work, fission cross section resulted from MCNP6 prediction will be compared with result from TALYS calculation. MCNP6 with its event generator CEM03.03 and LAQGSM03.03 have been validated and verified for several intermediate and heavy nuclides fission reaction data and also has a good agreement with experimental data for fission reaction that induced by photons, pions, and nucleons at energy from several ten of MeV to about 1 TeV. The calculation that induced within TALYS will be focused mainly to several hundred MeV for actinide and sub-actinide nuclides and will be compared with MCNP6 code and several experimental data from other evaluator.

  11. High-resolution X-ray absorption spectroscopy as a probe of crystal-field and covalency effects in actinide compounds.

    PubMed

    Butorin, Sergei M; Kvashnina, Kristina O; Vegelius, Johan R; Meyer, Daniel; Shuh, David K

    2016-07-19

    Applying the high-energy resolution fluorescence-detection (HERFD) mode of X-ray absorption spectroscopy (XAS), we were able to probe, for the first time to our knowledge, the crystalline electric field (CEF) splittings of the [Formula: see text] shell directly in the HERFD-XAS spectra of actinides. Using ThO2 as an example, data measured at the Th 3d edge were interpreted within the framework of the Anderson impurity model. Because the charge-transfer satellites were also resolved in the HERFD-XAS spectra, the analysis of these satellites revealed that ThO2 is not an ionic compound as previously believed. The Th [Formula: see text] occupancy in the ground state was estimated to be twice that of the Th [Formula: see text] states. We demonstrate that HERFD-XAS allows for characterization of the CEF interaction and degree of covalency in the ground state of actinide compounds as it is extensively done for 3d transition metal systems. PMID:27370799

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

    SciTech Connect

    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 this

  13. Selective Media for Actinide Collection and Pre-Concentration: Results of FY 2006 Studies

    SciTech Connect

    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

    3] > 0.3 M. Preliminary results suggest that the Kl?ui resins can separate Pu(IV) from sample solutions containing high concentrations of competing ions. Conceptual protocols for recovery of the Pu from the resin for subsequent analysis have been proposed, but further work is needed to perfect these techniques. Work on this subject will be continued in FY 2007. Automated laboratory equipment (in conjunction with Task 3 of the NA-22 Automation Project) will be used in FY 2007 to improve the efficiency of these experiments. The sorption of actinide ions on self-assembled monolayer on mesoporous supports materials containing diphosphonate groups was also investigated. These materials also showed a very high affinity for tetravalent actinides, and they also sorbed U(VI) fairly strongly. Computational Ligand Design An extended MM3 molecular mechanics model was developed for calculating the structures of Kl?ui ligand complexes. This laid the groundwork necessary to perform the computer-aided design of bis-Kl?ui architectures tailored for Pu(IV) complexation. Calculated structures of the Kl?ui ligand complexes [Pu(Kl?ui)2(OH2)2]2+ and [Fe(Kl?ui)2]+ indicate a ''bent'' sandwich arrangement of the Kl?ui ligands in the Pu(IV) complex, whereas the Fe(III) complex prefers a ''linear'' octahedral arrangement of the two Kl?ui ligands. This offers the possibility that two Kl?ui ligands can be tethered together to form a material with very high binding affinity for Pu(IV) over Fe(III). The next step in the design process is to use de novo molecule building software (HostDesigner) to identify potential candidate architectures.

  14. Skull counting in late stages after internal contamination by actinides.

    PubMed

    Tani, Kotaro; Shutt, Arron; Kurihara, Osamu; Kosako, Toshiso

    2015-02-01

    Monitoring preparation for internal contamination with actinides (e.g. Pu and Am) is required to assess internal doses at nuclear fuel cycle-related facilities. In this paper, the authors focus on skull counting in case of single-incident inhalation of (241)Am and propose an effective procedure for skull counting with an existing system, taking into account the biokinetic behaviour of (241)Am in the human body. The predicted response of the system to skull counting under a certain counting geometry was found to be only ∼1.0 × 10(-5) cps Bq(-1) 1y after intake. However, this disadvantage could be remedied by repeated measurements of the skull during the late stage of the intake due to the predicted response reaching a plateau at about the 1000th day after exposure and exceeding that in the lung counting. Further studies are needed for the development of a new detection system with higher sensitivity to perform reliable internal dose estimations based on direct measurements.

  15. Automated Loads Analysis System (ATLAS)

    NASA Technical Reports Server (NTRS)

    Gardner, Stephen; Frere, Scot; O’Reilly, Patrick

    2013-01-01

    ATLAS is a generalized solution that can be used for launch vehicles. ATLAS is used to produce modal transient analysis and quasi-static analysis results (i.e., accelerations, displacements, and forces) for the payload math models on a specific Shuttle Transport System (STS) flight using the shuttle math model and associated forcing functions. This innovation solves the problem of coupling of payload math models into a shuttle math model. It performs a transient loads analysis simulating liftoff, landing, and all flight events between liftoff and landing. ATLAS utilizes efficient and numerically stable algorithms available in MSC/NASTRAN.

  16. Trivalent Lanthanide/Actinide Separation Using Aqueous-Modified TALSPEAK Chemistry

    SciTech Connect

    Travis S. Grimes; Richard D. Tillotson; Leigh R. Martin

    2014-05-01

    TALSPEAK is a liquid/liquid extraction process designed to separate trivalent lanthanides (Ln3+) from minor actinides (MAs) Am3+ and Cm3+. Traditional TALSPEAK organic phase is comprised of a monoacidic dialkyl bis(2-ethylhexyl)phosphoric acid extractant (HDEHP) in diisopropyl benzene (DIPB). The aqueous phase contains a soluble aminopolycarboxylate diethylenetriamine-N,N,N’,N”,N”-pentaacetic acid (DTPA) in a concentrated (1.0-2.0 M) lactic acid (HL) buffer with the aqueous acidity typically adjusted to pH 3.0. TALSPEAK balances the selective complexation of the actinides by DTPA against the electrostatic attraction of the lanthanides by the HDEHP extractant to achieve the desired trivalent lanthanide/actinide group separation. Although TALSPEAK is considered a successful separations scheme, recent fundamental studies have highlighted complex chemical interactions occurring in the aqueous and organic phases during the extraction process. Previous attempts to model the system have shown thermodynamic models do not accurately predict the observed extraction trends in the p[H+] range 2.5-4.8. In this study, the aqueous phase is modified by replacing the lactic acid buffer with a variety of simple and longer-chain amino acid buffers. The results show successful trivalent lanthanide/actinide group separation with the aqueous-modified TALSPEAK process at pH 2. The amino acid buffer concentrations were reduced to 0.5 M (at pH 2) and separations were performed without any effect on phase transfer kinetics. Successful modeling of the aqueous-modified TALSPEAK process (p[H+] 1.6-3.1) using a simplified thermodynamic model and an internally consistent set of thermodynamic data is presented.

  17. Polarization analysis of optical systems

    NASA Technical Reports Server (NTRS)

    Chipman, Russell A.

    1989-01-01

    For most optical systems it is typically assumed that the transmitted wavefront has uniform (or Gaussian) amplitude and constant polarization state. This is the default assumption of geometrical optics. This paper considers methods suitable for analyzing systems for which this assumption is not valid. Such methods of polarization analysis include polarization ray tracing and polarization aberration theory. Definitions of the basic classes of polarization phenomena and a review of the Jones calculus are included to form a basis for the discussion.

  18. Actinide production in the reaction of heavy ions with curium-248

    SciTech Connect

    Moody, K.J.

    1983-01-01

    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/Kr and /sup 86/O, /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. A preliminary, unsuccessful attempt to isolate /sup 247/Pu is outlined. The absolute ..gamma.. ray intensities from /sup 251/Bk decay, necessary for calculating the /sup 251/Bk cross section, are also determined.

  19. AECL/US INERI - Development of Inert Matrix Fuels for Plutonium and Minor Actinide Management in Power Reactors -- Fuel Requirements and Down-Select Report

    SciTech Connect

    William Carmack; Randy D. Lee; Pavel Medvedev; Mitch Meyer; Michael Todosow; Holly B. Hamilton; Juan Nino; Simon Philpot; James Tulenko

    2005-06-01

    The U.S. Advanced Fuel Cycle Program and the Atomic Energy Canada Ltd (AECL) seek to develop and demonstrate the technologies needed to minimize the overall Pu and minor actinides present in the light water reactor (LWR) nuclear fuel cycles. It is proposed to reuse the Pu from LWR spent fuel both for the energy it contains and to decrease the hazard and proliferation impact resulting from storage of the Pu and minor actinides. The use of fuel compositions with a combination of U and Pu oxide (MOX) has been proposed as a way to recycle Pu and/or minor actinides in LWRs. It has also been proposed to replace the fertile U{sup 238} matrix of MOX with a fertile-free matrix (IMF) to reduce the production of Pu{sup 239} in the fuel system. It is important to demonstrate the performance of these fuels with the appropriate mixture of isotopes and determine what impact there might be from trace elements or contaminants. Previous work has already been done to look at weapons-grade (WG) Pu in the MOX configuration [1][2] and the reactor-grade (RG) Pu in a MOX configuration including small (4000 ppm additions of Neptunium). This program will add to the existing database by developing a wide variety of MOX fuel compositions along with new fuel compositions called inert-matrix fuel (IMF). The goal of this program is to determine the general fabrication and irradiation behavior of the proposed IMF fuel compositions. Successful performance of these compositions will lead to further selection and development of IMF for use in LWRs. This experiment will also test various inert matrix material compositions with and without quantities of the minor actinides Americium and Neptunium to determine feasibility of incorporation into the fuel matrices for destruction. There is interest in the U.S. and world-wide in the investigation of IMF (inert matrix fuels) for scenarios involving stabilization or burn down of plutonium in the fleet of existing commercial power reactors. IMF offer the

  20. The technical and economic impact of minor actinide transmutation in a sodium fast reactor

    SciTech Connect

    Gautier, G. M.; Morin, F.; Dechelette, F.; Sanseigne, E.; Chabert, C.

    2012-07-01

    Within the frame work of the French National Act of June 28, 2006 pertaining to the management of high activity, long-lived radioactive waste, one of the proposed processes consists in transmuting the Minor Actinides (MA) in the radial blankets of a Sodium Fast Reactor (SFR). With this option, we may assess the additional cost of the reactor by comparing two SFR designs, one with no Minor Actinides, and the other involving their transmutation. To perform this exercise, we define a reference design called SFRref, of 1500 MWe that is considered to be representative of the Reactor System. The SFRref mainly features a pool architecture with three pumps, six loops with one steam generator per loop. The reference core is the V2B core that was defined by the CEA a few years ago for the Reactor System. This architecture is designed to meet current safety requirements. In the case of transmutation, for this exercise we consider that the fertile blanket is replaced by two rows of assemblies having either 20% of Minor Actinides or 20% of Americium. The assessment work is performed in two phases. - The first consists in identifying and quantifying the technical differences between the two designs: the reference design without Minor Actinides and the design with Minor Actinides. The main differences are located in the reactor vessel, in the fuel handling system and in the intermediate storage area for spent fuel. An assessment of the availability is also performed so that the impact of the transmutation can be known. - The second consists in making an economic appraisal of the two designs. This work is performed using the CEA's SEMER code. The economic results are shown in relative values. For a transmutation of 20% of MA in the assemblies (S/As) and a hypothesis of 4 kW allowable for the washing device, there is a large external storage demanding a very long cooling time of the S/As. In this case, the economic impact may reach 5% on the capital part of the Levelized Unit

  1. Systems analysis - independent analysis and verification

    SciTech Connect

    DiPietro, J.P.; Skolnik, E.G.; Badin, J.S.

    1996-10-01

    The Hydrogen Program of the U.S. Department of Energy (DOE) funds a portfolio of activities ranging from conceptual research to pilot plant testing. The long-term research projects support DOE`s goal of a sustainable, domestically based energy system, and the development activities are focused on hydrogen-based energy systems that can be commercially viable in the near-term. Energetics develops analytic products that enable the Hydrogen Program Manager to assess the potential for near- and long-term R&D activities to satisfy DOE and energy market criteria. This work is based on a pathway analysis methodology. The authors consider an energy component (e.g., hydrogen production from biomass gasification, hybrid hydrogen internal combustion engine (ICE) vehicle) within a complete energy system. The work involves close interaction with the principal investigators to ensure accurate representation of the component technology. Comparisons are made with the current cost and performance of fossil-based and alternative renewable energy systems, and sensitivity analyses are conducted to determine the effect of changes in cost and performance parameters on the projects` viability.

  2. Reactions of actinide ions with ethylene oxide.

    PubMed

    Gibson, J K

    2001-03-01

    Naked and oxo-ligated actinide (An) monopositive ions were reacted with ethylene oxide, cyclo-C(2)H(4)O (EtO). Along with An = U, Np, Pu and Am, ions of two lanthanide (Ln) elements, Ln = Tb and Tm, were studied for comparison. Metal and metal oxide ions, M(+), MO(+) and MO(2)(+), were generated by laser ablation and immediately reacted with EtO. Unreacted and product ions were detected by time-of-flight mass spectrometry. It was apparent that the overall reaction cross-sections decreased in the order U(+) > or = Np(+) > Pu(+) > Am(+). A primary reaction channel for each studied metal was the formation of MO(+) from M(+), in accord with the expected exothermicity of oxygen abstraction from EtO. For U, Np and Pu, the dioxides were also major products, indicating OAn(+)--O dissociation energies of at least 350 kJ mol(-1), the energy required for O-atom abstraction from EtO. For Am, Tb and Tm, the dioxides were only very minor products, reflecting the stabilities of the trivalent states and resistance to oxidation to higher valence states; the structures/bonding in these MO(2)(+) are intriguing given that the formal pentavalent bonding state is effectively unattainable. It was demonstrated that EtO, unlike more thermochemically favorable but kinetically restricted O-donors, is effective at achieving facile oxidation of actinide metal ions to the monoxide, and to the dioxide if the second O-abstraction reaction is exothermic. Several intriguing minor products were also identified, most of which incorporate metal--oxygen bonding and are attributed to the oxophilicity of the f-block elements; the contrast to the behavior of first-row d-block transition elements is striking in this regard. Particularly noteworthy was the formation of MH(4)(+) (and MOH(4)(+)), evidently via abstraction of all four H atoms from a single C(2)H(4)O molecule; the structures/bonding in these novel 'hydride' species are indeterminate and warrant further attention.

  3. An Assessment of Spent Fuel Reprocessing for Actinide Destruction and Resource Sustainability.

    SciTech Connect

    Cipiti, Benjamin B.; Smith, James D.

    2008-09-01

    The reprocessing and recycling of spent nuclear fuel can benefit the nuclear fuel cycle by destroying actinides or extending fissionable resources if uranium supplies become limited. The purpose of this study was to assess reprocessing and recycling in both fast and thermal reactors to determine the effectiveness for actinide destruction and resource utilization. Fast reactor recycling will reduce both the mass and heat load of actinides by a factor of 2, but only after 3 recycles and many decades. Thermal reactor recycling is similarly effective for reducing actinide mass, but the heat load will increase by a factor of 2. Economically recoverable reserves of uranium are estimated to sustain the current global fleet for the next 100 years, and undiscovered reserves and lower quality ores are estimated to contain twice the amount of economically recoverable reserves--which delays the concern of resource utilization for many decades. Economic analysis reveals that reprocessed plutonium will become competitive only when uranium prices rise to about %24360 per kg. Alternative uranium sources are estimated to be competitive well below that price. Decisions regarding the development of a near term commercial-scale reprocessing fuel cycle must partially take into account the effectiveness of reactors for actnides destruction and the time scale for when uranium supplies may become limited. Long-term research and development is recommended in order to make more dramatic improvements in actinide destruction and cost reductions for advanced fuel cycle technologies.The original scope of this work was to optimize an advanced fuel cycle using a tool that couples a reprocessing plant simulation model with a depletion analysis code. Due to funding and time constraints of the late start LDRD process and a lack of support for follow-on work, the project focused instead on a comparison of different reprocessing and recycling options. This optimization study led to new insight into

  4. System Safety Common Cause Analysis

    1992-03-10

    The COMCAN fault tree analysis codes are designed to analyze complex systems such as nuclear plants for common causes of failure. A common cause event, or common mode failure, is a secondary cause that could contribute to the failure of more than one component and violates the assumption of independence. Analysis of such events is an integral part of system reliability and safety analysis. A significant common cause event is a secondary cause common tomore » all basic events in one or more minimal cut sets. Minimal cut sets containing events from components sharing a common location or a common link are called common cause candidates. Components share a common location if no barrier insulates any one of them from the secondary cause. A common link is a dependency among components which cannot be removed by a physical barrier (e.g.,a common energy source or common maintenance instructions).« less

  5. Prognostic Analysis System and Methods of Operation

    NASA Technical Reports Server (NTRS)

    MacKey, Ryan M. E. (Inventor); Sneddon, Robert (Inventor)

    2014-01-01

    A prognostic analysis system and methods of operating the system are provided. In particular, a prognostic analysis system for the analysis of physical system health applicable to mechanical, electrical, chemical and optical systems and methods of operating the system are described herein.

  6. Actinide ions for testing the spatial α -variation hypothesis

    NASA Astrophysics Data System (ADS)

    Dzuba, V. A.; Safronova, M. S.; Safronova, U. I.; Flambaum, V. V.

    2015-12-01

    Testing the spatial variation of the fine-structure constant α indicated by Webb et al. [J. K. Webb, J. A. King, M. T. Murphy, V. V. Flambaum, R. F. Carswell, and M. B. Bainbridge, Phys. Rev. Lett. 107, 191101 (2011), 10.1103/PhysRevLett.107.191101] with terrestrial laboratory atomic measurements requires at least α ˙/α ˜10-19yr-1 sensitivity. We conduct a systematic search of atomic systems for such a test that have all features of the best optical clock transitions leading to the possibility of the frequency measurements with fractional accuracy on the level of 10-18 or better and have a factor of 100 extra enhancement of α variation in comparison to experimental frequency ratio measurement accuracy. We identify the pair of actinide Cf15 + and Es16 + ions as the best system for a test of spatial α -variation hypothesis as it satisfies both of these requirements and has sufficiently simple electronic structure to allow for high-precision predictions of all atomic properties required for rapid experimental progress.

  7. Microfabricated integrated DNA analysis systems

    SciTech Connect

    Woolley, A.T.; Mathies, R.A.; Northrup, M.A.

    1996-12-31

    Microfabrication has the potential to revolutionize chemical analysis, from reactions to separations to molecular biotechnology. Microfabricated devices allow high speed separations, automated sample handling, and the study of reactions in the pl to {mu}l volume range. Our research has focused on microfabricated integrated DNA analysis systems (MIDAS). As a first step, we have demonstrated high-speed DNA restriction fragment sizing, and DNA sequencing on microfabricated capillary electrophoresis (CE) chips. We have recently coupled microfabricated PCR reactors and CE chips to make integrated DNA analysis devices. With these devices, rapid PCR can be performed and the reaction products immediately analyzed on the CE chip, eliminating the need for manual transfer of the amplified sample. PCR amplifications have been done in less than 16 minutes, followed by CE analysis in under 100 seconds. These PCR-CE chips represent an important step towards completely integrated sample manipulation on microfabricated devices.

  8. A traffic situation analysis system

    NASA Astrophysics Data System (ADS)

    Sidla, Oliver; Rosner, Marcin

    2011-01-01

    The observation and monitoring of traffic with smart visions systems for the purpose of improving traffic safety has a big potential. For example embedded vision systems built into vehicles can be used as early warning systems, or stationary camera systems can modify the switching frequency of signals at intersections. Today the automated analysis of traffic situations is still in its infancy - the patterns of vehicle motion and pedestrian flow in an urban environment are too complex to be fully understood by a vision system. We present steps towards such a traffic monitoring system which is designed to detect potentially dangerous traffic situations, especially incidents in which the interaction of pedestrians and vehicles might develop into safety critical encounters. The proposed system is field-tested at a real pedestrian crossing in the City of Vienna for the duration of one year. It consists of a cluster of 3 smart cameras, each of which is built from a very compact PC hardware system in an outdoor capable housing. Two cameras run vehicle detection software including license plate detection and recognition, one camera runs a complex pedestrian detection and tracking module based on the HOG detection principle. As a supplement, all 3 cameras use additional optical flow computation in a low-resolution video stream in order to estimate the motion path and speed of objects. This work describes the foundation for all 3 different object detection modalities (pedestrians, vehi1cles, license plates), and explains the system setup and its design.

  9. Marine systems analysis and modeling

    NASA Astrophysics Data System (ADS)

    Fedra, K.

    1995-03-01

    Oceanography and marine ecology have a considerable history in the use of computers for modeling both physical and ecological processes. With increasing stress on the marine environment due to human activities such as fisheries and numerous forms of pollution, the analysis of marine problems must increasingly and jointly consider physical, ecological and socio-economic aspects in a broader systems framework that transcends more traditional disciplinary boundaries. This often introduces difficult-to-quantify, “soft” elements, such as values and perceptions, into formal analysis. Thus, the problem domain combines a solid foundation in the physical sciences, with strong elements of ecological, socio-economic and political considerations. At the same time, the domain is also characterized by both a very large volume of some data, and an extremely datapoor situation for other variables, as well as a very high degree of uncertainty, partly due to the temporal and spatial heterogeneity of the marine environment. Consequently, marine systems analysis and management require tools that can integrate these diverse aspects into efficient information systems that can support research as well as planning and also policy- and decisionmaking processes. Supporting scientific research, as well as decision-making processes and the diverse groups and actors involved, requires better access and direct understanding of the information basis as well as easy-to-use, but powerful tools for analysis. Advanced information technology provides the tools to design and implement smart software where, in a broad sense, the emphasis is on the man-machine interface. Symbolic and analogous, graphical interaction, visual representation of problems, integrated data sources, and built-in domain knowledge can effectively support users of complex and complicated software systems. Integration, interaction, visualization and intelligence are key concepts that are discussed in detail, using an

  10. Synthesis of crystalline ceramics for actinide immobilisation

    SciTech Connect

    Burakov, B.; Gribova, V.; Kitsay, A.; Ojovan, M.; Hyatt, N.C.; Stennett, M.C.

    2007-07-01

    Methods for the synthesis of ceramic wasteforms for the immobilization of actinides are common to those for non-radioactive ceramics: hot uniaxial pressing (HUP); hot isostatic pressing (HIP); cold pressing followed by sintering; melting (for some specific ceramics, such as garnet/perovskite composites). Synthesis of ceramics doped with radionuclides is characterized with some important considerations: all the radionuclides should be incorporated into crystalline structure of durable host-phases in the form of solid solutions and no separate phases of radionuclides should be present in the matrix of final ceramic wasteform; all procedures of starting precursor preparation and ceramic synthesis should follow safety requirements of nuclear industry. Synthesis methods that avoid the use of very high temperatures and pressures and are easily accomplished within the environment of a glove-box or hot cell are preferable. Knowledge transfer between the V. G. Khlopin Radium Institute (KRI, Russia) and Immobilisation Science Laboratory (ISL, UK) was facilitated in the framework of a joint project supported by UK Royal Society. In order to introduce methods of precursor preparation and ceramic synthesis we selected well-known procedures readily deployable in radiochemical processing plants. We accounted that training should include main types of ceramic wasteforms which are currently discussed for industrial applications. (authors)

  11. Microbial transformations of actinides in the environment

    NASA Astrophysics Data System (ADS)

    Livens, F. R.; Al-Bokari, M.; Fomina, M.; Gadd, G. M.; Geissler, A.; Lloyd, J. R.; Renshaw, J. C.; Vaughan, D. J.

    2010-03-01

    The diversity of microorganisms is still far from understood, although many examples of the microbial biotransformation of stable, pollutant and radioactive elements, involving Bacteria, Archaea and Fungi, are known. In estuarine sediments from the Irish Sea basin, which have been labelled by low level effluent discharges, there is evidence of an annual cycle in Pu solubility, and microcosm experiments have demonstrated both shifts in the bacterial community and changes in Pu solubility as a result of changes in redox conditions. In the laboratory, redox transformation of both U and Pu by Geobacter sulfurreducens has been demonstrated and EXAFS spectroscopy has been used to understand the inability of G. sufurreducens to reduce Np(V). Fungi promote corrosion of metallic U alloy through production of a range of carboxylic acid metabolites, and are capable of translocating the dissolved U before precipitating it externally to the hyphae, as U(VI) phosphate phases. These examples illustrate the far-reaching but complex effects which microorganisms can have on actinide behaviour.

  12. Actinide Measurements by Accelerator Mass Spectrometry at Lawrence Livermore National Laboratory

    SciTech Connect

    Brown, T A; Marchetti, A A; Martinelli, R E; Cox, C C; Knezovich, J P; Hamilton, T F

    2003-09-25

    We report on the development of an accelerator mass spectrometry (AMS) system for the measurement of actinides at Lawrence Livermore National Laboratory. This AMS system is centered on a recently completed heavy isotope beam line that was designed particularly for high sensitivity, robust, high-throughput measurements of actinide concentrations and isotopic ratios. A fast isotope switching capability has been incorporated in the system, allowing flexibility in isotope selection and for the quasi-continuous normalization to a reference isotope spike. Initially, our utilization of the heavy isotope system has concentrated on the measurement of Pu isotopes. Under current operating conditions, background levels equivalent to {approx}1 x 10{sup 5} atoms are observed during routine {sup 239}Pu and {sup 240}Pu measurements. Measurements of samples containing {approx}10{sup 13} {sup 238}U atoms demonstrate that the system provides a {sup 238}U rejection factor during {sup 239}Pu measurements of {approx}10{sup 7}. Measurements of known materials, combined with results from an externally organized inter-comparison program, indicate that our {sup 239}Pu measurements are accurate and precise down to the {micro}Bq level ({approx}10{sup 6} atoms). Recently, we have investigated the performance of our heavy isotope AMS system in measurements of {sup 237}Np and {sup 236}U. Results of these investigations are discussed. The sensitivity shown by our Pu measurements, combined with the high throughput and interference rejection capabilities of our AMS system, demonstrate that AMS can provide a rapid and cost-effective measurement technique for actinides in a wide variety of studies.

  13. An Approach for Validating Actinide and Fission Product Burnup Credit Criticality Safety Analyses: Criticality (keff) Predictions

    DOE PAGES

    Scaglione, John M.; Mueller, Don E.; Wagner, John C.

    2014-12-01

    One of the most important remaining challenges associated with expanded implementation of burnup credit in the United States is the validation of depletion and criticality calculations used in the safety evaluation—in particular, the availability and use of applicable measured data to support validation, especially for fission products (FPs). Applicants and regulatory reviewers have been constrained by both a scarcity of data and a lack of clear technical basis or approach for use of the data. In this study, this paper describes a validation approach for commercial spent nuclear fuel (SNF) criticality safety (keff) evaluations based on best-available data and methodsmore » and applies the approach for representative SNF storage and transport configurations/conditions to demonstrate its usage and applicability, as well as to provide reference bias results. The criticality validation approach utilizes not only available laboratory critical experiment (LCE) data from the International Handbook of Evaluated Criticality Safety Benchmark Experiments and the French Haut Taux de Combustion program to support validation of the principal actinides but also calculated sensitivities, nuclear data uncertainties, and limited available FP LCE data to predict and verify individual biases for relevant minor actinides and FPs. The results demonstrate that (a) sufficient critical experiment data exist to adequately validate keff calculations via conventional validation approaches for the primary actinides, (b) sensitivity-based critical experiment selection is more appropriate for generating accurate application model bias and uncertainty, and (c) calculated sensitivities and nuclear data uncertainties can be used for generating conservative estimates of bias for minor actinides and FPs. Results based on the SCALE 6.1 and the ENDF/B-VII.0 cross-section libraries indicate that a conservative estimate of the bias for the minor actinides and FPs is 1.5% of their worth within the

  14. Launch vehicle systems design analysis

    NASA Technical Reports Server (NTRS)

    Ryan, Robert; Verderaime, V.

    1993-01-01

    Current launch vehicle design emphasis is on low life-cycle cost. This paper applies total quality management (TQM) principles to a conventional systems design analysis process to provide low-cost, high-reliability designs. Suggested TQM techniques include Steward's systems information flow matrix method, quality leverage principle, quality through robustness and function deployment, Pareto's principle, Pugh's selection and enhancement criteria, and other design process procedures. TQM quality performance at least-cost can be realized through competent concurrent engineering teams and brilliance of their technical leadership.

  15. Nuclear Dissipation via Peripheral Collisions with Relativistic Radioactive Actinides Beams

    SciTech Connect

    Schmitt, C.; Heinz, A.; Jurado, B.; Kelic, A.; Schmidt, K.-H.

    2007-05-22

    Peripheral collisions with radioactive actinide beams at relativistic energies are proposed as a relevant approach for the study of dissipation in nuclear matter. The characteristics of the systems resulting from the primary fragmentation of such beams are particularly well suited for probing the controversial existence of a sizeable delay in fission. Thanks to the radioactive beam facility at GSI an unusually large set of data involving about 60 secondary unstable projectiles between At and U has been collected under identical conditions. The properties of the set-up enabled the coincident measurement of the atomic number of both fission fragments, permitting a judicious classification of the data. The width of the fission-fragment charge distribution is shown to establish a thermometer at the saddle point which is directly related to the transient delay caused by the friction force. From a comparison with realistic model calculations, the dissipation strength at small deformation and the transient time are inferred. The present strategy is promoted as a complementary approach that avoids some complex problems inherent to conventional techniques. Combined to the paramount size of the data set, it sheds light on contradictory conclusions that have been published in the past. There is at this point no definite consensus on our understanding of the damping process in fission.

  16. New insights into formation of trivalent actinides complexes with DTPA.

    PubMed

    Leguay, Sébastien; Vercouter, Thomas; Topin, Sylvain; Aupiais, Jean; Guillaumont, Dominique; Miguirditchian, Manuel; Moisy, Philippe; Le Naour, Claire

    2012-12-01

    Complexation of trivalent actinides with DTPA (diethylenetriamine pentaacetic acid) was studied as a function of pcH and temperature in (Na,H)Cl medium of 0.1 M ionic strength. Formation constants of both complexes AnHDTPA(-) and AnDTPA(2-) (where An stands for Am, Cm, and Cf) were determined by TRLFS, CE-ICP-MS, spectrophotometry, and solvent extraction. The values of formation constants obtained from the different techniques are coherent and consistent with reinterpreted literature data, showing a higher stability of Cf complexes than Am and Cm complexes. The effect of temperature indicates that formation constants of protonated and nonprotonated complexes are exothermic with a high positive entropic contribution. DFT calculations were also performed on the An/DTPA system. Geometry optimizations were conducted on AnDTPA(2-) and AnHDTPA(-) considering all possible protonation sites. For both complexes, one and two water molecules in the first coordination sphere of curium were also considered. DFT calculations indicate that the lowest energy structures correspond to protonation on oxygen that is not involved in An-DTPA bonds and that the structures with two water molecules are not stable.

  17. Functionalization of mesoporous materials for lanthanide and actinide extraction.

    PubMed

    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. PMID:27240525

  18. Functionalization of mesoporous materials for lanthanide and actinide extraction.

    PubMed

    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.

  19. Thermodynamic and Structural Investigation of Synthetic Actinide-Peptide Scaffolds.

    PubMed

    Safi, Samir; Jeanson, Aurélie; Roques, Jérome; Solari, Pier Lorenzo; Charnay-Pouget, Florence; Den Auwer, Christophe; Creff, Gaëlle; Aitken, David J; Simoni, Eric

    2016-01-19

    The complexation of uranium and europium, in oxidation states +VI and +III, respectively, was investigated with pertinent bio-inorganic systems. Three aspartate-rich pentapeptides with different structural properties were selected for study to rationalize the structure-affinity relationships. Thermodynamic results, crosschecked by both isothermal titration calorimetry and time-resolved laser fluorescence spectroscopy, showed different affinity depending on the peptide for both Eu(III) and U(VI). The thermodynamic aspects were correlated to structural predictions, which were acquired by density functional theory quantum chemical calculations and from IR and extended X-ray absorption fine structure experiments. The combination of these microscopic properties revealed that carbonyl-metal interactions affected the entropy in the case of europium, while the larger uranyl cation was mostly affected by preorganization and steric effects, so that the affinity was enhanced through enthalpy. The approach described here revealed various microscopic aspects governing peptide actinide affinity. Highlighting these mechanisms should certainly contribute to the rational synthesis of higher affinity biomimetic aspartic ligands.

  20. Hydrothermal Methods as a New Way of Actinide Phosphate Preparation

    SciTech Connect

    Clavier, Nicolas; Wallez, Gilles; Quarton, Michel

    2007-07-01

    Precipitation processes driven in hydrothermal conditions were applied to the preparation of phosphate-based ceramics. In particular, three systems composed by a crystallized precursor linked with a high temperature compound were examined: M(OH)PO{sub 4} / M{sub 2}O(PO{sub 4}){sub 2} (M = Th, U), MPO{sub 4} 0.5 H{sub 2}O / MPO{sub 4} (M = La - Dy), and Th{sub 2-x/2}An{sub x/2}(PO{sub 4}){sub 2}(HPO{sub 4}) H{sub 2}O / {beta}-Th{sub 4-x}An{sub x}(PO{sub 4}){sub 4}P{sub 2}O{sub 7} (M = U, Np, Pu). A significant improvement of several physico-chemical properties of the powders, especially in the sintering capability and the homogeneity of the final solids, was evidenced when starting from the precursors. Furthermore, these phases were also found to control the solubility of lanthanides and actinides during leaching experiments when reaching the saturation conditions in the solution. (authors)

  1. System analysis of high performance MHD systems

    SciTech Connect

    Chang, S.L.; Berry, G.F.; Hu, N.

    1988-01-01

    This paper presents the results of an investigation on the upper ranges of performance that an MHD power plant using advanced technology assumptions might achieve and a parametric study on the key variables affecting this high performance. To simulate a high performance MHD power plant and conduct a parametric study, the Systems Analysis Language Translator (SALT) code developed at Argonne National Laboratory was used. The parametric study results indicate that the overall efficiency of an MHD power plant can be further increased subject to the improvement of some key variables such as, the MHD generator inverter efficiency, channel electrical loading factor, magnetic field strength, preheated air temperature, and combustor heat loss. In an optimization calculation, the simulated high performance MHD power plant using advanced technology assumptions can attain an ultra high overall efficiency, exceeding 62%. 12 refs., 5 figs., 4 tabs.

  2. Laboratory studies of actinide metal-silicate fractionation

    NASA Technical Reports Server (NTRS)

    Jones, J. H.; Burnett, D. S.

    1980-01-01

    Actinide and Sm partition coefficients between silicate melt and several metallic phases have been measured. Under reducing conditions Si, Th, U and Pu can be reduced to metals from silicate melts and alloyed with a platinum-gold alloy. U and Pu enter a molten Pt-Si alloy with roughly equal affinity but U strongly partitions into the solid Pt. Th behaves qualitatively the same as Pu but is much less readily reduced than U, and Sm appears to remain unreduced. Experiments with Fe metal have shown that the partition coefficients of the actinides between Fe and silicate liquid are extremely low, suggesting a very low actinide concentration in planetary cores. Experiments show that platinum metals can efficiently fractionate actinides and fractionate actinides from lanthanides and this process may be relevant to the condensation behavior of these elements from the solar nebula. Pt-metal grains in Allende Ca-Al-rich inclusions appear to be U-poor, although the sub-class of Zr-bearing Pt metals may have high U contents.

  3. Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides.

    PubMed

    Allred, Benjamin E; Rupert, Peter B; Gauny, Stacey S; An, Dahlia D; Ralston, Corie Y; Sturzbecher-Hoehne, Manuel; Strong, Roland K; Abergel, Rebecca J

    2015-08-18

    Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin-transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein-ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications.

  4. Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides

    PubMed Central

    Allred, Benjamin E.; Rupert, Peter B.; Gauny, Stacey S.; An, Dahlia D.; Ralston, Corie Y.; Sturzbecher-Hoehne, Manuel; Strong, Roland K.; Abergel, Rebecca J.

    2015-01-01

    Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin–transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein–ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications. PMID:26240330

  5. Siderocalin-mediated recognition, sensitization, and cellular uptake of actinides.

    PubMed

    Allred, Benjamin E; Rupert, Peter B; Gauny, Stacey S; An, Dahlia D; Ralston, Corie Y; Sturzbecher-Hoehne, Manuel; Strong, Roland K; Abergel, Rebecca J

    2015-08-18

    Synthetic radionuclides, such as the transuranic actinides plutonium, americium, and curium, present severe health threats as contaminants, and understanding the scope of the biochemical interactions involved in actinide transport is instrumental in managing human contamination. Here we show that siderocalin, a mammalian siderophore-binding protein from the lipocalin family, specifically binds lanthanide and actinide complexes through molecular recognition of the ligands chelating the metal ions. Using crystallography, we structurally characterized the resulting siderocalin-transuranic actinide complexes, providing unprecedented insights into the biological coordination of heavy radioelements. In controlled in vitro assays, we found that intracellular plutonium uptake can occur through siderocalin-mediated endocytosis. We also demonstrated that siderocalin can act as a synergistic antenna to sensitize the luminescence of trivalent lanthanide and actinide ions in ternary protein-ligand complexes, dramatically increasing the brightness and efficiency of intramolecular energy transfer processes that give rise to metal luminescence. Our results identify siderocalin as a potential player in the biological trafficking of f elements, but through a secondary ligand-based metal sequestration mechanism. Beyond elucidating contamination pathways, this work is a starting point for the design of two-stage biomimetic platforms for photoluminescence, separation, and transport applications. PMID:26240330

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

    NASA Astrophysics Data System (ADS)

    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.

  7. System for analysis of explosives

    DOEpatents

    Haas, Jeffrey S.

    2010-06-29

    A system for analysis of explosives. Samples are spotted on a thin layer chromatography plate. Multi-component explosives standards are spotted on the thin layer chromatography plate. The thin layer chromatography plate is dipped in a solvent mixture and chromatography is allowed to proceed. The thin layer chromatography plate is dipped in reagent 1. The thin layer chromatography plate is heated. The thin layer chromatography plate is dipped in reagent 2.

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

    PubMed

    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.

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

    PubMed

    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. PMID:26821345

  10. Dynamic Recovery in Silicate-Apatite Structures Under Irradiation and Implications for Long-Term Immobilization of Actinides

    SciTech Connect

    Weber, William J.; Zhang, Yanwen; Xiao, Haiyan Y.; Wang, Lumin M.

    2011-11-14

    The irradiation responses of Ca{sub 2}La{sub 8}(SiO{sub 4}){sub 6}O{sub 2} and Sr{sub 2}Nd{sub 8}(SiO{sub 4}){sub 6}O{sub 2} with the apatite structure are investigated to predict their long-term behaviour as host phases for immobilization of actinide elements from the nuclear fuel cycle. Different ions and energies are used to study the effects of dose, temperature, atomic displacement rate and ionization rate on irradiation-induced amorphization and recrystallization. The dose for amorphization increases with temperature in two stages, below and above 150 K. In the high temperature stage relevant to actinide immobilization, the increase of amorphization dose with temperature exhibits a strong dependence on the ratio of ionization rate to displacement rate for the different ions. Data analysis using a dynamic model for amorphization reveals that ionization-induced processes, with activation energy of 0.15 {+-} 0.02 eV, dominate dynamic recovery for ions from Ne through Xe. For heavier Au ions or for alpha-recoil nuclei emitted in alpha decay of actinides, ionization becomes less dominant and dynamic recovery is controlled primarily by thermally-driven processes. In post-irradiation annealing studies of amorphous samples, epitaxial thermal recrystallization is observed at 1123 K, and irradiation-enhanced nucleation of nanocrystallites is observed under irradiation with heavier ions. The recrystallization temperature under irradiation decreases with increasing ion mass to a value of {approx} 823 K, which also defines the thermally-driven critical temperature for amorphization under irradiation with heavy ions. Some partial recovery due to alpha particle irradiation at 300 K is observed that suggests a self-healing mechanism in apatite phases containing actinides. Based on the results and dynamic model, the temperature and time dependences of amorphization in silicate-apatite host phases for actinide immobilization are predicted.

  11. Dynamic recovery in silicate-apatite structures under irradiation and implications for long-term immobilization of actinides

    SciTech Connect

    Weber, William J; Zhang, Yanwen; Xiao, Haiyan; Wang, Prof. Lumin

    2012-01-01

    The irradiation responses of Ca2La8(SiO4)6O2 and Sr2Nd8(SiO4)6O2 with the apatite structure are investigated to predict their long-term behaviour as host phases for immobilization of actinide elements from the nuclear fuel cycle. Different ions and energies are used to study the effects of dose, temperature, atomic displacement rate and ionization rate on irradiation-induced amorphization and recrystallization. The dose for amorphization increases with temperature in two stages, below and above 150 K. In the high temperature stage relevant to actinide immobilization, the increase of amorphization dose with temperature exhibits a strong dependence on the ratio of ionization rate to displacement rate for the different ions. Data analysis using a dynamic model for amorphization reveals that ionization-induced processes, with activation energy of 0.15 0.02 eV, dominate dynamic recovery for ions from Ne through Xe. For heavier Au ions or for alpha-recoil nuclei emitted in alpha decay of actinides, ionization becomes less dominant and dynamic recovery is controlled primarily by thermally-driven processes. In post-irradiation annealing studies of amorphous samples, epitaxial thermal recrystallization is observed at 1123 K, and irradiation-enhanced nucleation of nanocrystallites is observed under irradiation with heavier ions. The recrystallization temperature under irradiation decreases with increasing ion mass to a value of ~ 823 K, which also defines the thermally-driven critical temperature for amorphization under irradiation with heavy ions. Some partial recovery due to alpha particle irradiation at 300 K is observed that suggests a self-healing mechanism in apatite phases containing actinides. Based on the results and dynamic model, the temperature and time dependences of amorphization in silicate-apatite host phases for actinide immobilization are predicted.

  12. The use of safeguards data for process monitoring in the Advanced Test Line for Actinide Separations

    SciTech Connect

    Barnes, J.W.; Yarbro, S.L.

    1987-01-01

    Los Alamos is constructing an integrated process monitoring/materials control and accounting (PM/MC and A) system in the Advanced Testing Line for Actinide Separations (ATLAS) at the Los Alamos Plutonium Facility. The ATLAS will test and demonstrate new methods for aqueous processing of plutonium. The ATLAS will also develop, test, and demonstrate the concepts for integrated process monitoring/materials control and accounting. We describe how this integrated PM/MC and A system will function and provide benefits to both process research and materials accounting personnel.

  13. Sigma Team for Minor Actinide Separation: PNNL FY 2011 Status Report

    SciTech Connect

    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.

  14. Film analysis systems and applications

    SciTech Connect

    Yonekura, Y.; Brill, A.B.

    1981-01-01

    The different components that can be used in modern film analysis systems are reviewed. TV camera and charge-coupled device sensors coupled to computers provide low cost systems for applications such as those described. The autoradiography (ARG) method provides an important tool for medical research and is especially useful for the development of new radiopharmaceutical compounds. Biodistribution information is needed for estimation of radiation dose, and for interpretation of the significance of observed patterns. The need for such precise information is heightened when one seeks to elucidate physiological principles/factors in normal and experimental models of disease. The poor spatial resolution achieved with current PET-imaging systems limits the information on radioreceptor mapping, neutrotransmitter, and neuroleptic drug distribution that can be achieved from patient studies. The artful use of ARG in carefully-controlled animal studies will be required to provide the additional information needed to fully understand results obtained with this new important research tool. (ERB)

  15. Prompt Fission Neutron Spectra of Actinides

    SciTech Connect

    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

  16. Modeling actinide chemistry with ASPEN PLUS

    SciTech Connect

    Grigsby, C.O.

    1995-12-31

    When chemical engineers think of chemical processing, they often do not include the US government or the national laboratories as significant participants. Compared to the scale of chemical processing in the chemical process, petrochemical and pharmaceutical industries, the government contribution to chemical processing is not large. However, for the past fifty years, the US government has been, heavily involved in chemical processing of some very specialized materials, in particular, uranium and plutonium for nuclear weapons. Individuals and corporations have paid taxes that, in part have been used to construct and to maintain a series of very expensive laboratories and production facilities throughout the country. Even ignoring the ongoing R & D costs, the price per pound of enriched uranium or of plutonium exceeds that of platinum by a wide margin. Now, with the end of the cold war, the government is decommissioning large numbers of nuclear weapons and cleaning up the legacy of radioactive wastes generated over the last fifty years. It is likely that the costs associated with the build-down and clean-up of the nuclear weapons complex will exceed the investment of the past fifty years of production. Los Alamos National Laboratory occupies a special place in the history of nuclear weapons. The first weapons were designed and assembled at Los Alamos using uranium produced in Oak Ridge, Tennessee or plutonium produced in Richland, Washington. Many of the thermophysical and metallurgical properties of actinide elements have been investigated at Los Alamos. The only plutonium processing facility currently operating in the US is in Los Alamos, and the Laboratory is striving to capture and maintain the uranium processing technology applicable to the post-cold war era. Laboratory researchers are actively involved in developing methods for cleaning up the wastes associated with production of nuclear weapons throughout the US.

  17. In pursuit of homoleptic actinide alkyl complexes.

    PubMed

    Seaman, Lani A; Walensky, Justin R; Wu, Guang; Hayton, Trevor W

    2013-04-01

    This Forum Article describes the pursuit of isolable homoleptic actinide alkyl complexes, starting with the pioneering work of Gilman during the Manhattan project. The initial reports in this area suggested that homoleptic uranium alkyls were too unstable to be isolated, but Wilkinson demonstrated that tractable uranium alkyls could be generated by purposeful "ate" complex formation, which serves to saturate the uranium coordination sphere and provide the complexes with greater kinetic stability. More recently, we reported the solid-state molecular structures of several homoleptic uranium alkyl complexes, including [Li(THF)4][U(CH2(t)Bu)5], [Li(TMEDA)]2[UMe6], [K(THF)]3[K(THF)2][U(CH2Ph)6]2, and [Li(THF)4][U(CH2SiMe3)6], by employing Wilkinson's strategy. Herein, we describe our attempts to extend this chemistry to thorium. The treatment of ThCl4(DME)2 with 5 equiv of LiCH2(t)Bu or LiCH2SiMe3 at -25 °C in THF affords [Th(CH2(t)Bu)5] (1) and [Li(DME)2][Th(CH2SiMe3)5 (2), respectively, in moderate yields. Similarly, the treatment of ThCl4(DME)2 with 6 equiv of K(CH2Ph) produces [K(THF)]2[Th(CH2Ph)6] (3), in good yield. Complexes 1-3 have been fully characterized, while the structures of 1 and 3 were confirmed by X-ray crystallography. Additionally, the electronic properties of 1 and 3 were explored by density functional theory.

  18. Computational Aeroacoustic Analysis System Development

    NASA Technical Reports Server (NTRS)

    Hadid, A.; Lin, W.; Ascoli, E.; Barson, S.; Sindir, M.

    2001-01-01

    Many industrial and commercial products operate in a dynamic flow environment and the aerodynamically generated noise has become a very important factor in the design of these products. In light of the importance in characterizing this dynamic environment, Rocketdyne has initiated a multiyear effort to develop an advanced general-purpose Computational Aeroacoustic Analysis System (CAAS) to address these issues. This system will provide a high fidelity predictive capability for aeroacoustic design and analysis. The numerical platform is able to provide high temporal and spatial accuracy that is required for aeroacoustic calculations through the development of a high order spectral element numerical algorithm. The analysis system is integrated with well-established CAE tools, such as a graphical user interface (GUI) through PATRAN, to provide cost-effective access to all of the necessary tools. These include preprocessing (geometry import, grid generation and boundary condition specification), code set up (problem specification, user parameter definition, etc.), and postprocessing. The purpose of the present paper is to assess the feasibility of such a system and to demonstrate the efficiency and accuracy of the numerical algorithm through numerical examples. Computations of vortex shedding noise were carried out in the context of a two-dimensional low Mach number turbulent flow past a square cylinder. The computational aeroacoustic approach that is used in CAAS relies on coupling a base flow solver to the acoustic solver throughout a computational cycle. The unsteady fluid motion, which is responsible for both the generation and propagation of acoustic waves, is calculated using a high order flow solver. The results of the flow field are then passed to the acoustic solver through an interpolator to map the field values into the acoustic grid. The acoustic field, which is governed by the linearized Euler equations, is then calculated using the flow results computed

  19. Actinide chemistry in Allende Ca-Al-rich inclusions

    NASA Technical Reports Server (NTRS)

    Murrell, M. T.; Burnett, D. S.

    1987-01-01

    Fission track radiography is used to investigate the U and Th microscale distribution in a set of Allende-meteorite Ca-Al-rich inclusions. In the Type B inclusions, the major phases melilite and fassaite are important actinide host phases, and on the rims of Type B inclusions and throughout all other inclusions studied, perovskite is the dominant actinide host phase. Results suggest that neither alteration nor loss or gain of an actinide-rich phase appears to have been an important Th/U fractionation mechanism, and that volatility differences may be the dominant factor. Th/U and rare earth element abundance patterns for the spinel and perovskite rim suggest rim formation by volatilization of interior material, and within the constraints of the brief time scale required for this heating, several mechanisms for spinel-perovskite rim formation are possible.

  20. Advancing the scientific basis of trivalent actinide-lanthanide separations

    SciTech Connect

    Nash, K.L.

    2013-07-01

    For advanced fuel cycles designed to support transmutation of transplutonium actinides, several options have been demonstrated for process-scale aqueous separations for U, Np, Pu management and for partitioning of trivalent actinides and fission product lanthanides away from other fission products. The more difficult mutual separation of Am/Cm from La-Tb remains the subject of considerable fundamental and applied research. The chemical separations literature teaches that the most productive alternatives to pursue are those based on ligand donor atoms less electronegative than O, specifically N- and S-containing complexants and chloride ion (Cl{sup -}). These 'soft-donor' atoms have exhibited usable selectivity in their bonding interactions with trivalent actinides relative to lanthanides. In this report, selected features of soft donor reagent design, characterization and application development will be discussed. The roles of thiocyanate, aminopoly-carboxylic acids and lactate in separation processes are detailed. (authors)

  1. Advances in actinide solid-state and coordination chemistry

    SciTech Connect

    Burns, Peter C; Ikeda, Y.; Czerwinski, K.

    2011-01-31

    Actinide solid-state and coordination chemistry has advanced through unexpected results that have further revealed the complex nature of the 5f elements. Nanoscale control of actinide materials is emerging, as shown by the creation of a considerable range of cluster and tubular topologies. Departures from established structural trends for actinyl ions are provided by cation-cation interactions in which an O atom of one actinyl ion is an equatorial ligand of a bipyramid of another actinyl ion. The solid-state structural complexity of actinide materials has been further demonstrated by open framework materials with interesting properties. The U(VI) tetraoxide core has been added to this cation's repertoire of coordination possibilities. The emergence of pentavalent uranium solid-state and coordination chemistry has resulted from the prudent selection of ligands. Finally, analogues of the uranyl ion have challenged our understanding of this normally unreactive functional group.

  2. Nuclear waste actinides as fissile fuel in hybrid blankets

    SciTech Connect

    Sahin, S.; Al-Kusayer, T.A.

    1983-12-01

    The widespread use of the present LWRs produces substantial quantities of nuclear waste materials. Among those, actinide nuclear waste poses a serious problem of stockage because the associated half life times for actinides is measured in terms of geological time periods (several millions of years) so that no waste disposal guarantee over such time intervals can be given, except for space disposal. On the other hand, these nuclear waste actinides are very good fissionable materials for high energetic (D,T) fusion neutrons. It is therefore worthwhile to investigate their quality as potential nuclear fuel in hybrid blankets. The present study investigates the neutronic performance of hybrid blankets containing Np/sup 237/ and Cm/sup 244/ as fissile materials. The isotopic composition of Americium has been adjusted to the spent fuel isotope composition of a LWR. The geometrical design has been made, according to the AYMAN fussion-fission (hybrid) experimental facility, now in the very early phase of planning.

  3. Crystal structure of actinide metals at high compression

    SciTech Connect

    Fast, L.; Soederlind, P.

    1995-08-01

    The crystal structures of some light actinide metals are studied theoretically as a function of applied pressure. The first principles electronic structure theory is formulated in the framework of density functional theory, with the gradient corrected local density approximation of the exchange-correlation functional. The light actinide metals are shown to be well described as itinerant (metallic) f-electron metals and generally, they display a crystal structure which have, in agreement with previous theoretical suggestions, increasing degree of symmetry and closed-packing upon compression. The theoretical calculations agree well with available experimental data. At very high compression, the theory predicts closed-packed structures such as the fcc or the hcp structures or the nearly closed-packed bcc structure for the light actinide metals. A simple canonical band picture is presented to explain in which particular closed-packed form these metals will crystallize at ultra-high pressure.

  4. Actinide Dioxides in Water: Interactions at the Interface

    SciTech Connect

    Alexandrov, Vitaly; Shvareva, Tatiana Y.; Hayun, Shmuel; Asta, Mark; Navrotsky, Alexandra

    2011-12-15

    A comprehensive understanding of chemical interactions between water and actinide dioxide surfaces is critical for safe operation and storage of nuclear fuels. Despite substantial previous research, understanding the nature of these interactions remains incomplete. In this work, we combine accurate calorimetric measurements with first-principles computational studies to characterize surface energies and adsorption enthalpies of water on two fluorite-structured compounds, ThO₂ and CeO₂, that are relevant for understanding the behavior of water on actinide oxide surfaces more generally. We determine coverage-dependent adsorption enthalpies and demonstrate a mixed molecular and dissociative structure for the first hydration layer. The results show a correlation between the magnitude of the anhydrous surface energy and the water adsorption enthalpy. Further, they suggest a structural model featuring one adsorbed water molecule per one surface cation on the most stable facet that is expected to be a common structural signature of water adsorbed on actinide dioxide compounds.

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

    SciTech Connect

    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.

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

    SciTech Connect

    G. S. Chang; Hongbin Zhang

    2009-09-01

    One approach to address the United States Nuclear Power (NP) 2010 program for the advanced light water reactor (LWR) (Gen-III+) intermediate-term spent fuel disposal need is to reduce spent fuel storage volume while enhancing proliferation resistance. One proposed solution includes increasing burnup of the discharged spent fuel and mixing minor actinide (MA) transuranic nuclides (237Np and 241Am) in the high burnup fuel. Thus, we can reduce the spent fuel volume while increasing the proliferation resistance by increasing the isotopic ratio of 238Pu/Pu. For future advanced nuclear systems, MAs are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. A typical boiling water reactor (BWR) fuel unit lattice cell model with UO2 fuel pins will be used to investigate the effectiveness of adding MAs (237Np and/or 241Am) to enhance proliferation resistance and improve fuel cycle performance for the intermediate-term goal of future nuclear energy systems. However, adding MAs will increase plutonium production in the discharged spent fuel. In this work, the Monte-Carlo coupling with ORIGEN-2.2 (MCWO) method was used to optimize the MA loading in the UO2 fuel such that the discharged spent fuel demonstrates enhanced proliferation resistance, while minimizing plutonium production. The axial averaged MA transmutation characteristics at different burnup were compared and their impact on neutronics criticality and the ratio of 238Pu/Pu discussed.

  7. Automation for System Safety Analysis

    NASA Technical Reports Server (NTRS)

    Malin, Jane T.; Fleming, Land; Throop, David; Thronesbery, Carroll; Flores, Joshua; Bennett, Ted; Wennberg, Paul

    2009-01-01

    This presentation describes work to integrate a set of tools to support early model-based analysis of failures and hazards due to system-software interactions. The tools perform and assist analysts in the following tasks: 1) extract model parts from text for architecture and safety/hazard models; 2) combine the parts with library information to develop the models for visualization and analysis; 3) perform graph analysis and simulation to identify and evaluate possible paths from hazard sources to vulnerable entities and functions, in nominal and anomalous system-software configurations and scenarios; and 4) identify resulting candidate scenarios for software integration testing. There has been significant technical progress in model extraction from Orion program text sources, architecture model derivation (components and connections) and documentation of extraction sources. Models have been derived from Internal Interface Requirements Documents (IIRDs) and FMEA documents. Linguistic text processing is used to extract model parts and relationships, and the Aerospace Ontology also aids automated model development from the extracted information. Visualizations of these models assist analysts in requirements overview and in checking consistency and completeness.

  8. Selection of actinide chemical analogues for WIPP tests

    SciTech Connect

    Villarreal, R.; Spall, D.

    1995-07-05

    The Department of Energy must demonstrate the effectiveness of the Waste Isolation Pilot Plant (WIPP) as a permanent repository for the disposal of transuranic (TRU) waste. Performance assessments of the WIPP require that estimates of the transportability and outcome of the radionuclides (actinides) be determined from disposal rooms that may become either partially or completely filled with brine. Federal regulations limit the amount of radioactivity that may be unintentionally released to the accessible environment by any mechanism during the post closure phase up to 10,000 years. Thermodynamic models have been developed to predict the concentrations of actinides in the WIPP disposal rooms under various situations and chemical conditions. These models are based on empirical and theoretical projections of the chemistry that might be present in and around the disposal room zone for both near and long-term periods. The actinides that are known to be present in the TRU wastes (and are included in the model) are Th, U, Np, Pu, and Am. Knowledge of the chemistry that might occur in the disposal rooms when the waste comes in contact with brine is important in understanding the range of oxidation states that might be present under different conditions. There is a need to establish the mechanisms and resultant rate of transport, migration, or effective retardation of actinides beyond the disposal rooms to the boundary of the accessible environment. The influence of the bulk salt rock, clay sediments and other geologic matrices on the transport behavior of actinides must be determined to establish the overall performance and capability of the WIPP in isolating waste from the environment. Tests to determine the capabilities of the WIPP geologic formations in retarding actinide species in several projected oxidation states would provide a means to demonstrate the effectiveness of the WIPP in retaining TRU wastes.

  9. Actinide and metal toxicity to prospective bioremediation bacteria.

    PubMed

    Ruggiero, Christy E; Boukhalfa, Hakim; Forsythe, Jennifer H; Lack, Joseph G; Hersman, Larry E; Neu, Mary P

    2005-01-01

    Bacteria may be beneficial for alleviating actinide contaminant migration through processes such as bioaccumulation or metal reduction. However, sites with radioactive contamination often contain multiple additional contaminants, including metals and organic chelators. Bacteria-based bioremediation requires that the microorganism functions in the presence of the target contaminant, as well as other contaminants. Here, we evaluate the toxicity of actinides, metals and chelators to two different bacteria proposed for use in radionuclide bioremediation, Deinococcus radiodurans and Pseudomonas putida, and the toxicity of Pu(VI) to Shewanella putrefaciens. Growth of D. radiodurans was inhibited at metal concentrations ranging from 1.8 microM Cd(II) to 32 mM Fe(III). Growth of P. putida was inhibited at metal concentrations ranging from 50 microM Ni(II) to 240 mM Fe(III). Actinides inhibited growth at mM concentrations: chelated Pu(IV), U(VI) and Np(V) inhibit D. radiodurans growth at 5.2, 2.5 and 2.1 mM respectively. Chelated U(VI) inhibits P. putida growth at 1.7 mM, while 3.6 mM chelated Pu(IV) inhibits growth only slightly. Pu(VI) inhibits S. putrefaciens growth at 6 mM. These results indicate that actinide toxicity is primarily chemical (not radiological), and that radiation resistance does not ensure radionuclide tolerance. This study also shows that Pu is less toxic than U and that actinides are less toxic than other types of metals, which suggests that actinide toxicity will not impede bioremediation using naturally occurring bacteria.

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

    SciTech Connect

    Soderquist, Chuck Z.; Weaver, Jamie L.

    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.

  11. Enhancing BWR Proliferation Resistance Fuel with Minor Actinides

    SciTech Connect

    Gray S. Chang

    2008-07-01

    Key aspects of the Global Nuclear Energy Partnership (GNEP) are to significantly advance the science and technology of nuclear energy systems and the Advanced Fuel Cycle (AFC) program. It consists of both innovative nuclear reactors and innovative research in separation and transmutation. To accomplish these goals, international cooperation is very important and public acceptance is crucial. The merits of nuclear energy are high-density energy, with low environmental impacts (i.e. almost zero greenhouse gas emission). Planned efforts involve near-term and intermediate-term improvements in fuel utilization and recycling in current light water reactors (LWRs) as well as the longer-term development of new nuclear energy systems that offer much improved fuel utilization and proliferation resistance, along with continued advances in operational safety. The challenges are solving the energy needs of the world, protection against nuclear proliferation, the problem of nuclear waste, and the global environmental problem. To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu and 240Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides (237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu /Pu. For future advanced nuclear systems, the minor actinides (MA) are viewed more as a resource to be recycled, or transmuted to less hazardous and possibly more useful forms, rather than simply as a waste stream to be disposed of in expensive repository facilities. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the

  12. An overview of results obtained in intercomparison exercises for determination of actinides.

    PubMed

    Benedik, L

    2013-11-01

    In recent years the Jožef Stefan Institute participated in numerous intercomparison exercises for determination of natural and man-made radionuclides. The reported values were mostly in good agreement with the resulting reference values. This paper describes an analysis of the measurement results obtained in intercomparison exercises for determination of actinides in the period from 2009 to 2011, organised by the National Physical Laboratory and the Bundesamt für Strahlenschutz. The review covers neptunium, plutonium and americium radioisotopes over this period.

  13. Actinides in metallic waste from electrometallurgical treatment of spent nuclear fuel

    NASA Astrophysics Data System (ADS)

    Janney, D. E.; Keiser, D. D.

    2003-09-01

    Argonne National Laboratory has developed a pyroprocessing-based technique for conditioning spent sodium-bonded nuclear-reactor fuel in preparation for long-term disposal. The technique produces a metallic waste form whose nominal composition is stainless steel with 15 wt.% Zr (SS-15Zr), up to ˜ 11 wt.% actinide elements (primarily uranium), and a few percent metallic fission products. Actual and simulated waste forms show similar eutectic microstructures with approximately equal proportions of iron solid solution phases and Fe-Zr intermetallics. This article reports on an analysis of simulated waste forms containing uranium, neptunium, and plutonium.

  14. Method for extracting lanthanides and actinides from acid solutions

    DOEpatents

    Horwitz, E. Philip; Kalina, Dale G.; Kaplan, Louis; Mason, George W.

    1985-01-01

    A process for the recovery of actinide and lanthanide values from aqueous acidic solutions with an organic extractant having the formula: ##STR1## where .phi. is phenyl, R.sup.1 is a straight or branched alkyl or alkoxyalkyl containing from 6 to 12 carbon atoms and R.sup.2 is an alkyl containing from 3 to 6 carbon atoms. The process is suitable for the separation of actinide and lanthanide values from fission product values found together in high level nuclear reprocessing waste solutions.

  15. Isotopic and criticality validation for actinide-only burnup credit

    SciTech Connect

    Fuentes, E.; Lancaster, D.; Rahimi, M.

    1997-07-01

    The techniques used for actinide-only burnup credit isotopic validation and criticality validation are presented and discussed. Trending analyses have been incorporated into both methodologies, requiring biases and uncertainties to be treated as a function of the trending parameters. The isotopic validation is demonstrated using the SAS2H module of SCALE 4.2, with the 27BURNUPLIB cross section library; correction factors are presented for each of the actinides in the burnup credit methodology. For the criticality validation, the demonstration is performed with the CSAS module of SCALE 4.2 and the 27BURNUPLIB, resulting in a validated upper safety limit.

  16. Production of heavy actinides in incomplete fusion reactions

    NASA Astrophysics Data System (ADS)

    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).

  17. New cubic structure compounds as actinide host phases

    NASA Astrophysics Data System (ADS)

    Stefanovsky, S. V.; Yudintsev, S. V.; Livshits, T. S.

    2010-03-01

    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 Gd2Zr2O7) has excellent radiation resistance and high chemical durability but requires high temperatures (at least 1500 °C) to be produced by hot-pressing from sol-gel derived precursor. Partial Sn4+ substitution for Zr4+ reduces production temperature and the compounds REE2ZrSnO7 may be hot-pressed or cold pressed and sintered at ~1400 °C. Pyrochlore, A2B2O7-x (two-fold elementary fluorite unit cell), and murataite, A3B6C2O20-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. % AnO2 (An = Th, U, Np, Pu) or REE/An fraction of HLW form at crystallization zoned grains composed sequentially of the 5C → 8C → 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 more promising actinide hosts are ferrites with garnet structure. The matrices containing sometime complex fluorite

  18. Analogue Study of Actinide Transport at Sites in Russia

    SciTech Connect

    Novikov, A P; Simmons, A M; Halsey, W G

    2003-02-12

    The U. S. Department of Energy (DOE) and the Russian Academy of Sciences (RAS) are engaged in a three-year cooperative study to observe the behavior of actinides in the natural environment at selected disposal sites and/or contamination sites in Russia. The purpose is to develop experimental data and models for actinide speciation, mobilization and transport processes in support of geologic repository design, safety and performance analyses. Currently at the mid-point of the study, the accomplishments to date include: evaluation of existing data and data needs, site screening and selection, initial data acquisition, and development of preliminary conceptual models.

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

    DOEpatents

    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)

  20. Thermodynamic constants for actinide oxides and oxyhydroxides relevant to actinide volatility calculations for thermal oxidation processes

    SciTech Connect

    Ebbinghaus, B.B.; Krikorian, O.H.

    1993-10-27

    The purpose of this report is to provide input of thermodynamic data on actinide volatilities to EERC for use in their computer code for modeling of metal volatilities in incinerators. It is also anticipated that the data may be documented later in an EPA sponsored ``Metals Bible.`` It should be noted that only upper limits for the volatility of PuO{sub 2}(s) due to PuO{sub 3}(g) and PuO{sub 2}(OH){sub 2}(g) and the volatility of AmO{sub 2} in PuO{sub 2}(s) due to AmO{sub 3}(g) and AmO{sub 2}(OH){sub 2}(g) could be set. The data on the americium vapor species are intended for calculations where AmO{sub 2} is present as a solid solution in PuO{sub 2}(s).

  1. Novel complexing agents for the efficient separation of actinides and remediation of actinide-contaminated sites

    SciTech Connect

    Baisden, P.; Kadkhodayan, B.

    1996-03-15

    Research into the coordination chemistry of transactinide elements should provide us with new fundamental knowledge about structure, geometry, and stability of these metal complexes. Our approach involves the design, synthesis, and characterization of {open_quotes}expanded porphyrin{close_quotes} macrocyclic ligands which coordinate the actinide metal cations with high thermodynamic affinity and kinetic stability. We can use the knowledge from understanding the fundamental coordination chemistry of these elements as a stepping stone to heavy metal detoxification, radioactive waste cleanup, and possibly radioactive isotope separation. The critical components of this research endeavor, along with the viability of metal complex formation, will be correlated to ring size and core geometry of the ligand and, the atomic radius, oxidation state, coordination geometry and coordination number of the transactinium metal ion. These chelating agents may have certain applications to the solution of some radioactive waste problems if they can be attached to polymer supports and used to chemically separate the radioactive components in waste.

  2. Hydrothermal method of preparation of actinide(IV) phosphate hydrogenphosphate hydrates and study of their conversion into actinide(IV) phosphate diphosphate solid solutions.

    PubMed

    Dacheux, N; Grandjean, S; Rousselle, J; Clavier, N

    2007-11-26

    Several compositions of Th2-x/2AnIVx/2(PO4)2(HPO4).H2O (An=U, Np, Pu) were prepared through hydrothermal precipitation from a mixture of nitric solutions containing cations and concentrated phosphoric acid. All the samples were fully characterized by X-ray diffraction, UV-vis, and infrared spectroscopies to check for the existence of thorium-actinide(IV) phosphate hydrogenphosphate hydrates solid solutions. Such compounds were obtained as single phases, up to x=4 for uranium, x=2 for neptunium, and x<4 for plutonium, the cations being fully maintained in the tetravalent oxidation state. In a second step, the samples obtained after heating crystallized precursors at high temperature (1100 degrees C) were characterized. Single-phase thorium-actinide(IV) phosphate-diphosphate solid solutions were obtained up to x=0.8 for Np(IV) and x=1.6 for Pu(IV). For higher substitution rates, polyphase systems composed by beta-TAnPD, An2O(PO4)2, and/or alpha-AnP2O7 were formed. Finally, this hydrothermal route of preparation was applied successfully to the synthesis of an original phosphate-based compound incorporating simultaneously tetravalent uranium, neptunium and plutonium. PMID:17973479

  3. Tank waste remediation system (TWRS) mission analysis

    SciTech Connect

    Rieck, R.H.

    1996-10-03

    The Tank Waste Remediation System Mission Analysis provides program level requirements and identifies system boundaries and interfaces. Measures of success appropriate to program level accomplishments are also identified.

  4. Monte Carlo isotopic inventory analysis for complex nuclear systems

    NASA Astrophysics Data System (ADS)

    Phruksarojanakun, Phiphat

    . Potential applications of MCise include molten salt fueled reactors and liquid breeders in fusion blankets. As an example, the inventory analysis of a liquid actinide fuel in the In-Zinerator, a sub-critical power reactor driven by a fusion source, is examined. The result reassures MCise as a reliable tool for inventory analysis of complex nuclear systems.

  5. Excitation functions for production of heavy actinides from interactions of /sup 18/O with /sup 248/Cm and /sup 249/Cf

    SciTech Connect

    Lee, D.; Moody, K.J.; Nurmia, M.J.; Seaborg, G.T.; von Gunten, H.R.; Hoffman, D.C.

    1983-06-01

    Excitation functions have been measured for the production of isotopes of Bk through Fm in bombardments of /sup 248/Cm with 97- to 122-MeV /sup 18/O ions and of isotopes of Bk through No in bombardments of /sup 249/Cf with 91- to 150-MeV /sup 18/O ions. The cross sections and widths of the mass distributions for the actinides produced in these reactions are very similar for transfer of the same numbers of nucleons. A semiquantitative comparison of the experimental results with calculations based on a simple model shows that calculations of this type are helpful in selection of projectile-target systems and optimum energies for production of specific actinide isotopes and for synthesis of as yet unknown heavy isotopes and elements. Comparisons of experimental results with calculations show that, in general, about half of the kinetic energy of the projectile is transferred to the actinide product.

  6. Actinide(IV) Deposits on Bone: Potential Role of the Osteopontin-Thorium Complex.

    PubMed

    Creff, Gaëlle; Safi, Samir; Roques, Jérôme; Michel, Hervé; Jeanson, Aurélie; Solari, Pier-Lorenzo; Basset, Christian; Simoni, Eric; Vidaud, Claude; Den Auwer, Christophe

    2016-01-01

    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. PMID:26684435

  7. Actinide(IV) Deposits on Bone: Potential Role of the Osteopontin-Thorium Complex.

    PubMed

    Creff, Gaëlle; Safi, Samir; Roques, Jérôme; Michel, Hervé; Jeanson, Aurélie; Solari, Pier-Lorenzo; Basset, Christian; Simoni, Eric; Vidaud, Claude; Den Auwer, Christophe

    2016-01-01

    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. Systems Analysis of Thrombus Formation.

    PubMed

    Diamond, Scott L

    2016-04-29

    The systems analysis of thrombosis seeks to quantitatively predict blood function in a given vascular wall and hemodynamic context. Relevant to both venous and arterial thrombosis, a Blood Systems Biology approach should provide metrics for rate and molecular mechanisms of clot growth, thrombotic risk, pharmacological response, and utility of new therapeutic targets. As a rapidly created multicellular aggregate with a polymerized fibrin matrix, blood clots result from hundreds of unique reactions within and around platelets propagating in space and time under hemodynamic conditions. Coronary artery thrombosis is dominated by atherosclerotic plaque rupture, complex pulsatile flows through stenotic regions producing high wall shear stresses, and plaque-derived tissue factor driving thrombin production. In contrast, venous thrombosis is dominated by stasis or depressed flows, endothelial inflammation, white blood cell-derived tissue factor, and ample red blood cell incorporation. By imaging vessels, patient-specific assessment using computational fluid dynamics provides an estimate of local hemodynamics and fractional flow reserve. High-dimensional ex vivo phenotyping of platelet and coagulation can now power multiscale computer simulations at the subcellular to cellular to whole vessel scale of heart attacks or strokes. In addition, an integrated systems biology approach can rank safety and efficacy metrics of various pharmacological interventions or clinical trial designs. PMID:27126646

  9. Systems Analysis of Thrombus Formation.

    PubMed

    Diamond, Scott L

    2016-04-29

    The systems analysis of thrombosis seeks to quantitatively predict blood function in a given vascular wall and hemodynamic context. Relevant to both venous and arterial thrombosis, a Blood Systems Biology approach should provide metrics for rate and molecular mechanisms of clot growth, thrombotic risk, pharmacological response, and utility of new therapeutic targets. As a rapidly created multicellular aggregate with a polymerized fibrin matrix, blood clots result from hundreds of unique reactions within and around platelets propagating in space and time under hemodynamic conditions. Coronary artery thrombosis is dominated by atherosclerotic plaque rupture, complex pulsatile flows through stenotic regions producing high wall shear stresses, and plaque-derived tissue factor driving thrombin production. In contrast, venous thrombosis is dominated by stasis or depressed flows, endothelial inflammation, white blood cell-derived tissue factor, and ample red blood cell incorporation. By imaging vessels, patient-specific assessment using computational fluid dynamics provides an estimate of local hemodynamics and fractional flow reserve. High-dimensional ex vivo phenotyping of platelet and coagulation can now power multiscale computer simulations at the subcellular to cellular to whole vessel scale of heart attacks or strokes. In addition, an integrated systems biology approach can rank safety and efficacy metrics of various pharmacological interventions or clinical trial designs.

  10. DIGITAL SPALL RADIOGRAPH ANALYSIS SYSTEM

    SciTech Connect

    CURTIS L. HARRIS - LATA

    1990-01-01

    This report describes progress on work to develop a cost effective, rapid response system for measuring Technology Assessment National Laboratory. momentum and kinetic energy of span for the Advanced Center (ATAC) Armor/Anti-Armor (As) program at Los Alamos The system will exploit data contained in two sets of simultaneous co-planar flash radiographs taken along the center line of anticipated span motion. Data contained in each set (which is proportional to the mass and z-number of the span material intersected by the exposing x-ray at each point) is digitized and used to construct a three dimensional model (called the reconstructed span image) that approximates the original span cloud. From the model the mass of span fragments is computed. The two sets of radiographs, separated in time, represent the span configuration at two instants of time. Span fragments from the first instant are matched with those from the second instant to determine velocity. Evaluation of the fidelity of candidate reconstruction algorithms is the highest priority task in. this development program for the obvious reason that the efficacy of the projected span analysis system depends upon the fidelity of the reconstruction techniques.

  11. Extraction of DBP and MBP from actinides: application to the recovery of actinides from TBP-sodium carbonate scrub solutions. [Aralex process

    SciTech Connect

    Horwitz, E.P.; Mason, G.W.; Bloomquist, C.A.A.; Leonard, R.A.; Bernstein, G.J.

    1980-01-01

    A flowsheet for the recovery of actinides from TBP-Na/sub 2/CO/sub 3/ scrub waste solutions has been developed, based on batch extraction data, and tested, using laboratory scale counter-current extraction techniques. The process, called the ARALEX process, utilizes 2-ethyl-1-hexanol (2-EHOH) to extract the TBP degradation products (HDBP and H/sub 2/MBP) from acidified Na/sub 2/CO/sub 3/ scrub waste leaving the actinides in the aqueous phase. Dibutyl and monobutyl phosphoric acids are attached to the 2-EHOH molecules through hydrogen bonds. These hydrogen bonds also diminish the ability of the HDBP and H/sub 2/MBP to complex actinides and thus all actinides remain in the aqueous raffinate. Dilute sodium hydroxide solutions can be used to back-extract the dibutyl and monobutyl phosphoric acid esters as their sodium salts. The 2-EHOH can then be recycled. After extraction of the acidified carbonate waste with 2-EHOH, the actinides may be readily extracted from the raffinate with DHDECMP or, in the case of tetra- and hexavalent actinides, with TBP. The ARALEX process is relatively simple and involves inexpensive and readily available chamicals. The ARALEX process can also be applied to other actinide waste streams which contain appreciable concentrations of polar organic compounds that interfere with conventional actinide ion exchange and liquid-liquid extraction procedures. One such application is the removal of detergents from laundry or clean-up solutions contaminated with actinides.

  12. Method for recovery of actinides from actinide-bearing scrap and waste nuclear material using O/sub 2/F/sub 2/

    DOEpatents

    Asprey, L.B.; Eller, P.G.

    1984-09-12

    Method for recovery of actinides from nuclear waste material containing sintered and other oxides thereof and from scrap materials containing the metal actinides using O/sub 2/F/sub 2/ to generate the hexafluorides of the actinides present therein. The fluorinating agent, O/sub 2/F/sub 2/, has been observed to perform the above-described tasks at sufficiently low temperatures that there is virtually no damage to the containment vessels. Moreover, the resulting actinide hexafluorides are not detroyed by high temperature reactions with the walls of the reaction vessel. Dioxygen difluoride is readily prepared, stored and transferred to the place of reaction.

  13. Physical and chemical characterization of actinides in soil from Johnston Atoll

    SciTech Connect

    Wolf, S.F.; Bates, J.K.; Buck, E.C.; Dietz, N.L.; Fortner, J.A.; Brown, N.R.

    1997-02-01

    Characterization of the actinide content of a sample of contaminated coral soil from Johnston Atoll, the site of three non-nuclear destructs of nuclear warhead-carrying THOR missiles in 1962, revealed that >99% of the total actinide content is associated with discrete bomb fragments. After removal of these fragments, there was an inverse correlation between actinide content and soil particle size in particles from 43 to 0.4 {mu}m diameter. Detailed analyses of this remaining soil revealed no discrete actinide phase in these soil particles, despite measurable actinide content. Observations indicate that exposure to the environment has caused the conversion of relatively insoluble actinide oxides to the more soluble actinyl oxides and actinyl carbonate coordinated complexes. This process has led to dissolution of actinides from discrete particles and migration to the surrounding soil surfaces, resulting in a dispersion greater than would be expected by physical transport of discrete particles alone. 26 refs., 4 figs., 1 tab.

  14. Placental transfer of the actinides and related heavy elements

    SciTech Connect

    Sikov, M.R.

    1986-11-01

    A selective literature review dealing with prenatal exposure of animals and humans to actinides and related heavy elements, comparative aspects of placental transfer and fetoplacental distribution are considered. General patterns have been derived from typical quantitative values, and used to compare similarities and dissimilarities, and to examine factors responsible for observed differences. 37 refs., 2 tabs.

  15. Citrate based ``TALSPEAK`` lanthanide-actinide separation process

    SciTech Connect

    Del Cul, G.D.; Bond, W.D.; Toth, L.M.; Davis, G.D.; Dai, S.; Metcalf, D.H.

    1994-09-01

    The potential hazard posed to future generations by long-lived radionuclides such as the transuranic elements (TRU) is perceived as a major problem associated with the use of nuclear power. TRU wastes have to remain isolated from the environment for ``geological`` periods of time. The costs of building, maintaining, and operating a ``geological TRU repository`` can be very high. Therefore, there are significant economical advantages in segregating the relatively low volume of TRU wastes from other nuclear wastes. The chemical behavior of lanthanides and actinides, 4f and 5f elements respectively, is rather similar. As a consequence, the separation of these two groups is difficult. The ``TALSPEAK`` process (Trivalent Actinide Lanthanide Separations by Phosphorus-reagent Extraction from Aqueous Complexes) is one of the few means available to separate the trivalent actinides from the lanthanides. The method is based on the preferential complexation of the trivalent actinides by an aminopolyacetic acid. Cold experiments showed that by using citric acid the deleterious effects produced by impurities such as zirconium are greatly reduced.

  16. Chemistry of the heaviest actinides: fermium, mendelevium, nobelium, and lawrencium

    SciTech Connect

    Hulet, E.K.

    1980-01-01

    Conclusions regarding these shifts toward greater stabilization of 5f orbitals with increasing atomic number are mainly supported by the appearance of the divalent oxidation state well before the end of the actinide series and the predominance of the divalent state in the next to last element in the series. These conclusions and the underlying experimental evidence are the main subject of this review.

  17. Actinide Targets for Neutron Cross Section Measurements (C)

    SciTech Connect

    J. D. Baker; C. A. McGrath

    2006-04-01

    The Advanced Fuel Cycle Initiative (AFCI) and the Generation IV Reactor Initiative have demonstrated a lack of detailed neutron cross-sections for certain "minor" actinides, those other than the most common (235U, 238U, and 239Pu). For some closed-fuel-cycle reactor designs more than 50% of reactivity will, at some point, be derived from “minor” actinides that currently have poorly known (n,g) and (n,f) cross sections. A program of measurements under AFCI has begun to correct this. One of the initial hurdles has been to produce well-characterized, highly isotopically enriched, and chemically pure actinide targets on thin backings. Using a combination of resurrected techniques and new developments, we have made a series of targets including highly enriched 240Pu, and 242Pu. Thus far, we have electrodeposited these actinide targets. In the future, we plan to study reductive distillation to achieve homogeneous, adherent targets on thin metal foils and polymer backings. As we move forward, separated isotopes become scarcer, and safety concerns become greater. The chemical purification and electodeposition techniques will be described.

  18. Colloid-borne forms of tetravalent actinides: a brief review.

    PubMed

    Zänker, Harald; Hennig, Christoph

    2014-02-01

    Tetravalent actinides, An(IV), are usually assumed to be little mobile in near-neutral environmental waters because of their low solubility. However, there are certain geochemical scenarios during which mobilization of An(IV) in a colloid-borne (waterborne) form cannot be ruled out. A compilation of colloid-borne forms of tetravalent actinides described so far for laboratory experiments together with several examples of An(IV) colloids observed in field experiments and real-world scenarios are given. They are intended to be a knowledge base and a tool for those who have to interpret actinide behavior under environmental conditions. Synthetic colloids containing structural An(IV) and synthetic colloids carrying adsorbed An(IV) are considered. Their behavior is compared with the behavior of An(IV) colloids observed after the intentional or unintentional release of actinides into the environment. A list of knowledge gaps as to the behavior of An(IV) colloids is provided and items which need further research are highlighted.

  19. Magnetism in the actinides: the role of neutron scattering

    SciTech Connect

    Lander, G.H.

    1982-01-01

    Neutron scattering has played a crucial and unique role of elucidating the magnetism in actinide compounds. Examples are given of elastic scattering to determine magnetic structures, measure spatial correlations in the critical regime, and magnetic form factors, and of inelastic scattering to measure the (often elusive) spin excitations. Some future directions will be discussed.

  20. Microwave landing system autoland system analysis

    NASA Technical Reports Server (NTRS)

    Feather, J. B.; Craven, B. K.

    1991-01-01

    The objective was to investigate the ability of present day aircraft equipped with automatic flight control systems to fly advanced Microwave Landing Systems (MLS) approaches. The tactical approach used to achieve this objective included reviewing the design and autoland operation of the MD-80 aircraft, simulating the MLS approaches using a batch computer program, and assessing the performance of the autoland system from computer generated data. The results showed changes were required to present Instrument Landing System (ILS) procedures to accommodate the new MLS curved paths. It was also shown that in some cases, changes to the digital flight guidance systems would be required so that an autoland could be performed.

  1. Flow analysis system and method

    NASA Technical Reports Server (NTRS)

    Hill, Wayne S. (Inventor); Barck, Bruce N. (Inventor)

    1998-01-01

    A non-invasive flow analysis system and method wherein a sensor, such as an acoustic sensor, is coupled to a conduit for transmitting a signal which varies depending on the characteristics of the flow in the conduit. The signal is amplified and there is a filter, responsive to the sensor signal, and tuned to pass a narrow band of frequencies proximate the resonant frequency of the sensor. A demodulator generates an amplitude envelope of the filtered signal and a number of flow indicator quantities are calculated based on variations in amplitude of the amplitude envelope. A neural network, or its equivalent, is then used to determine the flow rate of the flow in the conduit based on the flow indicator quantities.

  2. Evaluation of Heterogeneous Options: Effects of MgO versus UO2 Matrix Selection for Minor Actinide Targets in a Sodium Fast Reactor

    SciTech Connect

    M. Pope; S. Bays; R. Ferrer

    2008-03-01

    The primary focus of this work was to compare MgO with UO2 as target matrix material options for burning minor actinides in a transmutation target within a sodium fast reactor. This analysis compared the transmutation performance of target assemblies having UO2 matrix to those having specifically MgO inert matrix.

  3. Actinide Speciation and Solubility in a Salt Repository (Invited)

    NASA Astrophysics Data System (ADS)

    Reed, D.; Borkowski, M.; Richmann, M.; Lucchini, J.; Khaing, H.; Swanson, J.

    2009-12-01

    The use of bedded salt deposits for the permanent disposal of nuclear waste continues to receive much attention in the United States and internationally. This is largely based on the highly successful Waste Isolation Pilot Plant (WIPP) transuranic waste repository that was opened in 1999 in Southeastern New Mexico. A bedded salt formation, such as the one in which the WIPP is located, has many advantages that make it an ideal geology for permanent disposal of nuclear waste. This includes well established mining techniques, self-sealing that lead to a naturally-induced geologic isolation, a relatively dry environment, and a favorable chemistry. Herein we report on recent progress in our investigations, as part of ongoing recertification effort for the operating WIPP repository, to establish the redox distribution and overall solubility of actinides in brine. The overall ranking of actinides, from the perspective of potential contribution to release from the WIPP, is: Pu ~ Am >>U > Th >> Np, Cm. Our recent research emphasis has centered on the redox chemistry of multivalent actinides (e.g., U, Pu and Np) with the use of oxidation-state-invariant analogs (Th and Nd) to establish the solubilities. Under a wide range of conditions investigated, the predominant oxidation states established are Pu(III) and Pu(IV) for plutonium, U(IV) and U(VI) for uranium, and Am (III) for americium. Reduction pathways for plutonium include reaction with organics, reaction with reduced iron, and bioreduction by halophiles under anaerobic conditions. Uranium(VI) can also be reduced to U(IV) by reduced iron and microbial processes. Solubility data for neodymium (+3 analog), Uranium (+6 analog) and thorium (+4 analog) in brine are also reported. These data extend our past understanding of WIPP-specific actinide chemistry and show the WIPP, and salt-based repositories in general, to be a robust repository design from the perspective of actinide containment and immobilization.

  4. Actinide partitioning processes for fuel reprocessing and refabrication plant wastes

    SciTech Connect

    Finney, B.C.; Tedder, D.W.

    1980-01-01

    Chemical processing methods have been developed on a laboratory scale to partition the actinides from the liquid and solid fuel reprocessing plant (FRP) and refabrication plant (FFP) wastes. It was envisioned that these processes would be incorporated into separate waste treatment facilities (WTFs) that are adjacent to, but not integrated with, the fuel reprocessing and refabrication plants. Engineering equipment and material balance flowsheets have been developed for WTFs in support of a 2000-MTHM/year FRP and a 660-MTHM/year MOX-FFP. The processing subsystems incorporated in the FRP-WTF are: High-Level Solid Waste Treatment, High-Level Liquid Waste Treatment, Solid Alpha Waste Treatment, Cation Exchange Chromatography, Salt Waste Treatment, Actinide Recovery, Solvent Cleanup and recycle, Off-Gas Treatment, Actinide Product Concentration, and Acid and Water Recycle. The WTF supporting a fuel refabrication facility, although similar, does not contain subsystems (1) and (2). Based on the results of the laboratory and hot-cell experimental work, we believe that the processes and flowsheets offer the potential to reduce the total unrecovered actinides in FRP and FFP wastes to less than or equal to 0.25%. The actinide partitioning processes and the WTF concept represent advanced technology that would require substantial work before commercialization. It is estimated that an orderly development program would require 15 to 20 years to complete and would cost about 700 million 1979 dollars. It is estimated that the capital cost and annual operating cost, in mid-1979 dollars, for the FRP-WTF are $1035 million and $71.5 million/year, and for the FFP-WTF are $436 million and $25.6 million/year, respectively.

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

    SciTech Connect

    Raymond, K.N.; White, D.J.; Xu, Jide; Mohs, T.R.

    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.

  6. Dynamical analysis of an accelerator-based fluid-fueled subcritical radioactive waste burning system

    NASA Astrophysics Data System (ADS)

    Woosley, Michael Louis, Jr.

    The recent revival of interest in accelerator-driven subcritical fluid-fueled systems is documented. Several important applications of these systems are mentioned. In particular, new applications have focused on the destruction of high-level radioactive waste. Systems can be designed to quickly destroy the actinides and long-lived fission products from light water reactor fuel, weapons plutonium, and other high-level defense wastes. The proposed development of these systems is used to motivate the need for the development of dynamic analysis methods for their nuclear kinetics. A physical description of the Los Alamos Accelerator-Based Conversion (ABC) concept is provided. This system is used as the basis for the kinetics study in this research. The current approach to the dynamic simulation of an accelerator-driven subcritical fluid-fueled system includes three elements: A discrete ordinates model is used to calculate the flux distribution for the source-driven system; A nodal convection model is used to calculate time-dependent isotope and temperature distributions which impact reactivity; A nodal importance weighting model is used to calculate the reactivity impact of temperature and isotope distributions and to feed this information back to the time-dependent nodal convection model. Specific transients which have been analyzed with the current modeling system are discussed. These transients include loss-of-flow and loss-of-cooling accidents, xenon and samarium transients, and cold-plug and overfueling events. The results of various transients have uncovered unpredictable behavior, unresolved design issues, and the need for active control. Modest initiating events can cause significant swings in system temperature and power. The circulation of the fluid fuel can lead to oscillations on the relatively short scale of the loop circulation time. The system responds quickly to reactivity changes because the large neutron source overwhelms the damping effect of delayed

  7. Tank waste remediation system mission analysis report

    SciTech Connect

    Acree, C.D.

    1998-01-06

    The Tank Waste Remediation System Mission Analysis Report identifies the initial states of the system and the desired final states of the system. The Mission Analysis Report identifies target measures of success appropriate to program-level accomplishments. It also identifies program-level requirements and major system boundaries and interfaces.

  8. Actinide Production in the Reaction of Heavy Ions withCurium-248

    SciTech Connect

    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.

  9. Long-term risk from actinides in the environment: Modes of mobility. 1998 annual progress report

    SciTech Connect

    Breshears, D.D.; Whicker, J.J.; Ibrahim, S.A.; Whicker, F.W.; Hakonson, T.E.; Kirchner, T.

    1998-06-01

    'The mobility of actinides in surface soils is a key issue of concern at several DOE facilities in arid and semiarid environments, including Rocky Flats, Hanford, Nevada Test Site, Idaho National Engineering Laboratory, and Los Alamos National Laboratory and the Waste Isolation Pilot Plant (WIPP). Key sources of uncertainty in assessing Pu mobility are the magnitudes of mobility resulting from three modes of transport: (1) wind erosion, (2) water erosion, and (3) vertical migration. Each of these three processes depend on numerous environmental factors and they compete with one another, particularly for actinides in very shallow soils ({approximately} 1 \\265m). The overall goal of the study is to quantify the mobility of soil actinides from all three modes. The authors study is using field measurements, laboratory experiments, and ecological modeling to address these three processes at three DOE facilities where actinide kinetics are of concern: WIPP, Rocky Flats, and Hanford. Wind erosion is being measured with suite of monitoring equipment, water erosion is being studied with rainfall simulation experiments, vertical migration is being studied in controlled laboratory experiments, and the three processes are being integrated using ecological modeling. Estimates for clean up of soil actinides for the extensive tracts of DOE land range to hundreds of billion $ in the US Without studies of these processes, unnecessary clean-up of these areas may waste billions of dollars and cause irreparable ecological damage through the soil removal. Further, the outcomes of litigation against DOE are dependent on quantifying the mobility of actinides in surface soils. This report provides a summary of work for the first year of a 3-year project; subcontracts to collaborating institutions (Colorado State University and New Mexico State University) were not in place until late December 1997, and hence this report focuses on the results of the 5 months from January through May 1998

  10. Modeling and analysis of a molten salt electrowinning system with liquid cadmium cathode

    SciTech Connect

    Kim, K.R.; Ahn, D.H.; Paek, S.; Kwon, S.W.; Kim, S.H.; Shim, J.B.; Chung, H.; Kim, E.H.

    2007-07-01

    In the present work, an electrowinning process in the LiCl-KCl/Cd system is considered to model and analyze the equilibrium behavior and electro-transport of the actinide and rare-earth elements. Equilibrium distributions of the actinide and rare-earth elements in a molten salt and liquid cadmium system have been estimated for an infinite potentiostatic electrolysis from the thermodynamic data and material balance. A simple dynamic modeling of this process was performed by taking into account the material balances and diffusion-controlled electrochemical reactions in a diffusion layer at an electrode interface between the molten salt and liquid cadmium cathode. This model demonstrated a prediction of the concentration behaviors, a faradic current of each element and an electrochemical potential as function of the time up to the corresponding electro-transport satisfying a given applied current based on a galvano-static electrolysis. (authors)

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

    PubMed

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

    2012-08-01

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

  12. Integrated analysis environment for high impact systems

    SciTech Connect

    Martinez, M.; Davis, J.; Scott, J.; Sztipanovits, J.; Karsai, G.

    1998-02-01

    Modeling and analysis of high consequence, high assurance systems requires special modeling considerations. System safety and reliability information must be captured in the models. Previously, high consequence systems were modeled using separate, disjoint models for safety, reliability, and security. The MultiGraph Architecture facilitates the implementation of a model integrated system for modeling and analysis of high assurance systems. Model integrated computing allows an integrated modeling technique to be applied to high consequence systems. Among the tools used for analyzing safety and reliability are a behavioral simulator and an automatic fault tree generation and analysis tool. Symbolic model checking techniques are used to efficiently investigate the system models. A method for converting finite state machine models to ordered binary decision diagrams allows the application of symbolic model checking routines to the integrated system models. This integrated approach to modeling and analysis of high consequence systems ensures consistency between the models and the different analysis tools.

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

    SciTech Connect

    Gunnink, R

    1991-09-01

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

  14. Sigma Team for Minor Actinide Separation: PNNL FY 2010 Status Report

    SciTech Connect

    Lumetta, Gregg J.; Sinkov, Sergey I.; Neiner, Doinita; Levitskaia, Tatiana G.; Braley, Jenifer C.; Carter, Jennifer C.; Warner, Marvin G.; Pittman, Jonathan W.; Rapko, Brian M.

    2010-08-24

    Work conducted at Pacific Northwest National Laboratory (PNNL) in FY 2010 addressed two lines of inquiry. The two hypotheses put forth were: 1. The extractants from the TRUEX( ) process (CMPO)( ) and from the TALSPEAK( ) process (HDEHP)( ) can be combined into a single process solvent to separate 1) the lanthanides and actinides from acidic high-level waste and 2) the actinides from the lanthanides in a single solvent extraction process. (Note: This combined process will hereafter be referred to as the TRUSPEAK process.) A series of empirical measurements performed (both at PNNL and Argonne National Laboratory) in FY 2009 supported this hypothesis, but also indicated some nuances to the chemistry. Lanthanide/americium separation factors of 12 and higher were obtained with a prototypic TRUSPEAK solvent when extracting the lanthanides from a citrate-buffered DTPA( ) solution. Although the observed separation factors are sufficiently high to design an actinide/lanthanide separation process, a better understanding of the chemistry is expected to lead to improved solvent formulations and improved process performance. Work in FY 2010 focused on understanding the synergistic extraction behavior observed for Nd(III) and Am(III) when extracted into mixtures of CMPO and HDEHP. The interaction between CMPO and HDEHP in dodecane was investigated by 31P NMR spectroscopy, and an adduct of the type CMPO•HDEHP was found to form. The formation of this adduct will reduce the effective extractant concentrations and must be taken into account when modeling metal ion extraction data in this system. Studies were also initiated to determine the Pitzer parameters for Nd(III) in lactate media. 2. Higher oxidation states (e.g., +5 and +6) of Am can be stabilized in solution by complexation with uranophilic ligands, and this chemistry can be exploited to separate Am from Cm. To test this hypothesis, the previously reported stereognostic uranophilic ligands NPB( ) and ETAC(e) were

  15. Detection limits for actinides in a monochromatic, wavelength-dispersive x-ray fluorescence instrument

    SciTech Connect

    Collins, Michael L; Havrilla, George J

    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.

  16. The strength of actinide-element bonds from the quantum theory of atoms-in-molecules.

    PubMed

    Huang, Qian-Rui; Kingham, Jennifer R; Kaltsoyannis, Nikolas

    2015-02-14

    [AnX(3)](2)(μ-η(2):η(2)-N(2)) (An = Th-Pu; X = F, Cl, Br, Me, H, OPh) have been studied using relativistic density functional theory. Geometric and vibrational data suggest that metal→N(2) charge transfer maximises at the protactinium systems, which feature the longest N-N bonds and the smallest σ(N-N), as a result of partial population of the N-N π* orbitals. There is very strong correlation of the standard quantum theory of atoms-in-molecules (QTAIM) metrics - bond critical point ρ, ∇(2)ρ and H and delocalisation indices - with An-N and N-N bond lengths and σ(N-N), but the correlation with An-N interaction energies is very poor. A similar situation exists for the other systems studied; neutral and cationic actinide monoxide and dioxides, and AnL(3+) and AnL(3)(3+) (L = pyridine (Py), pyrazine (Pz) and triazine (Tz)) with the exception of some of the ∇(2)ρ data, for which moderate to good correlations with energy data are sometimes seen. By contrast, in almost all cases there is very strong correlation of interaction and bond energies with |ΔQ(QTAIM)(An)|, a simple QTAIM metric which measures the amount of charge transferred to or from the actinide on compound formation.

  17. The strength of actinide-element bonds from the quantum theory of atoms-in-molecules.

    PubMed

    Huang, Qian-Rui; Kingham, Jennifer R; Kaltsoyannis, Nikolas

    2015-02-14

    [AnX(3)](2)(μ-η(2):η(2)-N(2)) (An = Th-Pu; X = F, Cl, Br, Me, H, OPh) have been studied using relativistic density functional theory. Geometric and vibrational data suggest that metal→N(2) charge transfer maximises at the protactinium systems, which feature the longest N-N bonds and the smallest σ(N-N), as a result of partial population of the N-N π* orbitals. There is very strong correlation of the standard quantum theory of atoms-in-molecules (QTAIM) metrics - bond critical point ρ, ∇(2)ρ and H and delocalisation indices - with An-N and N-N bond lengths and σ(N-N), but the correlation with An-N interaction energies is very poor. A similar situation exists for the other systems studied; neutral and cationic actinide monoxide and dioxides, and AnL(3+) and AnL(3)(3+) (L = pyridine (Py), pyrazine (Pz) and triazine (Tz)) with the exception of some of the ∇(2)ρ data, for which moderate to good correlations with energy data are sometimes seen. By contrast, in almost all cases there is very strong correlation of interaction and bond energies with |ΔQ(QTAIM)(An)|, a simple QTAIM metric which measures the amount of charge transferred to or from the actinide on compound formation. PMID:25307773

  18. Technical and economic assessment of different options for minor actinide transmutation: the French case

    SciTech Connect

    Chabert, C.; Coquelet-Pascal, C.; Saturnin, A.; Mathonniere, G.; Boullis, B.; Warin, D.; Van Den Durpel, L.; Caron-Charles, M.; Garzenne, C.

    2013-07-01

    Studies have been performed to assess the industrial perspectives of partitioning and transmutation of long-lived elements. These studies were carried out in tight connection with GEN-IV systems development. The results include the technical and economic evaluation of fuel cycle scenarios along with different options for optimizing the processes between the minor actinide transmutation in fast neutron reactors, their interim storage and geological disposal of ultimate waste. The results are analysed through several criteria (impacts on waste, on waste repository, on fuel cycle plants, on radiological exposure of workers, on costs and on industrial risks). These scenario evaluations take place in the French context which considers the deployment of the first Sodium-cooled Fast Reactor (SFR) in 2040. 3 management options of minor actinides have been studied: no transmutation, transmutation in SFR and transmutation in an accelerator-driven system (ADS). Concerning economics the study shows that the cost overrun related to the transmutation process could vary between 5 to 9% in SFR and 26 % in the case of ADS.

  19. ADVANCED POWER SYSTEMS ANALYSIS TOOLS

    SciTech Connect

    Robert R. Jensen; Steven A. Benson; Jason D. Laumb

    2001-08-31

    The use of Energy and Environmental Research Center (EERC) modeling tools and improved analytical methods has provided key information in optimizing advanced power system design and operating conditions for efficiency, producing minimal air pollutant emissions and utilizing a wide range of fossil fuel properties. This project was divided into four tasks: the demonstration of the ash transformation model, upgrading spreadsheet tools, enhancements to analytical capabilities using the scanning electron microscopy (SEM), and improvements to the slag viscosity model. The ash transformation model, Atran, was used to predict the size and composition of ash particles, which has a major impact on the fate of the combustion system. To optimize Atran key factors such as mineral fragmentation and coalescence, the heterogeneous and homogeneous interaction of the organically associated elements must be considered as they are applied to the operating conditions. The resulting model's ash composition compares favorably to measured results. Enhancements to existing EERC spreadsheet application included upgrading interactive spreadsheets to calculate the thermodynamic properties for fuels, reactants, products, and steam with Newton Raphson algorithms to perform calculations on mass, energy, and elemental balances, isentropic expansion of steam, and gasifier equilibrium conditions. Derivative calculations can be performed to estimate fuel heating values, adiabatic flame temperatures, emission factors, comparative fuel costs, and per-unit carbon taxes from fuel analyses. Using state-of-the-art computer-controlled scanning electron microscopes and associated microanalysis systems, a method to determine viscosity using the incorporation of grey-scale binning acquired by the SEM image was developed. The image analysis capabilities of a backscattered electron image can be subdivided into various grey-scale ranges that can be analyzed separately. Since the grey scale's intensity is

  20. Radiological Safety Analysis Code System.

    2009-12-22

    Version 03 RSAC-6.2 can be used to model complex accidents and radiological consequences to individuals from the release of radionuclides to the atmosphere. A user can generate a fission product inventory; decay and ingrow the inventory during transport through processes, facilities, and the environment; model the downwind dispersion of the activity; and calculate doses to downwind individuals. Doses are calculated through the inhalation, immersion, ground surface and ingestion pathways. New to RSAC-6.2 are the abilitiesmore » to calculate inhalation from release to a room, inhalation from resuspension of activities, and a new model for dry deposition. Doses can now be calculated as close as 10 meters from the release point. RSAC-6.2 has been subjected to extensive independent verification and validation for use in performing safety-related dose calculations to support safety analysis reports. WinRP 2.0, a windows based overlay to RSAC-6.2, assists users in creating and running RSAC-6.2 input files. RSAC-6, Rev. 6.2 (03/11/02) corrects an earlier issue with RSAC-6, compiled with F77L-EM/32 Fortran 77 Version 5.10, which would not allow the executable to run with XP or VISTA Windows operating systems. Because this version is still in use at some facilities, it is being released through RSICC in addition to the new RSAC 7 (CCC-761).« less

  1. System Analysis and Risk Assessment System.

    2000-11-20

    Version 00 SARA4.16 is a program that allows the user to review the results of a Probabilistic Risk Assessment (PRA) and to perform limited sensitivity analysis on these results. This tool is intended to be used by a less technical oriented user and does not require the level of understanding of PRA concepts required by a full PRA analysis tool. With this program a user can review the information generated by a PRA analyst andmore » compare the results to those generated by making limited modifications to the data in the PRA. Also included in this program is the ability to graphically display the information stored in the database. This information includes event trees, fault trees, P&IDs and uncertainty distributions. SARA 4.16 is incorporated in the SAPHIRE 5.0 code package.« less

  2. GROUNDWATER INFORMATION TRACKING SYSTEM/STATISTICAL ANALYSIS SYSTEM

    EPA Science Inventory

    The Groundwater Information Tracking System with STATistical analysis capability (GRITS/STAT) is a tool designed to facilitate the storage, analysis, and reporting of data collected through groundwater monitoring programs at RCRA, CERCLA, and other regulated facilities an...

  3. Actinide crystal-liquid partitioning for clinopyroxene and Ca3/PO4/2

    NASA Technical Reports Server (NTRS)

    Benjamin, T.; Heuser, W. R.; Burnett, D. S.; Seitz, M. G.

    1980-01-01

    Coefficients for the partitioning of the actinide elements Th, U and Pu, which are used as indicators of r-process nucleosynthesis and the ages of meteorite and lunar samples, between diopsidic clinopyroxene, whitlockite and silicate liquid at 20 kbar are measured. Fission and alpha track radiography techniques are employed to detect element concentrations in synthetic crystals made using spiked starting materials, under the assumptions of equilibrium partitioning at the crystal-liquid interface and actinide zoning. Analysis of the data indicates results to be consistent with interface equilibrium except at high cooling rates. Th/U/Pu partition coefficients of about 0.002/0.002/O.06 are measured for clinopyroxene and 1.2/0.5/3.4 for whitlockite. The greater incorporation of Pu into the crystalline phases is attributed to the importance of trivalent Pu, and the similarity of its partition coefficient into clinopyroxene to that of the light rare earths supports the concept of Pu/rare earth dating.

  4. Comparative evaluation of actinide ion uptake by polymer inclusion membranes containing TODGA as the carrier extractant.

    PubMed

    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.

  5. MEDOR, a didactic tool to support interpretation of bioassay data after internal contamination by actinides.

    PubMed

    Mièle, A; Blanchin, N; Raynaud, P; Quesne, B; Giraud, J M; Fottorino, R; Bérard, P; Ansoborlo, E; Franck, D; Blanchardon, E; Challeton-de Vathaire, C; Lebaron-Jacobs, L; Poncy, J L; Piechowski, J; Fritsch, P

    2007-01-01

    A didactic software, MEthodes DOsimètriques de REférence (MEDOR), is being developed to provide help in the interpretation of biological data. Its main purpose is to evaluate the pertinence of the application of different models. This paper describes its first version that is focused on inhalation exposure to actinide aerosols. With this tool, sensitivity analysis on different parameters of the ICRP models can be easily done for aerosol deposition, in terms of activity and particle number, actinide biokinetics and doses. The user can analyse different inhalation cases showing either that dose per unit intake cannot be applied if the aerosol contains a low number of particles or that an inhibition of the late pulmonary clearance by particle transport can occur which contributes to a 3-4 fold increase in effective dose as compared with application of default parameters. This underlines the need to estimate systematically the number of deposited particles, as well as to do chest monitoring as long as possible.

  6. Rapid Separation Methods to Characterize Actinides and Metallic Impurities in Plutonium Scrap Materials at SRS

    SciTech Connect

    Maxwell, S.L. III; Jones, V.D.

    1998-07-01

    The Nuclear Materials Stabilization and Storage Division at SRS plans to stabilize selected plutonium scrap residue materials for long term storage by dissolution processing and plans to stabilize other plutonium vault materials via high-temperature furnace processing. To support these nuclear material stabilization activities, the SRS Analytical Laboratories Department (ALD) will provide characterization of materials required prior to the dissolution or the high-firing of these materials. Lab renovations to install new analytical instrumentation are underway to support these activities that include glove boxes with simulated-process dissolution and high- pressure microwave dissolution capability. Inductively-coupled plasma atomic emission spectrometry (ICP-AES), inductively- coupled mass spectrometry (ICP-MS) and thermal-ionization mass spectrometry (TIMS) will be used to measure actinide isotopics and metallic impurities. New high-speed actinide separation methods have been developed that will be applied to isotopic characterization of nuclear materials by TIMS and ICP-MS to eliminate isobaric interferences between Pu-238 /U- 238 and Pu-241/Am-241. TEVA Resin, UTEVA Resin, and TRU Resin columns will be used with vacuum-assisted flow rates to minimize TIMS and ICP-MS sample turnaround times. For metallic impurity analysis, rapid column removal methods using UTEVA Resin, AGMP-1 anion resin and AG MP-50 cation resin have also been developed to remove plutonium and uranium matrix interferences prior to ICP-AES and ICP- MS measurements.

  7. Laser power conversion system analysis, volume 1

    NASA Technical Reports Server (NTRS)

    Jones, W. S.; Morgan, L. L.; Forsyth, J. B.; Skratt, J. P.

    1979-01-01

    The orbit-to-orbit laser energy conversion system analysis established a mission model of satellites with various orbital parameters and average electrical power requirements ranging from 1 to 300 kW. The system analysis evaluated various conversion techniques, power system deployment parameters, power system electrical supplies and other critical supplies and other critical subsystems relative to various combinations of the mission model. The analysis show that the laser power system would not be competitive with current satellite power systems from weight, cost and development risk standpoints.

  8. Measurement of Actinides in Environmental Samples at Micro-Becquerel Levels by Accelerator Mass Spectrometry

    SciTech Connect

    Brown, T A; Knezovich, J P; Marchetti, A A; Hamilton, T F

    2002-09-03

    The need for ultra-sensitive actinide measurements continues to expand in the fields of environmental stewardship, nuclear isotope forensics, radiobioassay and environmental research. We have developed a heavy isotope accelerator mass spectrometry (AMS) system at Lawrence Livermore National Laboratory's Center for Accelerator Mass Spectrometry (CAMS). The system was designed particularly for the measurement of actinide concentrations and isotopic ratios. A fast isotope switching capability has been incorporated in the system, allowing flexibility in isotope selection and for the quasi-continuous normalization to a reference isotope spike. Initially, our utilization of the system has concentrated on the measurement of Pu isotopes. Under current operating conditions, background levels equivalent to <10{sup 6} atoms are observed during routine {sup 239}Pu and {sup 240}Pu measurements. Measurements of samples containing 10{sup 13} {sup 238}U atoms demonstrate that the system provides a {sup 238}U rejection factor of >10{sup 7}. Recently, we have utilized the high dynamic range of the AMS system in measuring samples whose Pu contents ranged from <10{sup 6} (background) to >10{sup 11} Pu atoms. Measurements of known materials, combined with results from an externally organized intercomparison program, indicate that our {sup 239}Pu measurements are accurate and precise down to the {mu}Bq level ({approx}10{sup 6} atoms). The development of the heavy isotope system was undertaken with particular interest in the measurement of environmental samples, including soils, sediments, waters, air filters, tissue samples, and human urine. The high rejection of interferences, including molecular interferences, and low susceptibility to matrix components, provided by the AMS technique are of particular relevance for such complex samples. These two factors significantly reduce demands on sample preparation chemistry for Pu analyses, allowing relatively simple, cost-effective procedures

  9. Crystalline matrices for immobilization of actinides: Corrosion resistance in water

    NASA Astrophysics Data System (ADS)

    Yudintsev, S. V.; Aleksandrova, E. V.; Livshits, T. S.; Mal'kovskii, V. I.; Bychkova, Ya. V.; Tagirov, B. R.

    2014-10-01

    The rate of leaching of actinide-simulating rare-earth elements from two types of crystalline matrices consisting of titanate and titanozirconate phases was examined. The experiments were carried out at 95°C in distilled water. The rates of REE leaching from the samples were below 10-3 g/m2 day, which satisfied the requirements for the characteristics of matrices for immobilization of actinides. After passing the treated solutions through filters of 450 to 25 nm pore sizes, the REE content was changed slightly or not at all. This fact points to the minor role or to the absence of the colloidal form of REE in the solutions after the experiments.

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

    DOEpatents

    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.

  11. The pentavalent actinide solution chemistry in the environment.

    PubMed

    Topin, Sylvain; Aupiais, Jean

    2016-03-01

    With regard to environmental monitoring of certain nuclear facilities, pentavalent actinides, in particular neptunium and plutonium, play a key role, as the chief soluble, mobile forms of actinides. In the past five years, investigations carried out by hyphenating capillary electrophoresis to ICP-MS (CE-ICP-MS) have allowed a number of hitherto unknown thermodynamic data to be determined for Np(V) and Pu(V) interactions with the chief environmentally abundant anions. For the first time, data were provided for Pu(V) interactions with carbonate, sulfate, oxalate, chloride, and nitrate ions, allowing the Np(V)/Pu(V) analogy to be verified experimentally. Knowledge of Np(V) chemistry, especially in carbonate, and sulfate media, was also refined. These CE-ICP-MS studies, combined with some earlier findings, have brought about a renewal in the knowledge of An(V) chemistry in solution. PMID:26808225

  12. Actinide-specific sequestering agents and decontamination applications

    SciTech Connect

    Smith, William L.; Raymond, Kenneth N.

    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.

  13. Chemistry of the heaviest actinides: fermium, mendelevium, nobelium, and lawrencium

    SciTech Connect

    Hulet, E.K.

    1980-01-01

    The chemical properties of the heavy actinides systematically deviate from those of their lanthanide counterparts. The differences between the later elements of the 4f and 5f series can be generally interpreted on the basis of subtle changes in electronic structure. The most important change is a lowering of the 5f energy levels with respect to the Fermi level and a wider separation between the 5f ground states and the first excited states in the 6d or 7p levels. It was concluded that these shifts toward greater stabilization of 5f orbitals with increasing atomic number are mainly supported by the appearance of the divalent oxidation state well before the end of the actinide series and the predominance of the divalent state in the next to last element in the series. The chemistry of fermium, mendelevium, nobelium, and lawrencium was discussed. 8 figures 4 tables. (DP)

  14. Observation of large scissors resonance strength in actinides.

    PubMed

    Guttormsen, M; Bernstein, L A; Bürger, A; Görgen, A; Gunsing, F; Hagen, T W; Larsen, A C; Renstrøm, T; Siem, S; Wiedeking, M; Wilson, J N

    2012-10-19

    The orbital M1 scissors resonance has been measured for the first time in the quasicontinuum of actinides. Particle-γ coincidences are recorded with deuteron and (3)He-induced reactions on (232)Th. The residual nuclei (231,232,233)Th and (232,233) Pa show an unexpectedly strong integrated strength of B(M1)=11-15μ(n)(2) in the E(γ)=1.0-3.5 MeV region. The increased γ-decay probability in actinides due to scissors resonance is important for cross-section calculations for future fuel cycles of fast nuclear reactors and may also have an impact on stellar nucleosynthesis. PMID:23215072

  15. Actinide solubility and spectroscopic speciation in alkaline Hanford waste solutions

    SciTech Connect

    Rao, L.; Felmy, A.R.; Rai, D.

    1996-10-01

    Information on the solubility and the speciation of actinide elements, especially plutonium and neptunium, in alkaline solutions is of importance in the development of separation techniques for the Hanford tank HLW supernatant. In the present study, experimental data on the solubilities of plutonium in simulated Hanford tank solutions were analyzed with Pitzer`s specific ion-interaction approach, which is applicable in dilute to highly concentrated electrolyte solutions. In order to investigate the formation of actinide species in alkaline solutions with ligands (e.g., hydroxide, aluminate and carbonate), spectroscopic measurements of neptunium (V), as a chemical analog of plutonium (V), were conducted. Based on the solubility data and available information on both solid and aqueous species, a thermodynamic model was proposed. The applicability and limitations of this model are discussed.

  16. Evaluation of Covariances for Actinides and Light Elements at LANL

    SciTech Connect

    Kawano, T. Talou, P.; Young, P.G.; Hale, G.; Chadwick, M.B.; Little, R.C.

    2008-12-15

    Los Alamos evaluates covariances for the evaluated nuclear data library (ENDF), mainly for actinides above the resonance region and for light elements in the entire energy range. We also develop techniques to evaluate the covariance data, like Bayesian and least-squares fitting methods, which are important to explore the uncertainty information on different types of physical quantities such as elastic scattering angular distribution, or prompt neutron fission spectra. This paper summarizes our current activities of the covariance evaluation work at LANL, including the actinide and light element data mainly for criticality safety studies and transmutation technology. The Bayesian method based on the Kalman filter technique, which combines uncertainties in the theoretical model and experimental data, is discussed.

  17. Coupled dynamics analysis of wind energy systems

    NASA Technical Reports Server (NTRS)

    Hoffman, J. A.

    1977-01-01

    A qualitative description of all key elements of a complete wind energy system computer analysis code is presented. The analysis system addresses the coupled dynamics characteristics of wind energy systems, including the interactions of the rotor, tower, nacelle, power train, control system, and electrical network. The coupled dynamics are analyzed in both the frequency and time domain to provide the basic motions and loads data required for design, performance verification and operations analysis activities. Elements of the coupled analysis code were used to design and analyze candidate rotor articulation concepts. Fundamental results and conclusions derived from these studies are presented.

  18. Dynamic Analysis of Nuclear Energy System Strategies

    SciTech Connect

    Den Durpel, Luc Van

    2004-06-17

    DANESS is an integrated process model for nuclear energy systems allowing the simulation of multiple reactors and fuel cycles in a continuously changing nuclear reactor park configuration. The model is energy demand driven and simulates all nuclear fuel cycle facilites, up to 10 reactors and fuels. Reactor and fuel cycle facility history are traced and the cost of generating energy is calculated per reactor and for total nuclear energy system. The DANESS model aims at performing dynamic systems analysis of nuclear energy development used for integrated analysis of development paths for nuclear energy, parameter scoping for new nuclear energy systems, economic analysis of nuclear energy, government role analysis, and education.

  19. Comparative food-chain behavior and distribution of actinide elements in and around a contaminated fresh-water pond

    SciTech Connect

    Garten, C.T. Jr.; Trabalka, J.R.; Bogle, M.A.

    1981-01-01

    The bioaccumulation of /sup 233/ /sup 234/U, /sup 238/U, /sup 238/Pu, /sup 239/ /sup 240/Pu, /sup 241/Am, and /sup 244/Cm in both native and introduced biota was studied at Pond 3513, a former low-level radioactive waste settling basin at Oak Ridge National Laboratory. This system, which was decommissioned in 1976 after more than 30 years use, contains approximately 5 Ci of /sup 239/ /sup 240/Pu; inventories of other actinide isotopes are considerably less. Significantly higher concentrations of actinides in fish that were allowed access to sediments indicated that sedimentary particulates may be the primary source of transuranics to biota in shallow fresh-water ecosystems. Our study determined habitat, in particular the degree of association of an organism with the sediment-water interface, to be the primary factor in controlling transuranic concentrations in aquatic biota. In most of the biological samples analyzed, excluding samples suspected of being contaminated by sediment, /sup 241/Am//sup 239/Pu, /sup 244/Cm//sup 239/Pu, and /sup 238/U//sup 239/Pu ratios were greater than the respective ratio in sediment while /sup 233/ /sup 234/U//sup 238/U, and /sup 239/ /sup 240/Pu//sup 238/Pu ratios were not different from the respective ratios in sediment. The relative uptake of actinides from contaminated sediment by aquatic and terrestrial biota at this site was U > Cm greater than or equal to Am > Pu. The relative extractability of actinides from shoreline sediment was U > Cm approx. = Am > Pu; we also observed the same relative ranking for sediment-water exchange in situ. Concentrations of transuranics in water, terrestrial vegetation, and vertebrate carcasses were less than 10% of the recommended public exposure maximum permissible concentration (MPC) of the ICRP.

  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

    SciTech Connect

    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.