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Sample records for actinide waste isotopes

  1. A Heterogeneous Sodium Fast Reactor Designed to Transmute Minor Actinide Actinide Waste Isotopes into Plutonium Fuel

    SciTech Connect

    Samuel E. Bays

    2011-02-01

    An axial heterogeneous sodium fast reactor design is developed for converting minor actinide waste isotopes into plutonium fuel. The reactor design incorporates zirconium hydride moderating rods in an axial blanket above the active core. The blanket design traps the active core’s axial leakage for the purpose of transmuting Am-241 into Pu-238. This Pu-238 is then co-recycled with the spent driver fuel to make new driver fuel. Because Pu-238 is significantly more fissile than Am-241 in a fast neutron spectrum, the fissile worth of the initial minor actinide material is upgraded by its preconditioning via transmutation in the axial targets. Because, the Am-241 neutron capture worth is significantly stronger in a moderated epithermal spectrum than the fast spectrum, the axial targets serve as a neutron trap which recovers the axial leakage lost by the active core. The sodium fast reactor proposed by this work is designed as an overall transuranic burner. Therefore, a low transuranic conversion ratio is achieved by a degree of core flattening which increases axial leakage. Unlike a traditional “pancake” design, neutron leakage is recovered by the axial target/blanket system. This heterogeneous core design is constrained to have sodium void and Doppler reactivity worth similar to that of an equivalent homogeneous design. Because minor actinides are irradiated only once in the axial target region; elemental partitioning is not required. This fact enables the use of metal targets with electrochemical reprocessing. Therefore, the irradiation environment of both drivers and targets was constrained to ensure applicability of the established experience database for metal alloy sodium fast reactor fuels.

  2. Nuclear waste forms for actinides.

    PubMed

    Ewing, R C

    1999-03-30

    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.

  3. 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

  4. Actinide Isotopes for the Synthesis of Superheavy Nuclei

    NASA Astrophysics Data System (ADS)

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

    2014-09-01

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

  5. Actinide removal from nitric acid waste streams

    SciTech Connect

    Muscatello, A.C.; Navratil, J.D.

    1986-01-01

    Actinide separations research at the Rocky Flats Plant (RFP) has found ways to significantly improve plutonium secondary recovery and americium removal from nitric acid waste streams generated by plutonium purification operations. Capacity and breakthrough studies show anion exchange with Dowex 1x4 (50 to 100 mesh) to be superior for secondary recovery of plutonium. Extraction chromatography with TOPO(tri-n-octyl-phosphine oxide) on XAD-4 removes the final traces of plutonium, including hydrolytic polymer. Partial neutralization and solid supported liquid membrane transfer removes americium for sorption on discardable inorganic ion exchangers, potentially allowing for non-TRU waste disposal.

  6. MICROBIAL TRANSFORMATIONS OF PLUTONIUM AND OTHER ACTINIDES IN TRANSURANIC AND MIXED WASTES.

    SciTech Connect

    FRANCIS,A.J.

    2003-07-06

    The presence of the actinides Th, U, Np, Pu, and Am in transuranic (TRU) and mixed wastes is a major concern because of their potential for migration from the waste repositories and long-term contamination of the environment. The toxicity of the actinide elements and the long half-lives of their isotopes are the primary causes for concern. In addition to the radionuclides the TRU waste consists a variety of organic materials (cellulose, plastic, rubber, chelating agents) and inorganic compounds (nitrate and sulfate). Significant microbial activity is expected in the waste because of the presence of organic compounds and nitrate, which serve as carbon and nitrogen sources and in the absence of oxygen the microbes can use nitrate and sulfate as alternate electron acceptors. Biodegradation of the TRU waste can result in gas generation and pressurization of containment areas, and waste volume reduction and subsidence in the repository. Although the physical, chemical, and geochemical processes affecting dissolution, precipitation, and mobilization of actinides have been investigated, we have only limited information on the effects of microbial processes. Microbial activity could affect the chemical nature of the actinides by altering the speciation, solubility and sorption properties and thus could increase or decrease the concentrations of actinides in solution. Under appropriate conditions, dissolution or immobilization of actinides is brought about by direct enzymatic or indirect non-enzymatic actions of microorganisms. Dissolution of actinides by microorganisms is brought about by changes in the Eh and pH of the medium, by their production of organic acids, such as citric acid, siderophores and extracellular metabolites. Immobilization or precipitation of actinides is due to changes in the Eh of the environment, enzymatic reductive precipitation (reduction from higher to lower oxidation state), biosorption, bioaccumulation, biotransformation of actinides complexed

  7. 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.

  8. Plutonium Futures -- The Science. Topical Conference on Plutonium and Actinides. AIP Conference Proceedings, No. 532 [APCPCS

    SciTech Connect

    Pillay, K.K.S.; Kim, K.C.

    2000-12-31

    Presentations at this conference covered the topics of materials science/nuclear fuels, condensed matter physics, actinides in the environment/separation and analysis, actinides/processing, actinides/TRU wastes, materials science, TRU waste forms, nuclear fuels/isotopes, separations and process chemistry, actinides in the environment, detection and analysis, Pu and Pu compounds, actinide compounds and complexes.

  9. The Most Useful Actinide Isotope: Americium-241.

    ERIC Educational Resources Information Center

    Navratil, James D.; And Others

    1990-01-01

    Reviewed is the discovery, nuclear and chemical properties, and uses of an isotope of Americium (Am-241). Production and separation techniques used in industry are emphasized. Processes are illustrated in flow sheets. (CW)

  10. Actinide removal from wastewater applying waste minimization techniques

    SciTech Connect

    Covey, J.R.; Midkiff, W.S. ); Cadena, F. )

    1992-01-01

    A major concern at LANL is the large volume of low level radioactive sludge that is generated by the current treatment technology. The plant meets current discharge limits but annually produces 200 55-gallon drums of sludge (approximately 60 tons) during the process of removing only few grants of radioactive isotopes. Most of the sludge results from the coagulants, iron and lime, added at the plant at a concentration of 10,000 parts-per-million (ppm). If the principal actinides in the influent could be separated and reduced to pure metallic form, the annual volume of plutonium would be about the size of a marble and the americium would be about the size of a BB. Waste minimization will be a key design criteria for the new facility. Records of total suspended solids (TSS) in the influent average about 1000 Kg per year (approximately 1 ton). Therefore, the theoretical sludge volume reduction is near 98%. Research is underway to develop and evaluate technologies that achieve the desired removal efficiency with a minimum of produced waste volume.

  11. Actinide removal from wastewater applying waste minimization techniques

    SciTech Connect

    Covey, J.R.; Midkiff, W.S.; Cadena, F.

    1992-07-01

    A major concern at LANL is the large volume of low level radioactive sludge that is generated by the current treatment technology. The plant meets current discharge limits but annually produces 200 55-gallon drums of sludge (approximately 60 tons) during the process of removing only few grants of radioactive isotopes. Most of the sludge results from the coagulants, iron and lime, added at the plant at a concentration of 10,000 parts-per-million (ppm). If the principal actinides in the influent could be separated and reduced to pure metallic form, the annual volume of plutonium would be about the size of a marble and the americium would be about the size of a BB. Waste minimization will be a key design criteria for the new facility. Records of total suspended solids (TSS) in the influent average about 1000 Kg per year (approximately 1 ton). Therefore, the theoretical sludge volume reduction is near 98%. Research is underway to develop and evaluate technologies that achieve the desired removal efficiency with a minimum of produced waste volume.

  12. Removal of actinides from nuclear reprocessing wastes: a pilot plant study using non-radioactive simulants

    SciTech Connect

    Maxey, H.R.; McIsaac, L.D.; Chamberlain, D.B.; McManus, G.J.

    1980-01-01

    Nuclear fuel reprocessing wastes generated at the ICPP contain small amounts of actinides, primarily Pu and Am. Removal of these actinides reduces the long term storage hazards of the waste. The development of a flowsheet to remove trivalent actinides is discussed in this paper. Pilot plant studies used actinide simulants. As a result of these studies, the Height of a Transfer Unit (HTU) was selected as the better measure of pulse column separation efficiency.

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

    PubMed

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

    2004-01-01

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

  14. Literature review of United States utilities computer codes for calculating actinide isotope content in irradiated fuel

    SciTech Connect

    Horak, W.C.; Lu, Ming-Shih

    1991-12-01

    This paper reviews the accuracy and precision of methods used by United States electric utilities to determine the actinide isotopic and element content of irradiated fuel. After an extensive literature search, three key code suites were selected for review. Two suites of computer codes, CASMO and ARMP, are used for reactor physics calculations; the ORIGEN code is used for spent fuel calculations. They are also the most widely used codes in the nuclear industry throughout the world. Although none of these codes calculate actinide isotopics as their primary variables intended for safeguards applications, accurate calculation of actinide isotopic content is necessary to fulfill their function.

  15. 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.

  16. Effects of actinide burning on waste disposal at Yucca Mountain

    SciTech Connect

    Hirschfelder, J.

    1992-07-01

    Release rates of 15 radionuclides from waste packages expected to result from partitioning and transmutation of Light-Water Reactor (LWR) and Actinide-Burning Liquid-Metal Reactor (ALMR) spent fuel are calculated and compared to release rates from standard LWR spent fuel packages. The release rates are input to a model for radionuclide transport from the proposed geologic repository at Yucca Mountain to the water table. Discharge rates at the water table are calculated and used in a model for transport to the accessible environment, defined to be five kilometers from the repository edge. Concentrations and dose rates at the accessible environment from spent fuel and wastes from reprocessing, with partitioning and transmutation, are calculated. Partitioning and transmutation of LWR and ALMR spent fuel reduces the inventories of uranium, neptunium, plutonium, americium and curium in the high-level waste by factors of 40 to 500. However, because release rates of all of the actinides except curium are limited by solubility and are independent of package inventory, they are not reduced correspondingly. Only for curium is the repository release rate much lower for reprocessing wastes.

  17. Disposition of actinides released from high-level waste glass

    SciTech Connect

    Ebert, W.L.; Bates, J.K.; Buck, E.C.; Gong, M.; Wolf, S.F.

    1994-05-01

    A series of static leach tests was conducted using glasses developed for vitrifying tank wastes at the Savannah River Site to monitor the disposition of actinide elements upon corrosion of the glasses. In these tests, glasses produced from SRL 131 and SRL 202 frits were corroded at 90{degrees}C in a tuff groundwater. Tests were conducted using crushed glass at different glass surface area-to-solution volume (S/V) ratios to assess the effect of the S/V on the solution chemistry, the corrosion of the glass, and the disposition of actinide elements. Observations regarding the effects of the S/V on the solution chemistry and the corrosion of the glass matrix have been reported previously. This paper highlights the solution analyses performed to assess how the S/V used in a static leach test affects the disposition of actinide elements between fractions that are suspended or dissolved in the solution, and retained by the altered glass or other materials.

  18. Strontium and Actinide Separations from High Level Nuclear Waste Solutions using Monosodium Titanate - Actual Waste Testing

    SciTech Connect

    Peters, T.B.; Barnes, M.J.; Hobbs,D.T.; Walker, D.D.; Fondeur, F.F.; Norato, M.A.; Pulmano, R.L.; Fink, S.D.

    2005-11-01

    Pretreatment processes at the Savannah River Site will separate {sup 90}Sr, alpha-emitting and radionuclides (i.e., actinides) and {sup 137}Cs prior to disposal of the high-level nuclear waste. Separation of {sup 90}Sr and alpha-emitting radionuclides occurs by ion exchange/adsorption using an inorganic material, monosodium titanate (MST). Previously reported testing with simulants indicates that the MST exhibits high selectivity for strontium and actinides in high ionic strength and strongly alkaline salt solutions. This paper provides a summary of data acquired to measure the performance of MST to remove strontium and actinides from actual waste solutions. These tests evaluated the effects of ionic strength, mixing, elevated alpha activities, and multiple contacts of the waste with MST. Tests also provided confirmation that MST performs well at much larger laboratory scales (300-700 times larger) and exhibits little affinity for desorption of strontium and plutonium during washing.

  19. Literature review of intrinsic actinide colloids related to spent fuel waste package release rates

    SciTech Connect

    Zhao, P.; Steward, S.A.

    1997-01-01

    Existence of actinide colloids provides an important mechanism in the migration of radionuclides and will be important in performance of a geologic repository for high-level nuclear waste. Actinide colloids have been formed during long-term unsaturated dissolution of spent fuel by groundwater. This article summarizes a literature search of actinide colloids. This report emphasizes the formation of intrinsic actinide colloids, because they would have the opportunity to form soon after groundwater contact with the spent fuel and before actinide-bearing groundwater reaches the surrounding geologic formations.

  20. 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.

  1. MICROBIAL TRANSFORMATIONS OF TRU AND MIXED WASTES: ACTINIDE SPECIATION AND WASTE VOLUME REDUCTION.

    SciTech Connect

    FRANCIS, A.J.; DODGE, C.J.

    2006-11-16

    The overall goals of this research project are to determine the mechanism of microbial dissolution and stabilization of actinides in Department of Energy's (DOE) TRU wastes, contaminated sludges, soils, and sediments. This includes (1) investigations on the fundamental aspects of microbially catalyzed radionuclide and metal transformations (oxidation/reduction reactions, dissolution, precipitation, chelation); (2) understanding of the microbiological processes that control speciation and alter the chemical forms of complex inorganic/organic contaminant mixtures; and (3) development of new and improved microbially catalyzed processes resulting in immobilization of metals and radionuclides in the waste with concomitant waste volume reduction.

  2. MICROBIAL TRANSFORMATIONS OF TRU AND MIXED WASTES: ACTINIDE SPECIATION AND WASTE VOLUME REDUCTION

    SciTech Connect

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

    2006-06-01

    The overall goals of this research project are to determine the mechanism of microbial dissolution and stabilization of actinides in Department of Energy’s (DOE) TRU wastes, contaminated sludges, soils, and sediments. This includes (i) investigations on the fundamental aspects of microbially catalyzed radionuclide and metal transformations (oxidation/reduction reactions, dissolution, precipitation, chelation); (ii) understanding of the microbiological processes that control speciation and alter the chemical forms of complex inorganic/organic contaminant mixtures; and (iii) development of new and improved microbially catalyzed processes resulting in immobilization of metals and radionuclides in the waste with concomitant waste volume reduction.

  3. MICROBIAL TRANSFORMATIONS OF TRU AND MIXED WASTES: ACTINIDE SPECIATION AND WASTE VOLUME REDUCTION

    SciTech Connect

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

    2006-06-01

    The overall goals of this research project are to determine the mechanism of microbial dissolution and stabilization of actinides in Department of Energy's (DOE) TRU wastes, contaminated sludges, soils, and sediments. This includes (1) investigations on the fundamental aspects of microbially catalyzed radionuclide and metal transformations (oxidation/reduction reactions, dissolution, precipitation, chelation); (2) understanding of the microbiological processes that control speciation and alter the chemical forms of complex inorganic/organic contaminant mixtures; and (3) development of new and improved microbially catalyzed processes resulting in immobilization of metals and radionuclides in the waste with concomitant waste volume reduction.

  4. 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.

  5. Evaluation of different solvent extraction methods for removing actinides from high acid waste streams

    SciTech Connect

    Yarbro, S.L.; Schreiber, S.B.; Dunn, S.L. ); Rogers, J. )

    1991-01-01

    At the Los Alamos National Laboratory Plutonium Facility, anion exchange is used to recover plutonium from nitric acid solutions. Although this approach recovers >99%, trace amounts of plutonium and other actinides remain the effluent and require additional processing. Currently, a ferric hydroxide carrier precipitation is used to remove the trace actinides and the resulting sludge is cemented. Because it costs approximately $10,000 per drum for disposal, we are developing an additional polishing step so that the effluent actinide levels are reduced to below 100 nCi/g. This would allow the resulting waste sludge to disposed as low-level waste at approximately $200 per drum. We are investigating various solvent extraction techniques for removing actinides. The most promising are chelating resins and membrane-based liquid-liquid solvent extraction. This report details some of our preliminary results. 4 refs., 3 tabs.

  6. Health and environmental risk-related impacts of actinide burning on high-level waste disposal

    SciTech Connect

    Forsberg, C.W.

    1992-05-01

    The potential health and environmental risk-related impacts of actinide burning for high-level waste disposal were evaluated. Actinide burning, also called waste partitioning-transmutation, is an advanced method for radioactive waste management based on the idea of destroying the most toxic components in the waste. It consists of two steps: (1) selective removal of the most toxic radionuclides from high-level/spent fuel waste and (2) conversion of those radionuclides into less toxic radioactive materials and/or stable elements. Risk, as used in this report, is defined as the probability of a failure times its consequence. Actinide burning has two potential health and environmental impacts on waste management. Risks and the magnitude of high-consequence repository failure scenarios are decreased by inventory reduction of the long-term radioactivity in the repository. (What does not exist cannot create risk or uncertainty.) Risk may also be reduced by the changes in the waste characteristics, resulting from selection of waste forms after processing, that are superior to spent fuel and which lower the potential of transport of radionuclides from waste form to accessible environment. There are no negative health or environmental impacts to the repository from actinide burning; however, there may be such impacts elsewhere in the fuel cycle.

  7. Chemical Speciation of Americium, Curium and Selected Tetravalent Actinides in High Level Waste

    SciTech Connect

    Felmy, Andrew R.

    2006-06-01

    Large volumes of high-level waste (HLW) currently stored in tanks at DOE sites contain both sludges and supernatants. The sludges are composed of insoluble precipitates of actinides, radioactive fission products, and nonradioactive components. The supernatants are alkaline carbonate solutions, which can contain soluble actinides, fission products, metal ions, and high concentrations of major electrolytes including sodium hydroxide, nitrate, nitrite, phosphate, carbonate, aluminate, sulfate, and organic complexants. The organic complexants include several compounds that can form strong aqueous complexes with actinide species and fission products including ethylenediaminetetraacetic acid (EDTA), N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA), nitrilotriacetic acid (NTA), iminodiacetic acid (IDA), citrate, glycolate, gluconate, and degradation products, formate and oxalate.

  8. Chemical Speciation of Americium, Curium and Selected Tetravalent Actinides in High Level Waste

    SciTech Connect

    Felmy, Andrew R.

    2005-06-01

    Large volumes of high-level waste (HLW) currently stored in tanks at DOE sites contain both sludges and supernatants. The sludges are composed of insoluble precipitates of actinides, radioactive fission products, and nonradioactive components. The supernatants are alkaline carbonate solutions, which can contain soluble actinides, fission products, metal ions, and high concentrations of major electrolytes including sodium hydroxide, nitrate, nitrite, phosphate, carbonate, aluminate, sulfate, and organic complexants. The organic complexants include several compounds that can form strong aqueous complexes with actinide species and fission products including ethylenediaminetetraacetic acid (EDTA), N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA), nitrilotriacetic acid (NTA), iminodiacetic acid (IDA), citrate, glycolate, gluconate, and degradation products, formate and oxalate.

  9. Assessment of actinide mass embedded in large concrete waste packages by photon interrogation and photofission.

    PubMed

    Gmar, M; Jeanneau, F; Lainé, F; Makil, H; Poumarède, B; Tola, F

    2005-01-01

    This paper describes a method based on photofission developed in our laboratory to characterize in depth large waste packages. The method consists in using photons of high-energy (Bremsstrahlung radiation) in order to induce reactions of photofission on the heavy nuclei present in the wastes. The measurement of the delayed neutrons allows quantifying the actinides in the wastes. We present the first results of measurement performed with a concrete mock-up of 870l and two real waste packages.

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

    SciTech Connect

    Halada, Gary P

    2008-04-10

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

  11. Technical requirements for the actinide source-term waste test program

    SciTech Connect

    Phillips, M.L.F.; Molecke, M.A.

    1993-10-01

    This document defines the technical requirements for a test program designed to measure time-dependent concentrations of actinide elements from contact-handled transuranic (CH TRU) waste immersed in brines similar to those found in the underground workings of the Waste Isolation Pilot Plant (WIPP). This test program wig determine the influences of TRU waste constituents on the concentrations of dissolved and suspended actinides relevant to the performance of the WIPP. These influences (which include pH, Eh, complexing agents, sorbent phases, and colloidal particles) can affect solubilities and colloidal mobilization of actinides. The test concept involves fully inundating several TRU waste types with simulated WIPP brines in sealed containers and monitoring the concentrations of actinide species in the leachate as a function of time. The results from this program will be used to test numeric models of actinide concentrations derived from laboratory studies. The model is required for WIPP performance assessment with respect to the Environmental Protection Agency`s 40 CFR Part 191B.

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

    SciTech Connect

    Nash, Kenneth L.

    2008-11-20

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

  13. Mechanical environmental transport of actinides and ¹³⁷Cs from an arid radioactive waste disposal site.

    PubMed

    Snow, Mathew S; Clark, Sue B; Morrison, Samuel S; Watrous, Matthew G; Olson, John E; Snyder, Darin C

    2015-10-01

    Aeolian and pluvial processes represent important mechanisms for the movement of actinides and fission products at the Earth's surface. Soil samples taken in the early 1970's near a Department of Energy radioactive waste disposal site (the Subsurface Disposal Area, SDA, located in southeastern Idaho) provide a case study for studying the mechanisms and characteristics of environmental actinide and (137)Cs transport in an arid environment. Multi-component mixing models suggest actinide contamination within 2.5 km of the SDA can be described by mixing between 2 distinct SDA end members and regional nuclear weapons fallout. The absence of chemical fractionation between (241)Am and (239+240)Pu with depth for samples beyond the northeastern corner and lack of (241)Am in-growth over time (due to (241)Pu decay) suggest mechanical transport and mixing of discrete contaminated particles under arid conditions. Occasional samples northeast of the SDA (the direction of the prevailing winds) contain anomalously high concentrations of Pu with (240)Pu/(239)Pu isotopic ratios statistically identical to those in the northeastern corner. Taken together, these data suggest flooding resulted in mechanical transport of contaminated particles into the area between the SDA and a flood containment dike in the northeastern corner, following which subsequent contamination spreading in the northeastern direction resulted from wind transport of discrete particles.

  14. 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.

  15. 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.

  16. Chemical Speciation of Americium, Curium and Selected Tetravalent Actinides in High Level Waste

    SciTech Connect

    Felmy, Andrew R.

    2004-06-01

    Large volumes of high-level waste (HLW) currently stored in tanks at DOE sites contain both sludges and supernatants. The sludges are composed of insoluble precipitates of actinides, radioactive fission products, and nonradioactive components. The supernatants are alkaline carbonate solutions, which can contain soluble actinides, fission products, metal ions, and high concentrations of major electrolytes including sodium hydroxide, nitrate, nitrite, phosphate, carbonate, aluminate, sulfate, and organic complexants. The organic complexants include several compounds that can form strong aqueous complexes with actinide species and fission products including ethylenediaminetetraacetic acid (EDTA), N-(2-hydroxyethyl)ethylenediaminetriacetic acid (HEDTA), nitrilotriacetic acid (NTA), iminodiacetic acid (IDA), citrate, glycolate, gluconate, and degradation products, formate and oxalate. The goal of this project is to determine the effects of hydrolysis, carbonate complexation, and metal ion displacement on trivalent and selected tetravalent actinide speciation in the presence of organic chelates present in tank waste and to use these data to develop accurate predictive thermodynamic models for use in chemical engineering applications at Hanford and other DOE sites.

  17. ENHANCED CHEMICAL CLEANING OF SRS WASTE TANKS TO IMPROVE ACTINIDE SOLUBILITY

    SciTech Connect

    Rudisill, T.; Thompson, M.

    2011-09-20

    Processes for the removal of residual sludge from SRS waste tanks have historically used solutions containing up to 0.9 M oxalic acid to dissolve the remaining material following sludge removal. The selection of this process was based on a comparison of a number of studies performed to evaluate the dissolution of residual sludge. In contrast, the dissolution of the actinide mass, which represents a very small fraction of the waste, has not been extensively studied. The Pu, Np, and Am in the sludge is reported to be present as hydrated and crystalline oxides. To identify aqueous solutions which have the potential to increase the solubility of the actinides, the alkaline and mildly acidic test solutions shown below were selected as candidates for use in a series of solubility experiments. The efficiency of the solutions in solubilizing the actinides was evaluated using a simulated sludge prepared by neutralizing a HNO{sub 3} solution containing Pu, Np, and Am. The hydroxide concentration was adjusted to a 1.2 M excess and the solids were allowed to age for several weeks prior to starting the experiments. The sludge was washed with 0.01 M NaOH to prepare the solids for use. Following the addition of an equal portion of the solids to each test solution, the concentrations of Pu, Np, and Am were measured as a function of time over a 792 h (33 day) period to provide a direct comparison of the efficiency of each solution in solubilizing the actinide elements. Although the composition of the sludge was limited to the hydrated actinide oxides (and did not contain other components of demonstrated importance), the results of the study provides guidance for the selection of solutions which should be evaluated in subsequent tests with a more realistic surrogate sludge and actual tank waste.

  18. Measurement of actinides and strontium-90 in high activity waste

    SciTech Connect

    Maxwell, S.L. III; Nelson, M.R.

    1994-08-01

    The reliable measurement of trace radionuclides in high activity waste is important to support waste processing activities at SRS (F and H Area Waste Tanks, Extended Sludge Processing (ESP) and In-Tank precipitation (ITP) processing). Separation techniques are needed to remove high levels of gamma activity and alpha/beta interferences prior to analytical measurement. Using new extraction chromatographic resins from EiChrom Industries, Inc., the SRS Central Laboratory has developed new high speed separation methods that enable measurement of neptunium, thorium, uranium, plutonium, americium and strontium-90 in high activity waste solutions. Small particle size resin and applied vacuum are used to reduce analysis times and enhance column performance. Extraction chromatographic resins are easy to use and eliminate the generation of contaminated liquid organic waste.

  19. Conjugates of magnetic nanoparticle-actinide specific chelator for radioactive waste separation.

    PubMed

    Kaur, Maninder; Zhang, Huijin; Martin, Leigh; Todd, Terry; Qiang, You

    2013-01-01

    A novel nanotechnology for the separation of radioactive waste that uses magnetic nanoparticles (MNPs) conjugated with actinide specific chelators (MNP-Che) is reviewed with a focus on design and process development. The MNP-Che separation process is an effective way of separating heat generating minor actinides (Np, Am, Cm) from spent nuclear fuel solution to reduce the radiological hazard. It utilizes coated MNPs to selectively adsorb the contaminants onto their surfaces, after which the loaded particles are collected using a magnetic field. The MNP-Che conjugates can be recycled by stripping contaminates into a separate, smaller volume of solution, and then become the final waste form for disposal after reusing number of times. Due to the highly selective chelators, this remediation method could be both simple and versatile while allowing the valuable actinides to be recovered and recycled. Key issues standing in the way of large-scale application are stability of the conjugates and their dispersion in solution to maintain their unique properties, especially large surface area, of MNPs. With substantial research progress made on MNPs and their surface functionalization, as well as development of environmentally benign chelators, this method could become very flexible and cost-effective for recycling used fuel. Finally, the development of this nanotechnology is summarized and its future direction is discussed.

  20. Fundamental Thermodynamics of Actinide-Bearing Mineral Waste Forms - Final Report

    SciTech Connect

    Williamson, Mark A.; Ebbinghaus, Bartley B.; Navrotsky, Alexandra

    2001-03-01

    The end of the Cold War raised the need for the technical community to be concerned with the disposition of excess nuclear weapon material. The plutonium will either be converted into mixed-oxide fuel for use in nuclear reactors or immobilized in glass or ceramic waste forms and placed in a repository. The stability and behavior of plutonium in the ceramic materials as well as the phase behavior and stability of the ceramic material in the environment is not well established. In order to provide technically sound solutions to these issues, thermodynamic data are essential in developing an understanding of the chemistry and phase equilibria of the actinide-bearing mineral waste form materials proposed as immobilization matrices. Mineral materials of interest include zircon, zirconolite, and pyrochlore. High temperature solution calorimetry is one of the most powerful techniques, sometimes the only technique, for providing the fundamental thermodynamic data needed to establish optimum material fabrication parameters, and more importantly understand and predict the behavior of the mineral materials in the environment. The purpose of this project is to experimentally determine the enthalpy of formation of actinide orthosilicates, the enthalpies of formation of actinide substituted zirconolite and pyrochlore, and develop an understanding of the bonding characteristics and stabilities of these materials.

  1. Fundamental thermodynamics of actinide-bearing mineral waste forms.

    SciTech Connect

    Gallegos, U. F.; Putnam, R. L.

    2002-01-01

    This report summarizes work after completion of a three-year project and our current ongoing efforts. Research efforts at UC Davis have focused on establishing the thermodynamic properties of zirconolite and pyrochlore, and the synthesis of other minerals relevant to storage of nuclear material. Heat capacity, entropy, enthalpy of formation, and fkee energy of formation data were established for zirconolite, CaZrTi{sub 2}O{sub 7}, in the range from 0 to 1500 K. The heat capacity, entropy, enthalpy of formation, and free energy of formation at 298 K for zirconolite are 211.9 J/K mol, 193.3 J/K mol, -3713.8 kJ/mol, and -35 14.6 kJ/mol, respectively. Solution calorimetry experiments with cerium pyrochlore, Ca{sub 0.8}Ce{sub 1.2}Ti{sub 2}O{sub 7}, are complete. Heat capacity data and confirmation of the pyrochlore composition are required for final data analysis. Synthesis and characterization of CaHfTi{sub 2}O{sub 7}, CaZr{sub 0.5}Hf{sub 0.5}Ti{sub 2}O{sub 7}, Gd{sub 2}Ti{sub 2}O{sub 7}, and CeTi{sub 2}O{sub 6} is complete. Research efforts at Los Alamos have focused on establishing synthesis techniques for actinide-bearing minerals and preparation of the calorimetry laboratory. The preparation of Pu-pyrochlore, nominally CaPuTi{sub 2}O{sub 7} has been achieved by Ebbinghaus at Lawrence Livermore National Laboratory. A sample of this material has been sent to Putnam at Los Alamos National Laboratory.

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

    NASA Astrophysics Data System (ADS)

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

    2010-04-01

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

  3. Neutron-Induced Fission Cross Section Measurements for Uranium Isotopes and Other Actinides at LANSCE

    SciTech Connect

    Laptev, Alexander B.; Tovesson, Fredrik K.; Hill, Tony S.

    2012-08-16

    A well established program of neutron-induced fission cross section measurement at Los Alamos Neutron Science Center (LANSCE) is supporting the Fuel Cycle Research program (FC R&D). The incident neutron energy range spans from sub-thermal up to 200 MeV by combining two LANSCE facilities, the Lujan Center and the Weapons Neutron Research center (WNR). The time-of-flight method is implemented to measure the incident neutron energy. A parallel-plate fission ionization chamber was used as a fission fragment detector. The event rate ratio between the investigated foil and a standard {sup 235}U foil is translated into a fission cross section ratio. Thin actinide targets with deposits of <200 {micro}g/cm{sup 2} on stainless steel backing were loaded into a fission chamber. In addition to previously measured data for {sup 237}Np, {sup 239-242}Pu, {sup 243}Am, new measurements include the recently completed {sup 233,238}U isotopes, {sup 236}U data which is being analyzed, and {sup 234}U data acquired in the 2011-2012 LANSCE run cycle. The new data complete the full suite of Uranium isotopes which were investigated with this experimental approach. When analysis of the new measured data is completed, data will be delivered to evaluators. Having data for multiple Uranium isotopes will support theoretical modeling capabilities and strengthens nuclear data evaluation.

  4. A comparision of TRUEX and CMP solvent extraction processes for actinide removal from ICPP wastes

    SciTech Connect

    Herbst, R.S.; Brewer, K.N.; Garn, T.G.; Law, J.D.

    1996-04-01

    The Idaho Chemical Processing Plant (ICPP) is currently engaged in development efforts for the decontamination of high-level radioactive wastes generated from decades of nuclear fuel reprocessing. These wastes include several types of calcine, generated by high temperature solidification of reprocessing raffinates. In addition to calcine, there are smaller quantities of secondary wastes from decontamination and solvent wash activities which are typically referred to as sodium-bearing waste (SBW). Solvent extraction technologies based on octyl(phenyl)-N,N-diisobutyl-carbamoylmethylphosphine oxide (CMPO, the active extractant in the TRUEX process) and dihexyl-N,N-diethylcarbamoylmethylphosphonate (DHDECMP, the active extractant in the CMP process) are being evaluated for actinide partitioning from these waste streams. Calcines must first be dissolved in an appropriate acidic solution prior to treatment in solvent extraction based processes. The SBW is currently stored as an acidic solution and readily amenable to liquid extraction techniques. Development efforts to date have revolved around defining and refining baseline flowsheets with the TRUEX and CMP processes for each waste stream. Another objective of this work was to determine which of these technologies are best suited for the treatment of ICPP wastes. Laboratory batch contacts were performed to identify relevant chemistry and distribution coefficients. This information was then used to establish baseline flowsheet configuration with regard to chemistry. The laboratory data were used to model the behavior of the actinides and other constituents in the wastes in countercurrent, continuous processes based on centrifugal contactor technology. The laboratory data and modelling results form the basis for comparison of the two processes.

  5. Actinide chemistry research supporting the Waste Isolation Pilot Plant (WIPP): FY94 results

    SciTech Connect

    Novak, C.F.

    1995-08-01

    This document contains six reports on actinide chemistry research supporting the Waste Isolation Pilot Plant (WIPP). These reports, completed in FY94, are relevant to the estimation of the potential dissolved actinide concentrations in WIPP brines under repository breach scenarios. Estimates of potential dissolved actinide concentrations are necessary for WIPP performance assessment calculations. The specific topics covered within this document are: the complexation of oxalate with Th(IV) and U(VI); the stability of Pu(VI) in one WIPP-specific brine environment both with and without carbonate present; the solubility of Nd(III) in a WIPP Salado brine surrogate as a function of hydrogen ion concentration; the steady-state dissolved plutonium concentrations in a synthetic WIPP Culebra brine surrogate; the development of a model for Nd(III) solubility and speciation in dilute to concentrated sodium carbonate and sodium bicarbonate solutions; and the development of a model for Np(V) solubility and speciation in dilute to concentrated sodium Perchlorate, sodium carbonate, and sodium chloride media.

  6. Ageing of a phosphate ceramic used to immobilize chloride contaminated actinide waste

    SciTech Connect

    Metcalfe, Brian L.; Donald, Ian W.; Fong, Shirley K.; Gerrard, Lee A.; Strachan, Denis M.; Scheele, Randall D.

    2009-03-31

    AWE has developed a process for the immobilization of ILW waste containing a significant quantity of chloride using Ca3(PO4)2 as the host material. Waste ions are incorporated into two phosphate based phases, chlorapatite, Ca5(PO4)3Cl, and spodiosite, Ca2(PO4)Cl. Non-active trials performed at AWE using samarium as the actinide surrogate demonstrated the durability of these phases in aqueous solution. Trials of the process using actinide-doped material were performed at PNNL which confirmed the immobilized wasteform resistant to aqueous leaching. Initial leach trials conducted on 239Pu /241Am loaded ceramic at 40°C/28 days gave normalized mass losses of 1.2 x 10-5 g.m-2 and 2.7 x 10-3 g.m-2 for Pu and Cl respectively. In order to assess the response of the phases to radiation-induced damage, accelerated ageing trials were performed on samples in which the 239Pu was replaced by 238Pu. No changes to the crystalline structure of the waste were detected using XRD after the samples had experienced a radiation dose of 4 x 1018 α.g-1. Leach trials showed that there had been an increase in the P and Ca release rates but no change in the Pu release rate.

  7. Mechanical environmental transport of actinides and ¹³⁷Cs from an arid radioactive waste disposal site

    DOE PAGES

    Snow, Mathew S.; Clark, Sue B.; Morrison, Samuel S.; ...

    2015-10-01

    Particulate transport represents an important mechanism for actinides and fission products at the Earth's surface; soil samples taken in the early 1970's near the Subsurface Disposal Area (SDA) at Idaho National Laboratory (INL) provide a case study for examining the mechanisms and characteristics of actinide transport under arid conditions. Transuranic waste was disposed via shallow land burial at the SDA until shortly after a flooding event that occurred in 1969. In this study we analyze soils collected in the early 1970's for ¹³⁷Cs, ²⁴¹Am, and Pu using a combination of radiometric and mass spectrometric techniques. Two distinct ²⁴⁰Pu/²³⁹Pu isotopic ratiosmore » are observed for contamination from the SDA, with values ranging from at least 0.059 to 0.069. ²⁴¹Am concentrations are observed to increase only slightly in 0-4 cm soils over the ~40 year period since soil sampling, contrary to Markham's previous hypothesis that ²⁴¹Pu is principally associated with the 0-4 cm soil fractions (Markham 1978). The lack of statistical difference in ²⁴¹Am/²³⁹⁺²⁴⁰Pu ratios with depth suggests mechanical transport and mixing discrete contaminated particles under arid conditions. Occasional samples beyond the northeastern corner are observed to contain anomalously high Pu concentrations with corresponding low ²⁴⁰Pu/²³⁹Pu atoms ratios, suggesting the occurrence of "hot particles;" application of a background Pu subtraction results in calculated Pu atom ratios for the "hot particles" which are statistically similar to those observed in the northeastern corner. Taken together, our data suggests that flooding resulted in mechanical transport of contaminated particles into the area between the SDA and the flood containment dike in the northeastern corner, following which subsequent contamination spreading resulted from wind transport of discrete particles.« less

  8. Mechanical environmental transport of actinides and ¹³⁷Cs from an arid radioactive waste disposal site

    SciTech Connect

    Snow, Mathew S.; Clark, Sue B.; Morrison, Samuel S.; Watrous, Matthew G.; Olson, John E.; Snyder, Darin C.

    2015-10-01

    Particulate transport represents an important mechanism for actinides and fission products at the Earth's surface; soil samples taken in the early 1970's near the Subsurface Disposal Area (SDA) at Idaho National Laboratory (INL) provide a case study for examining the mechanisms and characteristics of actinide transport under arid conditions. Transuranic waste was disposed via shallow land burial at the SDA until shortly after a flooding event that occurred in 1969. In this study we analyze soils collected in the early 1970's for ¹³⁷Cs, ²⁴¹Am, and Pu using a combination of radiometric and mass spectrometric techniques. Two distinct ²⁴⁰Pu/²³⁹Pu isotopic ratios are observed for contamination from the SDA, with values ranging from at least 0.059 to 0.069. ²⁴¹Am concentrations are observed to increase only slightly in 0-4 cm soils over the ~40 year period since soil sampling, contrary to Markham's previous hypothesis that ²⁴¹Pu is principally associated with the 0-4 cm soil fractions (Markham 1978). The lack of statistical difference in ²⁴¹Am/²³⁹⁺²⁴⁰Pu ratios with depth suggests mechanical transport and mixing discrete contaminated particles under arid conditions. Occasional samples beyond the northeastern corner are observed to contain anomalously high Pu concentrations with corresponding low ²⁴⁰Pu/²³⁹Pu atoms ratios, suggesting the occurrence of "hot particles;" application of a background Pu subtraction results in calculated Pu atom ratios for the "hot particles" which are statistically similar to those observed in the northeastern corner. Taken together, our data suggests that flooding resulted in mechanical transport of contaminated particles into the area between the SDA and the flood containment dike in the northeastern corner, following which subsequent contamination spreading resulted from wind transport of discrete particles.

  9. Method for the recovery of actinide elements from nuclear reactor waste

    DOEpatents

    Horwitz, E. Philip; Delphin, Walter H.; Mason, George W.

    1979-01-01

    A process for partitioning and recovering actinide values from acidic waste solutions resulting from reprocessing of irradiated nuclear fuels by adding hydroxylammonium nitrate and hydrazine to the waste solution to adjust the valence of the neptunium and plutonium values in the solution to the +4 oxidation state, thus forming a feed solution and contacting the feed solution with an extractant of dihexoxyethyl phosphoric acid in an organic diluent whereby the actinide values, most of the rare earth values and some fission product values are taken up by the extractant. Separation is achieved by contacting the loaded extractant with two aqueous strip solutions, a nitric acid solution to selectively strip the americium, curium and rare earth values and an oxalate solution of tetramethylammonium hydrogen oxalate and oxalic acid or trimethylammonium hydrogen oxalate to selectively strip the neptunium, plutonium and fission product values. Uranium values remain in the extractant and may be recovered with a phosphoric acid strip. The neptunium and plutonium values are recovered from the oxalate by adding sufficient nitric acid to destroy the complexing ability of the oxalate, forming a second feed, and contacting the second feed with a second extractant of tricaprylmethylammonium nitrate in an inert diluent whereby the neptunium and plutonium values are selectively extracted. The values are recovered from the extractant with formic acid.

  10. Ageing of a phosphate ceramic used to immobilize chloride-contaminated actinide waste

    SciTech Connect

    Metcalfe, Brian; Donald, Ian W.; Fong, Shirley K.; Gerrard, Lee A.; Strachan, Denis M.; Scheele, Randall D.

    2009-03-31

    At AWE, we have developed a process for the immobilization of ILW waste containing a significant quantity of chloride with Ca3(PO4)2 as the host material. Waste ions are incorporated into two phosphate-based phases, chlorapatite [Ca5(PO4)3Cl] and spodiosite [Ca2(PO4)Cl]. Non-active trials performed at AWE with Sm as the actinide surrogate demonstrated the durability of these phases in aqueous solution. Trials of the process, in which actinide-doped materials were used, wer performed at PNNL where the waste form was found to be resistant to aqueous leaching. Initial leach trials conducted on 239Pu /241Am loaded ceramic at 40°C/28 days gave normalized mass losses of 1.2 x 10-5 g.m-2 and 2.7 x 10-3 g.m-2 for Pu and Cl respectively. In order to assess the response of the phases to radiation-induced damage, accelerated ageing trials were performed on samples in which the 239Pu was replaced with 238Pu. No changes to the crystalline structure of the waste were detected in the XRD patterns after the samples had experienced an α radiation dose of 4 x 1018 g-1. Leach trials showed that there was an increase in the P and Ca release rates but no change in the Pu release rate.

  11. Establishment of uncertainty ranges and probability distributions of actinide solubilities for performance assessment in the Waste Isolation Pilot Plant (WIPP).

    SciTech Connect

    Long, Jennifer; Nowak, Jim; Ismail, Ahmed E.; Brush, Laurence H.; Xiong, Yongliang

    2010-03-01

    The Fracture-Matrix Transport (FMT) code developed at Sandia National Laboratories solves chemical equilibrium problems using the Pitzer activity coefficient model with a database containing actinide species. The code is capable of predicting actinide solubilities at 25 C in various ionic-strength solutions from dilute groundwaters to high-ionic-strength brines. The code uses oxidation state analogies, i.e., Am(III) is used to predict solubilities of actinides in the +III oxidation state; Th(IV) is used to predict solubilities of actinides in the +IV state; Np(V) is utilized to predict solubilities of actinides in the +V state. This code has been qualified for predicting actinide solubilities for the Waste Isolation Pilot Plant (WIPP) Compliance Certification Application in 1996, and Compliance Re-Certification Applications in 2004 and 2009. We have established revised actinide-solubility uncertainty ranges and probability distributions for Performance Assessment (PA) by comparing actinide solubilities predicted by the FMT code with solubility data in various solutions from the open literature. The literature data used in this study include solubilities in simple solutions (NaCl, NaHCO{sub 3}, Na{sub 2}CO{sub 3}, NaClO{sub 4}, KCl, K{sub 2}CO{sub 3}, etc.), binary mixing solutions (NaCl+NaHCO{sub 3}, NaCl+Na{sub 2}CO{sub 3}, KCl+K{sub 2}CO{sub 3}, etc.), ternary mixing solutions (NaCl+Na{sub 2}CO{sub 3}+KCl, NaHCO{sub 3}+Na{sub 2}CO{sub 3}+NaClO{sub 4}, etc.), and multi-component synthetic brines relevant to the WIPP.

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

    SciTech Connect

    Koch, M.; Kazimi, M.S.

    1991-04-01

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

  13. Role of Microbes as Biocolloids in the Transport of Actinides from a Deep Underground Radioactive Waste Repository

    SciTech Connect

    Dodge, C.J.; Dunn, M.; Francis, A.J.; Gillow, J.B.; Mantione, K.; Pansoy-Hjelvik, M.E.; Papenguth, H.W.; Strietelmeier, B.A.

    1998-12-17

    We investigated the interaction of dissolved actinides Th, U, Np Zgpu, and Am, with a pure and a mixed culture of halophilic bactezia isolated from the Waste Isolation H.Iot Plant repository under anaerobic conditions to evaluate their potentiaI transport as biocolloids from the waste site. The sizes of the bacterial cells studied ranged from ().54 x 0.48 pm to 7.7 x 0.67pm Using sequential mimofiltration, we determined the ~~ation of actinides with fi-ee-living (mobile) bacterial cells suspended in a fluid medium containing. NaCl or M=W12 brine, at various phaes of their growth cycIes. The number of suspended kcteria rangy-d born 106 to 109 cells ml-*. Tine amount of actinide associatd with the wspend~ cell fraction (cakzdated & mol cell-*) was very Iow: Th, 10-*2; U, 10-1s - 10-lS; - ~ Np, 1o-15- 10-19; Pu, 10-ls -10-21 ; and h, 10-1* - 10-*9 ; and it varied with the bacteihl - CUIture studied. l%e differe&es in the asswiation are amibuted to the extent of bioamxmdation and biosorption by the bacteria pH, the compo&on of the brine, and the speziation and bioavaiIability of the actinides.

  14. Tracing Waste Water with Li isotopes

    NASA Astrophysics Data System (ADS)

    Millot, R.; Desaulty, A. M.

    2015-12-01

    The contribution of human activities such as industries, agriculture and various domestic inputs, becomes more and more significant in the chemical composition of the dissolved load of rivers. Human factors act as a supplementary key process. Therefore the mass-balance for the budget of catchments and river basins include anthropogenic disturbances. In the present study, we investigate waste water tracing by the use of Li isotopes in a small river basin near Orléans in France (l'Egoutier, 15 km² and 5 km long). It is well known that Li has strategic importance for numerous industrial applications including its use in the production of batteries for both mobile devices (computers, tablets, smartphones, etc.) and electric vehicles, but also in pharmaceutical formulations. In the present work, we collected river waters samples before and after the release from a waste water treatment plant connected to an hospital. Lithium isotopic compositions are rather homogeneous in river waters with δ7Li values around -0.5‰ ± 1 along the main course of the stream (n=7). The waste water sample is very different from the natural background of the river basin with Li concentration being twice of the values without pollution and significant heavy lithium contribution (δ7Li = +4‰). These preliminary results will be discussed in relation with factors controlling the distribution of Li and its isotopes in this specific system and compared with the release of other metals such as Pb or Zn.

  15. Extraction processes and solvents for recovery of cesium, strontium, rare earth elements, technetium and actinides from liquid radioactive waste

    DOEpatents

    Zaitsev, Boris N.; Esimantovskiy, Vyacheslav M.; Lazarev, Leonard N.; Dzekun, Evgeniy G.; Romanovskiy, Valeriy N.; Todd, Terry A.; Brewer, Ken N.; Herbst, Ronald S.; Law, Jack D.

    2001-01-01

    Cesium and strontium are extracted from aqueous acidic radioactive waste containing rare earth elements, technetium and actinides, by contacting the waste with a composition of a complex organoboron compound and polyethylene glycol in an organofluorine diluent mixture. In a preferred embodiment the complex organoboron compound is chlorinated cobalt dicarbollide, the polyethylene glycol has the formula RC.sub.6 H.sub.4 (OCH.sub.2 CH.sub.2).sub.n OH, and the organofluorine diluent is a mixture of bis-tetrafluoropropyl ether of diethylene glycol with at least one of bis-tetrafluoropropyl ether of ethylene glycol and bis-tetrafluoropropyl formal. The rare earths, technetium and the actinides (especially uranium, plutonium and americium), are extracted from the aqueous phase using a phosphine oxide in a hydrocarbon diluent, and reextracted from the resulting organic phase into an aqueous phase by using a suitable strip reagent.

  16. Flowsheet report for baseline actinide blanket processing for accelerator transmutation of waste

    SciTech Connect

    Walker, R.B.

    1992-04-08

    We provide a flowsheet analysis of the chemical processing of actinide and fission product materials form the actinide blanket of an accelerator-based transmutation concept. An initial liquid ion exchange step is employed to recover unburned plutonium and neptunium, so that it can be returned quickly to the transmitter. The remaining materials, consisting of fission products and trivalent actinides (americium, curium), is processed after a cooling period. A reverse Talspeak process is employed to separate these trivalent actinides from lanthanides and other fission products.

  17. 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

  18. Microbial Transformation of TRU and Mixed Wastes: Actinide Speciation and Waste Volume Reduction

    SciTech Connect

    Halada, Gary P.

    2004-12-01

    I. To characterize the biodegradation of cellulosic materials using Fourier Transform Infrared (FTIR) Spectroscopy. II. To develop an electrochemical/spectroscopic methodology to characterize TRU waste microbial transformation III. To develop molecular models of TRU complexes in order to understand microbial transformation In all cases, objectives are designed to compliment the efforts from other team members, and will be periodically coordinated through the lead P.I. at Brookhaven National Laboratory (BNL), A.J. Francis.

  19. An Approach for Validating Actinide and Fission Product Burnup Credit Criticality Safety Analyses-Isotopic Composition Predictions

    SciTech Connect

    Radulescu, Georgeta; Gauld, Ian C; Ilas, Germina; Wagner, John C

    2011-01-01

    The expanded use of burnup credit in the United States (U.S.) for storage and transport casks, particularly in the acceptance of credit for fission products, has been constrained by the availability of experimental fission product data to support code validation. The U.S. Nuclear Regulatory Commission (NRC) staff has noted that the rationale for restricting the Interim Staff Guidance on burnup credit for storage and transportation casks (ISG-8) to actinide-only is based largely on the lack of clear, definitive experiments that can be used to estimate the bias and uncertainty for computational analyses associated with using burnup credit. To address the issues of burnup credit criticality validation, the NRC initiated a project with the Oak Ridge National Laboratory to (1) develop and establish a technically sound validation approach for commercial spent nuclear fuel (SNF) criticality safety evaluations based on best-available data and methods and (2) apply 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 purpose of this paper is to describe the isotopic composition (depletion) validation approach and resulting observations and recommendations. Validation of the criticality calculations is addressed in a companion paper at this conference. For isotopic composition validation, the approach is to determine burnup-dependent bias and uncertainty in the effective neutron multiplication factor (keff) due to bias and uncertainty in isotopic predictions, via comparisons of isotopic composition predictions (calculated) and measured isotopic compositions from destructive radiochemical assay utilizing as much assay data as is available, and a best-estimate Monte Carlo based method. This paper (1) provides a detailed description of the burnup credit isotopic validation approach and its technical bases, (2) describes the application of the approach for

  20. Association of actinides with microorganisms and clay: Implications for radionuclide migration from waste-repository sites

    SciTech Connect

    Ohnuki, T.; Francis, A.; Kozai, N.; Sakamoto, F.; Ozaki, T.; Nankawa, T.; Suzuki, Y.

    2010-04-01

    We conducted a series of basic studies on the microbial accumulation of actinides to elucidate their migration behavior around backfill materials used in the geological disposal of radioactive wastes. We explored the interactions of U(VI) and Pu(VI) with Bacillus subtilis, kaolinite clay, and within a mixture of the two, directly analyzing their association with the bacterium in the mixture by transmission electron microscopy (TEM) and scanning electron microscopy (SEM). The accumulation of U by the mixture rose as the numbers of B. subtilis cells increased. Treating the kaolinite with potassium acetate (CH{sub 3}COOK) removed approximately 80% of the associated uranium while only 65% was removed in the presence of B. subtilis. TEM-EDS analysis confirmed that most of the U taken from solution was associated with B. subtilis. XANES analyses revealed that the oxidation state of uranium associated with B. subtilis, kaolinite, and with the mixture containing both was U(VI). The amount of Pu sorbed by B. subtilis increased with time, but did not reach equilibrium in 48 h; in kaolinite alone, equilibrium was attained within 8 h. After 48 h, the oxidation state of Pu in the solutions exposed to B. subtilis and to the mixture had changed to Pu(V), whereas the oxidation state of the Pu associated with both was Pu(IV). In contrast, there was no change in the oxidation state of Pu in the solution nor on kaolinite after exposure to Pu(VI). SEM-EDS analysis indicated that most of the Pu in the mixture was associated with the bacteria. These results suggest that U(VI) and Pu(VI) preferentially are sorbed to bacterial cells in the presence of kaolinite clay, and that the mechanism of accumulation of U and Pu differs. U(VI) is sorbed directly to the bacterial cells, whereas Pu(VI) first is reduced to Pu(V) and then to Pu(IV), and the latter is associated with the cells. These results have important implications on the migrations of radionuclides around the repository sites of

  1. Neodymium isotope analyses after combined extraction of actinide and lanthanide elements from seawater and deep-sea coral aragonite

    NASA Astrophysics Data System (ADS)

    Struve, Torben; van de Flierdt, Tina; Robinson, Laura F.; Bradtmiller, Louisa I.; Hines, Sophia K.; Adkins, Jess F.; Lambelet, Myriam; Crocket, Kirsty C.; Kreissig, Katharina; Coles, Barry; Auro, Maureen E.

    2016-01-01

    Isotopes of the actinide elements protactinium (Pa), thorium (Th), and uranium (U), and the lanthanide element neodymium (Nd) are often used as complementary tracers of modern and past oceanic processes. The extraction of such elements from low abundance matrices, such as seawater and carbonate, is however labor-intensive and requires significant amounts of sample material. We here present a combined method for the extraction of Pa, Th, and Nd from 5 to 10 L seawater samples, and of U, Th, and Nd from <1 g carbonate samples. Neodymium is collected in the respective wash fractions of Pa-Th and U-Th anion exchange chromatographies. Regardless of the original sample matrix, Nd is extracted during a two-stage ion chromatography, followed by thermal ionization mass spectrometry (TIMS) analysis as NdO+. Using this combined procedure, we obtained results for Nd isotopic compositions on two GEOTRACES consensus samples from Bermuda Atlantic Time Series (BATS), which are within error identical to results for separately sampled and processed dedicated Nd samples (ɛNd = -9.20 ± 0.21 and -13.11 ± 0.21 for 15 and 2000 m water depths, respectively; intercalibration results from 14 laboratories: ɛNd = -9.19 ± 0.57 and -13.14 ± 0.57). Furthermore, Nd isotope results for an in-house coral reference material are identical within analytical uncertainty for dedicated Nd chemistry and after collection of Nd from U-Th anion exchange chromatography. Our procedure does not require major adaptations to independently used ion exchange chromatographies for U-Pa-Th and Nd, and can hence be readily implemented for a wide range of applications.

  2. Calculation of the fission-fragment yields of the pre-actinide nuclei by the example of the natPb isotopes

    NASA Astrophysics Data System (ADS)

    Maslyuk, V. T.; Parlag, O. A.; Lendyel, O. I.; Marynets, T. I.; Romanyuk, M. I.; Shevchenko, O. S.; Ranyuk, Ju. Ju.; Dovbnya, A. M.

    2016-11-01

    The calculations of the fission-fragment yields (mass and charge spectra) carried out within the frameworks of the proposed statistical method for the pre-actinide nuclei by the example of natPb (20 isotopes) are presented. The role of neutron shells with N = 50 and N = 82 in realizing the single- and double-humped shape of the fission-fragment yields, respectively, for the neutron-deficit and neutron-excess Pb isotopes has been investigated. An explanation of the experimental results on the natPb fission was performed taking into account transformations to the ensemble of the long- and short-lived nuclear fragments.

  3. 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.

  4. Isotope tracer studies of diffusion in silicates and of geological transport processes using actinide elements

    SciTech Connect

    Wasserburg, G.J.

    1992-01-01

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

  5. The Effects of Flux Spectrum Perturbation on Transmutation of Actinides: Optimizing the Production of Transcurium Isotopes

    SciTech Connect

    Hogle, Susan L; Maldonado, G Ivan; Alexander, Charles W

    2012-01-01

    This research presented herein involves the optimization of transcurium production in the High Flux Isotope Reactor at Oak Ridge National Laboratory. Due to the dependence of isotope cross sections on incoming neutron energy, the efficiency with which an isotope is transmuted is highly dependent upon the flux spectrum. There are certain energy bands in which the rate of fission of transcurium production feedstock materials is minimized, relative to the rate of non-fission absorptions. It is proposed that by perturbing the flux spectrum, it is possible to increase the amount of key isotopes, such as 249Bk and 252Cf, that are produced during a transmutation cycle, relative to the consumption of feedstock material. This optimization process is carried out by developing an iterative objective framework involving problem definition, flux spectrum and cross section analysis, simulated transmutation, and analysis of final yields and transmutation parameters. It is shown that it is possible to perturb the local flux spectrum in the transcurium target by perturbing the composition of the target. It is further shown that these perturbations are able to alter the target yields in a non-negligible way. Future work is necessary to develop the optimization framework, and identify the necessary algorithms to update the problem definition based upon progress towards the optimization goals.

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

    NASA Astrophysics Data System (ADS)

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

    2016-06-01

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

  7. Evaluation and testing of sequestering agents for the removal of actinides from waste streams

    SciTech Connect

    Hoffman, D.C.; Romanovski, V.V.; Veeck, A.C.

    1997-10-01

    The purpose of this project is to evaluate and test the complexing ability of a variety of promising new complexing agents synthesized by Professor Kenneth Raymond`s group at the University of California, Berkeley (ESP-CP TTP Number SF16C311). Some of these derivatives have already shown the potential for selectivity binding Pu(IV) in a wide range of solutions in the presence of other metals. Professor Raymond`s group uses molecular modeling to design and synthesize ligands based on modification of natural siderophores, or their analogs, for chelation of actinides. The ligands are then modified for use as liquid/liquid and solid/liquid extractants. The authors` group at the Glenn T. Seaborg Institute for Transactinium Science (ITS) at Lawrence Livermore National Laboratory determines the complex formation constants between the ligands and actinide ions, the capacity and time dependence for uptake on the resins, and the effect of other metal ions and pH.

  8. Evaluation of extractants and chelating resins in polishing actinide-contaminated waste streams

    SciTech Connect

    Schreiber, S.B.; Dunn, S.L.; Yarbro, S.L.

    1991-06-01

    At the Los Alamos National Laboratory Plutonium Facility, anion exchange is used for recovering plutonium from nitric acid solutions. Although this approach recovers >99%, the trace amounts of plutonium and other actinides remaining in the effluent require additional processing. We are doing research to develop a secondary unit operation that can directly polish the effluent so that actinide levels are reduced to below the maximum allowed for facility discharge. We selected solvent extraction, the only unit operation that can meet the stringent process requirements imposed; several carbonyl and phosphoryl extractants were evaluated and their performance characterized. We also investigated various engineering approaches for solvent extraction; the most promising was a chelating resin loaded with extractant. Our research now focuses on the synthesis of malonamides, and our goal is to bond these extractants to a resin matrix. 7 refs., 12 figs., 1 tab.

  9. Lessons Learned from Characterization, Performance Assessment, and EPA Regulatory Review of the 1996 Actinide Source Term for the Waste Isolation Pilot Plant

    SciTech Connect

    Larson, K.W.; Moore, R.C.; Nowak, E.J.; Papenguth, H.W.; Jow, H.

    1999-03-22

    The Waste Isolation Pilot Plant (WIPP) is a US Department of Energy (DOE) facility for the permanent disposal of transuranic waste from defense activities. In 1996, the DOE submitted the Title 40 CFR Part 191 Compliance Certification Application for the Waste Isolation Pilot Plant (CCA) to the US Environmental Protection Agency (EPA). The CCA included a probabilistic performance assessment (PA) conducted by Sandia National Laboratories to establish compliance with the quantitative release limits defined in 40 CFR 191.13. An experimental program to collect data relevant to the actinide source term began around 1989, which eventually supported the 1996 CCA PA actinide source term model. The actinide source term provided an estimate of mobile dissolved and colloidal Pu, Am, U, Th, and Np concentrations in their stable oxidation states, and accounted for effects of uncertainty in the chemistry of brines in waste disposal areas. The experimental program and the actinide source term included in the CCA PA underwent EPA review lasting more than 1 year. Experiments were initially conducted to develop data relevant to the wide range of potential future conditions in waste disposal areas. Interim, preliminary performance assessments and actinide source term models provided insight allowing refinement of experiments and models. Expert peer review provided additional feedback and confidence in the evolving experimental program. By 1995, the chemical database and PA predictions of WIPP performance were considered reliable enough to support the decision to add an MgO backfill to waste rooms to control chemical conditions and reduce uncertainty in actinide concentrations, especially for Pu and Am. Important lessons learned through the characterization, PA modeling, and regulatory review of the actinide source term are (1) experimental characterization and PA should evolve together, with neither activity completely dominating the other, (2) the understanding of physical processes

  10. 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

    2015-06-02

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

  11. Loading Actinides in Multilayered Structures for Nuclear Waste Treatment: The First Case Study of Uranium Capture with Vanadium Carbide MXene.

    PubMed

    Wang, Lin; Yuan, Liyong; Chen, Ke; Zhang, Yujuan; Deng, Qihuang; Du, Shiyu; Huang, Qing; Zheng, Lirong; Zhang, Jing; Chai, Zhifang; Barsoum, Michel W; Wang, Xiangke; Shi, Weiqun

    2016-06-29

    Efficient nuclear waste treatment and environmental management are important hurdles that need to be overcome if nuclear energy is to become more widely used. Herein, we demonstrate the first case of using two-dimensional (2D) multilayered V2CTx nanosheets prepared by HF etching of V2AlC to remove actinides from aqueous solutions. The V2CTx material is found to be a highly efficient uranium (U(VI)) sorbent, evidenced by a high uptake capacity of 174 mg g(-1), fast sorption kinetics, and desirable selectivity. Fitting of the sorption isotherm indicated that the sorption followed a heterogeneous adsorption model, most probably due to the presence of heterogeneous adsorption sites. Density functional theory calculations, in combination with X-ray absorption fine structure characterizations, suggest that the uranyl ions prefer to coordinate with hydroxyl groups bonded to the V-sites of the nanosheets via forming bidentate inner-sphere complexes.

  12. Isotope Tracer Studies of Diffusion in Sillicates and of Geological Transport Processes Using Actinide Elements

    SciTech Connect

    Wasserburg, Gerald J

    2008-07-31

    The objectives were directed toward understanding the transport of chemical species in nature, with particular emphasis on aqueous transport in solution, in colloids, and on particles. Major improvements in measuring ultra-low concentrations of rare elements were achieved. We focused on two areas of studies: (1) Field, laboratory, and theoretical studies of the transport and deposition of U, Th isotopes and their daughter products in natural systems; and (2) Study of calcium isotope fractionation effects in marine carbonates and in carbonates precipitated in the laboratory, under controlled temperature, pH, and rates of precipitation. A major study of isotopic fractionation of Ca during calcite growth from solution has been completed and published. It was found that the isotopic shifts widely reported in the literature and attributed to biological processes are in fact due to a small equilibrium fractionation factor that is suppressed by supersaturation of the solution. These effects were demonstrated in the laboratory and with consideration of the solution conditions in natural systems, where [Ca{sup 2+}] >> [CO{sub 3}{sup 2-}] + [HCO{sub 3}{sup -}]. The controlling rate is not the diffusion of Ca, as was earlier proposed, but rather the rate of supply of [CO{sub 3}{sup 2-}] ions to the interface. This now opens the issues of isotopic fractionation of many elements to a more physical-chemical approach. The isotopic composition of Ca {Delta}({sup 44}Ca/{sup 40}Ca) in calcite crystals has been determined relative to that in the parent solutions by TIMS using a double spike. Solutions were exposed to an atmosphere of NH{sub 3} and CO{sub 2}, provided by the decomposition of (NH4)2CO3. Alkalinity, pH, and concentrations of CO{sub 3}{sup 2-}, HCO{sub 3}{sup -}, and CO{sub 2} in solution were determined. The procedures permitted us to determine {Delta}({sup 44}Ca/{sup 40}Ca) over a range of pH conditions, with the associated ranges of alkalinity. Two solutions with

  13. Study of extraterrestrial disposal of radioactive wastes. Part 3: Preliminary feasibility screening study of space disposal of the actinide radioactive wastes with 1 percent and 0.1 percent fission product contamination

    NASA Technical Reports Server (NTRS)

    Hyland, R. E.; Wohl, M. L.; Finnegan, P. M.

    1973-01-01

    A preliminary study was conducted of the feasibility of space disposal of the actinide class of radioactive waste material. This waste was assumed to contain 1 and 0.1 percent residual fission products, since it may not be feasible to completely separate the actinides. The actinides are a small fraction of the total waste but they remain radioactive much longer than the other wastes and must be isolated from human encounter for tens of thousands of years. Results indicate that space disposal is promising but more study is required, particularly in the area of safety. The minimum cost of space transportation would increase the consumer electric utility bill by the order of 1 percent for earth escape and 3 percent for solar escape. The waste package in this phase of the study was designed for normal operating conditions only; the design of next phase of the study will include provisions for accident safety. The number of shuttle launches per year required to dispose of all U.S. generated actinide waste with 0.1 percent residual fission products varies between 3 and 15 in 1985 and between 25 and 110 by 2000. The lower values assume earth escape (solar orbit) and the higher values are for escape from the solar system.

  14. Semi-empirical models of actinide alloying

    NASA Astrophysics Data System (ADS)

    Gibson, John K.; Haire, Richard G.; Ogawa, Toru

    1999-07-01

    Alloys of Np have been studied less than those of the neighboring elements, U and Pu; the higher actinides have received even less attention. Recent interest in 237Np, 241Am and other actinide isotopes as significant, long-lived and highly radiotoxic nuclear waste components, and particularly the roles of metallic materials in new handling/separations and remediation technologies, demands that this paucity of information concerning alloy behaviors be addressed. An additional interest in these materials arises from the possibility of revealing fundamental properties and bonding interactions, which would further characterize the unique electronic structures (e.g., 5f electrons) of the actinide elements. The small empirical knowledge basis presently available for understanding and modeling the alloying behavior of Np is summarized here, with emphasis on our recent results for the Np-Am, Np-Zr and Np-Fe phase diagrams. In view of the limited experimental data base for neptunium and the transplutonium metals, the value of semi-empirical intermetallic bonding models for predicting actinide alloy thermodynamics is evaluated.

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

    SciTech Connect

    Prof. G. J. Wasserburg

    2001-01-19

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

  16. 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).

  17. 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.

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

    SciTech Connect

    G. Palmiottti; H. Hiruta; M. Salvatores

    2011-09-01

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

  19. Determination of long-lived fission products and actinides in Savannah River site HLW sludge and glass for waste acceptance

    SciTech Connect

    Bibler, N.E.; Boyce, W.T.; Coleman, C.J.

    1997-10-01

    Savannah River Site (SRS) is currently immobilizing the radioactive, caustic, high-level waste sludge in Tank 51 into a borosilicate glass for disposal in a geologic repository. A requirement for repository acceptance is that SRS report the concentrations of certain fission product and actinide radionuclides in the glass. This paper presents measurements of many of these concentrations in both Tank 51 sludge and the final glass. The radionuclides were measured by inductively coupled plasma - mass spectrometry and {alpha}, {beta}, and {gamma} counting methods. Examples of the radionuclides are Sr-90, Cs-137, U-238, Pu-239, and Cm-244. Concentrations in the glass are 3.1 times lower due to dilution of the sludge with a nonradioactive glass forming frit in the vitrification process. Results also indicated that in both the sludge and glass the relative concentrations of the long lived fission products insoluble in caustic area in proportion to their yields from the fission of U-235 in the SRS reactors. This allowed the calculation of a fission yield scaling factor. This factor in addition to the sludge dilution factor can be used to estimate concentrations of waste acceptance radionuclides that cannot be measured in the glass.

  20. Laboratory evaluation of colloidal actinide transport at the Waste Isolation Pilot Plant (WIPP): 1. crushed-dolomite column flow...

    SciTech Connect

    Yelton, W.G.; Behl, Y.K.; Kelly, J.W.; Dunn, M.; Gillow, J.B.; Francis, A.J.; Papenguth, H.W.

    1996-12-31

    Colloid-facilitated transport of Pu, Am, U, Th, and Np has been recognized as a potentially important phenomenon affecting the performance of the Waste Isolation Pilot Plant (WIPP) facility being developed for safe disposal of transuranic radioactive waste. In a human intrusion scenario, actinide-bearing colloidal particles may be released from the repository and be transported by brines (approximately 0.8 to 3 molal ionic strength) through the Culebra, a thin fractured microcrystalline (mean grain size 2 micrometers) dolomite aquifer overlying the repository. Transport experiments were conducted using sieved, uniformly packed crushed Culebra rock or nonporous dolomite cleavage rhombohedra. Experiments with mineral fragments and fixed and live WIPP-relevant bacteria cultures showed significant levels of retardation due to physical filtration effects. Humic substances were not attenuated by the Culebra dolomite. Comparison of elution curves of latex microspheres in columns prepared with microcrystalline rock and nonporous rock showed minimal effect of Culebra micropores on colloid transport. These data form part of the basis to parameterize numerical codes being used to evaluate the performance of the WIPP.

  1. Computational Chemistry for Nuclear Waste Characterization and Processing: Relativistic Quantum Chemistry of Actinides

    SciTech Connect

    Harrison, Robert J.; Bernholdt, David E.; Bursten, Bruce E.; De Jong, Wibe A.; Dixon, David A.; Dyall, Kenneth G.; Ermler, Walter V.; Fann, George I.; Hay, P. J.; Ismail Buchner, Nina; Kendall, Ricky A.; Li, Jun; Marino, Maria M.; Marsden, Colin J.; Martin, Richard L.; Minkoff, Michael; Nichols, Jeffrey A.; Nieplocha, Jarek; Pitzer, Russell M.; Pratt, Lawrence R.; Schreckenbach, Hans Georg; Seth, Michael C.; Shepard, Ron; Stevens, Rick L.; Tilson, Jeffrey L.; Wagner, Albert F.; Wang, Qi; Windus, Theresa L.; Wong, Adrian; Zhang, Zhiyong

    2002-08-02

    In the course of the 3 years we have conducted calculations on molecular structures containing actinides, lanthanides, and other heavy elements. Our calculations were done at the relativistically-correct, all-electron, 4-component calculations (DHF, MP2, and CCSD(T)), using density functional theory (DFT) with relativistic effective core potentials (RECPs), and various other methodologies. We studied the ground- and excited state structures, energetics, vibrational frequencies, and NMR, excitation and ionization spectra. In addition a considerable amount of codes and methodologies have been developed during the GC3 period, enabling us to do the extensive research described in this final report, and providing researchers worldwide with new computational chemistry tools. In this section we will give a brief overview of our activities and accomplishments, grouped by each research institution. A more extensive overview can be found in the appendices containing the full yearly reports.

  2. PF-4 actinide disposition strategy

    SciTech Connect

    Margevicius, Robert W

    2010-05-28

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

  3. Subsurface Biogeochemistry of Actinides

    SciTech Connect

    Kersting, Annie B.; Zavarin, Mavrik

    2016-06-29

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

  4. 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)

  5. Bridging the Gap in the Chemical Thermodynamic Database for Nuclear Waste Repository: Studies of the Effect of Temperature on Actinide Complexation

    SciTech Connect

    Rao, Linfeng; Tian, Guoxin; Xia, Yuanxian; Friese, Judah I.; Zanonato, PierLuigi; Di Bernardo, Plinio

    2009-12-21

    Recent results of thermodynamic studies on the complexation of actinides (UO{sub 2}{sup 2+}, NpO{sub 2}{sup +} and Pu{sup 4+}) with F{sup -}, SO{sub 4}{sup 2-} and H{sub 2}PO{sub 4}{sup -}/HPO{sub 4}{sup 2-} at elevated temperatures are reviewed. The data indicate that, for all systems except the 1:1 complexation of Np(V) with HPO{sub 4}{sup 2-}, the complexation of actinides is enhanced by the increase in temperature. The enhancement is primarily due to the increase in the entropy term (T{Delta}S) that exceeds the increase in the enthalpy ({Delta}H) as the temperature is increased. These data bridge the gaps in the chemical thermodynamic database for nuclear waste repository where the temperature could remain significantly higher than 25 C for a long time after the closure of the repository.

  6. 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.

  7. High Flux Isotopes Reactor (HFIR) Cooling Towers Demolition Waste Management

    SciTech Connect

    Pudelek, R. E.; Gilbert, W. C.

    2002-02-26

    This paper describes the results of a joint initiative between Oak Ridge National Laboratory, operated by UT-Battelle, and Bechtel Jacobs Company, LLC (BJC) to characterize, package, transport, treat, and dispose of demolition waste from the High Flux Isotope Reactor (HFIR), Cooling Tower. The demolition and removal of waste from the site was the first critical step in the planned HFIR beryllium reflector replacement outage scheduled. The outage was scheduled to last a maximum of six months. Demolition and removal of the waste was critical because a new tower was to be constructed over the old concrete water basin. A detailed sampling and analysis plan was developed to characterize the hazardous and radiological constituents of the components of the Cooling Tower. Analyses were performed for Resource Conservation and Recovery Act (RCRA) heavy metals and semi-volatile constituents as defined by 40 CFR 261 and radiological parameters including gross alpha, gross beta, gross gamma, alpha-emitting isotopes and beta-emitting isotopes. Analysis of metals and semi-volatile constituents indicated no exceedances of regulatory limits. Analysis of radionuclides identified uranium and thorium and associated daughters. In addition 60Co, 99Tc, 226Rm, and 228Rm were identified. Most of the tower materials were determined to be low level radioactive waste. A small quantity was determined not to be radioactive, or could be decontaminated. The tower was dismantled October 2000 to January 2001 using a detailed step-by-step process to aid waste segregation and container loading. The volume of waste as packaged for treatment was approximately 1982 cubic meters (70,000 cubic feet). This volume was comprised of plastic ({approx}47%), wood ({approx}38%) and asbestos transite ({approx}14%). The remaining {approx}1% consisted of the fire protection piping (contaminated with lead-based paint) and incidental metal from conduit, nails and braces/supports, and sludge from the basin. The waste

  8. 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

  9. Magnetic fusion driventransmutation of nuclear waste (FTW)

    SciTech Connect

    Peng, Yueng Kay Martin; Cheng, E.T.

    1993-01-01

    The possibility of magnetic Fusion driven Transmutation of Waste (FTW) was revisted and discussed recently. Nuclear wastes include all transuranium elements: Pu isotopes, minor actinides separated from the spent fission fuel, and fissile products. Elimination of thse long-life nuclear wastes is necessary for the long-term viability of fission power. A Small Business Innovative Research program has been initiated under the leadership of TSI Research to examine the efficacy of fusion transmutation of waste utilizing small fusion drivers.

  10. Demonstration of the UNEX Process for the Simultaneous Separation of Cesium, Strontium, and the Actinides from Actual INEEL Sodium-Bearing Waste

    SciTech Connect

    Law, Jack Douglas; Herbst, Ronald Scott; Todd, Terry Allen; Romanovskiy, V.; Smirnov, I.; Babain, V.; Zaitsev, B.; Esimantovskiy, V.

    1999-11-01

    A universal solvent extraction (UNEX) process for the simultaneous separation of cesium, strontium, and the actinides from actual radioactive acidic tank waste was demonstrated at the Idaho National Engineering and Environmental Laboratory. The waste solution used in the countercurrent flowsheet demonstration was obtained from tank WM-185. The UNEX process uses a tertiary solvent containing 0.08 M chlorinated cobalt dicarbollide, 0.5% polyethylene glycol-400 (PEG-400), and 0.02 M diphenyl-N,N-dibutylcarbamoyl phosphine oxide (Ph2Bu2CMPO) in a diluent consisting of phenyltrifluoromethyl sulfone (FS-13). The countercurrent flowsheet demonstration was performed in a shielded cell facility using 24 stages of 2-cm diameter centrifugal contactors. Removal efficiencies of 99.4%, 99.995%, and 99.96% were obtained for 137Cs, 90Sr, and total alpha, respectively. This is sufficient to reduce the activities of 137Cs, 90Sr, and actinides in the WM-185 waste to below NRC Class A LLW requirements. Flooding and/or precipitate formation were not observed during testing. Significant amounts of the Zr (87%), Ba (>99%), Pb (98.8%), Fe (8%), Ca (10%), Mo (32%), and K (28%) were also removed from the feed with the universal solvent extraction flowsheet. 99Tc, Al, Hg, and Na were essentially inextractable (<1% extracted).

  11. Actinide recovery techniques utilizing electromechanical processes

    SciTech Connect

    Westphal, B.R.; Benedict, R.W.

    1994-01-01

    Under certain conditions, the separation of actinides using electromechanical techniques may be an effective means of residue processing. The separation of granular mixtures of actinides and other materials discussed in this report is based on appreciable differences in the magnetic and electrical properties of the actinide elements. In addition, the high density of actinides, particularly uranium and plutonium, may render a simultaneous separation based on mutually complementary parameters. Both high intensity magnetic separation and electrostatic separation have been investigated for the concentration of an actinide waste stream. Waste stream constituents include an actinide metal alloy and broken quartz shards. The investigation of these techniques is in support of the Integral Fast Reactor (IFR) concept currently being developed at Argonne National Laboratory under the auspices of the Department of Energy.

  12. Durability of Actinide Ceramic Waste Forms Under Conditions of Granitoid Rocks

    SciTech Connect

    Burakov, B. E.; Anderson, E. B.

    2002-02-26

    Three samples of {sup 239}Pu-{sup 241}Am-doped ceramics obtained from previous research were used for alteration experiments simulating corrosion of waste forms in ion-saturated solutions. These were ceramics based on: pyrochlore, (Ca,Hf,Pu,U,Gd){sub 2}Ti{sub 2}O{sub 7}, containing 10 wt.% Pu and 0.1 wt.% Am; zircon, (Zr,Pu)SiO{sub 4}, containing 5-6 wt.% Pu and 0.05 wt.% Am; cubic zirconia, (Zr,Gd,Pu)O{sub 2}, containing 10 wt.% Pu and 0.1 wt.% Am. All these samples were milled in an agate mortar to obtain powder with particle sizes less than 30 micron. Sample of granite taken from the depth 500-503 m was studied and then used for preparing ion-saturated water solutions. A rock sample was ground, washed and classified. A fraction with particle size 0.10-0.25 mm was selected for alteration experiments. Powdered ceramic samples were separately placed into deionized water together with ground granite (approximately 1gram granite per 12-ml water) in special Teflon{trademark} vessels and set at 90 C in the oven for 3 months. After alteration experiments, the ceramic powders were studied by precise XRD analysis. Aqueous solutions and granite grains were analyzed for Am and Pu contents. The results show that alteration did not cause significant phase transformation in all ceramic samples. For all altered samples, the Am contents in aqueous solutions after experiments were similar (approximately n x 10{sup 2} Bq/ml) as well as Am amounts absorbed on granite grains (approximately n x 10{sup 5} Bq/g). Results on Pu contents were varied: for the solutions--from 60 Bq/ml for pyrochlore ceramic to 2.1 x 10{sup 3} Bq/ml for zircon ceramic; and for the absorption on granite--from 2.6 x 10{sup 4} Bq/g for zirconia ceramic to 1.4-6.8 x 10{sup 5} Bq/g for pyrochlore and zircon ceramics.

  13. 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.

  14. Experimental and calculational analyses of actinide samples irradiated in EBR-II

    SciTech Connect

    Gilai, D.; Williams, M.L.; Cooper, J.H.; Laing, W.R.; Walker, R.L.; Raman, S.; Stelson, P.H.

    1982-10-01

    Higher actinides influence the characteristics of spent and recycled fuel and dominate the long-term hazards of the reactor waste. Reactor irradiation experiments provide useful benchmarks for testing the evaluated nuclear data for these actinides. During 1967 to 1970, several actinide samples were irradiated in the Idaho EBR-II fast reactor. These samples have now been analyzed, employing mass and alpha spectrometry, to determine the heavy element products. A simple spherical model for the EBR-II core and a recent version of the ORIGEN code with ENDF/B-V data were employed to calculate the exposure products. A detailed comparison between the experimental and calculated results has been made. For samples irradiated at locations near the core center, agreement within 10% was obtained for the major isotopes and their first daughters, and within 20% for the nuclides up the chain. A sensitivity analysis showed that the assumed flux should be increased by 10%.

  15. 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.

  16. SALTSTONE VAULT CLASSIFICATION SAMPLES MODULAR CAUSTIC SIDE SOLVENT EXTRACTION UNIT/ACTINIDE REMOVAL PROCESS WASTE STREAM APRIL 2011

    SciTech Connect

    Eibling, R.

    2011-09-28

    inorganic species measured in the leachate do not exceed the MCL, SMCL or TW limits. (4) The inorganic waste species that exceeded the MCL by more than a factor of 10 were nitrate, nitrite and the sum of nitrate and nitrite. (5) Analyses met all quality assurance specifications of US EPA SW-846. (6) The organic species (benzene, toluene, 1-butanol, phenol) were either not detected or were less than reportable for the vault classification samples. (7) The gross alpha and radium isotopes could not be determined to the MCL because of the elevated background which raised the detection limits. (8) Most of the beta/gamma activity was from 137Cs and its daughter 137mBa. (9) The concentration of 137Cs and 90Sr were present in the leachate at concentrations 1/40th and 1/8th respectively than in the 2003 vault classification samples. The saltstone waste form placed in the Saltstone Disposal Facility in 2QCY11 met the SCHWMR R.61-79.261.24(b) RCRA metals requirements for a nonhazardous waste form. The TCLP leachate concentrations for nitrate, nitrite and the sum of nitrate and nitrite were greater than 10x the MCLs in SCDHEC Regulations R.61-107.19, Part I A, which confirms the Saltstone Disposal Facility classification as a Class 3 Landfill. The saltstone waste form placed in the Saltstone Disposal Facility in 2QCY11 met the R.61-79.268.48(a) non wastewater treatment standards.

  17. Use of Dissolved and Colloidal Actinide Parameters within the 1996 Waste Isolation Pilot Plant Compliance Certification Application

    SciTech Connect

    Moore, R.C.; Stockman, C.T.

    1998-10-15

    Many of the papers in this volume present detailed descriptions of the chemical analyses and methodologies that have been used to evaluate the maximum dissolved and colloid concentrations of actinides within the WIPP repository as part of the performance assessment. This paper describes the program fcm collecting experimental data and provides an overview of how the PA modeled the release of radionuclides to the accessible environment, and how volubility and colloid parameters were used by the PA models.

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

    SciTech Connect

    Wasserburg, G.J.

    1992-12-31

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

  19. Fundamental Chemistry of the Universal Extractant (UNEX) for the Simultaneous Separation of Major Radionuclides (Cesium, Strontium, Actinides, and Lanthanides) from Radioactive Wastes

    SciTech Connect

    Herbst, R. Scott; Peterman, Dean R.; Luther, Thomas A.; Garn, Troy G.; Tillotson, Richard D.; Babain, Vasily A.; Smirnov, Igor V.; Stoyanov, Evgenii S.

    2004-03-28

    4 Scientists at the INEEL and KRI collaboratively developed and validated the concept of a Universal Extractant (UNEX) for simultaneously removing the major radionuclides (Cs, Sr, actinides and lanthanides) from acidic radioactive waste in a single solvent extraction process. The UNEX solvent incorporates three active extractants: chlorinated cobalt dicarbollide, polyethylene glycol and a carbamoylmethylphosphine oxide derivative, dissolved in a suitable organic diluent to simultaneously extract target radionuclides. The process chemistry is unique, but complicated, since the extractants operate synergistically to extract the radionuclides. Results indicate that water dissolved in the organic phase dramatically impacts the process chemistry. In order to investigate this phenomenon, we have varied the amount of water dissolved in the organic phase by using several different organic diluents. The results of 137Cs and 89Sr batch distribution studies for the different organic diluents will be presented. These data and data from other spectroscopic techniques will be used to elucidate the details of the extraction mechanism.

  20. Isotope tracer studies of diffusion in silicates and of geological transport processes in aqueous systems using actinide elements

    SciTech Connect

    Wasserburg, G.J.

    1999-02-01

    This research program has moved ahead with success in several areas. The isotopic composition of osmium in seawater and in some rivers was directly determined for the first time. The concentration of osmium was first estimated in both seawater and rivers. A major effort was directed toward the transport of the U,Th series nuclides in a watershed in Sweden. A serious effort was directed at developing a transport model for the U,Th series nuclides in aquifers. A detailed study of {sup 238}U-{sup 230}Th dating of a cave in Israel was carried out collaboratively. The Os-Re fractionation between silicate and sulfide melts were determined in MORB basalts and glasses and the isotopic composition of Os was measured in sulfide samples.

  1. Rapid determination of actinides in seawater samples

    DOE PAGES

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

    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

  2. Selection of Isotopes and Elements for Fuel Cycle Analysis

    SciTech Connect

    Steven J. Piet

    2009-04-01

    Fuel cycle system analysis simulations examine how the selection among fuel cycle options for reactors, fuel, separation, and waste management impact uranium ore utilization, waste masses and volumes, radiotoxicity, heat to geologic repositories, isotope-dependent proliferation resistance measures, and so forth. Previously, such simulations have tended to track only a few actinide and fission product isotopes, those that have been identified as important to a few criteria from the standpoint of recycled material or waste, taken as a whole. After accounting for such isotopes, the residual mass is often characterized as “fission product other” or “actinide other”. However, detailed assessment of separation and waste management options now require identification of key isotopes and residual mass for Group 1A/2A elements (Rb, Cs, Sr, Ba), inert gases (Kr, Xe), halogens (Br, I), lanthanides, transition metals, transuranic (TRU), uranium, actinide decay products. The paper explains the rationale for a list of 81 isotopes and chemical elements to better support separation and waste management assessment in dynamic system analysis models such as Verifiable Fuel Cycle Simulation (VISION)

  3. Actinide chemistry in ionic liquids.

    PubMed

    Takao, Koichiro; Bell, Thomas James; Ikeda, Yasuhisa

    2013-04-01

    This Forum Article provides an overview of the reported studies on the actinide chemistry in ionic liquids (ILs) with a particular focus on several fundamental chemical aspects: (i) complex formation, (ii) electrochemistry, and (iii) extraction behavior. The majority of investigations have been dedicated to uranium, especially for the 6+ oxidation state (UO2(2+)), because the chemistry of uranium in ordinary solvents has been well investigated and uranium is the most abundant element in the actual nuclear fuel cycles. Other actinides such as thorium, neptunium, plutonium, americium, and curiumm, although less studied, are also of importance in fully understanding the nuclear fuel engineering process and the safe geological disposal of radioactive wastes.

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

    SciTech Connect

    Timothy A. Hyde

    2012-06-01

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

  5. 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.

  6. Detection of the actinides and cesium from environmental samples

    NASA Astrophysics Data System (ADS)

    Snow, Mathew Spencer

    Detection of the actinides and cesium in the environment is important for a variety of applications ranging from environmental remediation to safeguards and nuclear forensics. The utilization of multiple different elemental concentrations and isotopic ratios together can significantly improve the ability to attribute contamination to a unique source term and/or generation process; however, the utilization of multiple elemental "signatures" together from environmental samples requires knowledge of the impact of chemical fractionation for various elements under a variety of environmental conditions (including predominantly aqueous versus arid conditions). The research reported in this dissertation focuses on three major areas: 1. Improving the understanding of actinide-mineral interactions at ultra-low concentrations. Chapter 2 reports a batch sorption and modeling study of Np(V) sorption to the mineral goethite from attomolar to micromolar concentrations. 2. Improving the detection capabilities for Thermal Ionization Mass Spectrometry (TIMS) analyses of ultra-trace cesium from environmental samples. Chapter 4 reports a new method which significantly improves the chemical yields, purification, sample processing time, and ultimately, the detection limits for TIMS analyses of femtogram quantities of cesium from a variety of environmental sample matrices. 3. Demonstrating how actinide and cesium concentrations and isotopic ratios from environmental samples can be utilized together to determine a wealth of information including environmental transport mechanisms (e.g. aqueous versus arid transport) and information on the processes which generated the original material. Chapters1, 3 and 5 demonstrate these principles using Pu, Am, Np, and Cs concentrations and isotopic ratios from contaminated soils taken near the Subsurface Disposal Area (SDA) of Idaho National Laboratory (INL) (a low level radioactive waste disposal site in southeastern Idaho).

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

    SciTech Connect

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

    2009-09-23

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

  8. Molybdenum and zinc stable isotope variation in mining waste rock drainage and waste rock at the Antamina mine, Peru.

    PubMed

    Skierszkan, E K; Mayer, K U; Weis, D; Beckie, R D

    2016-04-15

    The stable isotope composition of molybdenum (Mo) and zinc (Zn) in mine wastes at the Antamina Copper-Zn-Mo mine, Peru, was characterized to investigate whether isotopic variation of these elements indicated metal attenuation processes in mine drainage. Waste rock and ore minerals were analyzed to identify the isotopic composition of Mo and Zn sources, namely molybdenites (MoS2) and sphalerites (ZnS). Molybdenum and Zn stable isotope ratios are reported relative to the NIST-SRM-3134 and PCIGR-1 Zn standards, respectively. δ(98)Mo among molybdenites ranged from -0.6 to +0.6‰ (n=9) while sphalerites showed no δ(66)Zn variations (0.11±0.01‰, 2 SD, n=5). Mine drainage samples from field waste rock weathering experiments were also analyzed to examine the extent of isotopic variability in the dissolved phase. Variations spanned 2.2‰ in δ(98)Mo (-0.1 to +2.1‰) and 0.7‰ in δ(66)Zn (-0.4 to +0.3‰) in mine drainage over a wide pH range (pH2.2-8.6). Lighter δ(66)Zn signatures were observed in alkaline pH conditions, which was consistent with Zn adsorption and/or hydrozincite (Zn5(OH)6(CO3)2) formation. However, in acidic mine drainage Zn isotopic compositions reflected the value of sphalerites. In addition, molybdenum isotope compositions in mine drainage were shifted towards heavier values (0.89±1.25‰, 2 SD, n=16), with some overlap, in comparison to molybdenites and waste rock (0.13±0.82‰, 2 SD, n=9). The cause of heavy Mo isotopic signatures in mine drainage was more difficult to resolve due to isotopic heterogeneity among ore minerals and a variety of possible overlapping processes including dissolution, adsorption and secondary mineral precipitation. This study shows that variation in metal isotope ratios are promising indicators of metal attenuation. Future characterization of isotopic fractionation associated to key environmental reactions will improve the power of Mo and Zn isotope ratios to track the fate of these elements in mine drainage.

  9. Statistical analysis of radiochemical measurements of TRU radionuclides in REDC waste

    SciTech Connect

    Beauchamp, J.; Downing, D.; Chapman, J.; Fedorov, V.; Nguyen, L.; Parks, C.; Schultz, F.; Yong, L.

    1996-10-01

    This report summarizes results of the study on the isotopic ratios of transuranium elements in waste from the Radiochemical Engineering Development Center actinide-processing streams. The knowledge of the isotopic ratios when combined with results of nondestructive assays, in particular with results of Active-Passive Neutron Examination Assay and Gamma Active Segmented Passive Assay, may lead to significant increase in precision of the determination of TRU elements contained in ORNL generated waste streams.

  10. Use of high gradient magnetic separation for actinide application

    SciTech Connect

    Avens, L.R.; Worl, L.A.; Padilla, D.D.

    1996-08-01

    Decontamination of materials such as soils or waste water that contain radioactive isotopes, heavy metals, or hazardous components is a subject of great interest. Magnetic separation is a physical separation process that segregates materials on the basis of magnetic susceptibility. Because the process relies on physical properties, separations can be achieved while producing a minimum of secondary waste. Most traditional physical separation processes effectively treat particles larger than 70 microns. In many situations, the radioactive contaminants are found concentrated in the fine particle size fraction of less than 20 microns. For effective decontamination of the fine particle size fraction most current operations resort to chemical dissolution methods for treatment. High gradient magnetic separation (HGMS) is able to effectively treat particles from 90 to {approximately}0.1 micron in diameter. The technology is currently used on the 60 ton per hour scale in the kaolin clay industry. When the field gradient is of sufficiently high intensity, paramagnetic particles can be physically captured and separated from extraneous nonmagnetic material. Because all actinide compounds are paramagnetic, magnetic separation of actinide containing mixtures is feasible. The advent of reliable superconducting magnets also makes magnetic separation of weakly paramagnetic species attractive. HGMS work at Los Alamos National Laboratory (LANL) is being developed for soil remediation, waste water treatment and treatment of actinide chemical processing residues. LANL and Lockheed Environmental Systems and Technologies Company (LESAT) have worked on a co-operative research and development agreement (CRADA) to develop HGMS for radioactive soil decontamination. The program is designed to transfer HGMS from the laboratory and other industries for the commercial treatment of radioactive contaminated materials. 9 refs., 2 figs., 2 tabs.

  11. Fundamental Chemistry of the Universal Extractant (UNEX) for the Simultaneous Separation of Major Radionuclides (Cesium, Strontium, Actinides, and Lanthanides) from Radioactive Wastes

    SciTech Connect

    Herbst, R. Scott; Peterman, Dean R.; Luther, Thomas A.; Babain, Vasily A.; Smirnov, Igor V.; Stoyanov, Evgenii S.

    2003-09-10

    Scientists at the INEEL and KRI collaboratively developed and validated the concept of a Universal Extractant (UNEX) for simultaneously removing the major radionuclides (Cs, Sr, actinides, and lanthanides) from acidic radioactive waste in a single solvent extraction process. The UNEX solvent incorporates three active extractants: chlorinated cobalt dicarbollide, polyethylene glycol, and a carbamoylmethylphosphine oxide derivative, dissolved in a suitable organic diluent to simultaneously extract target radionuclides. The process chemistry is unique, but complicated, since the extractants operate synergistically to extract the radionuclides. Furthermore, interactions with the diluent are quite important as the diluent strongly influences the extraction properties of the solvent system. We are currently studying the fundamental chemical phenomena responsible for the selective extraction of the different species to understand the underlying mechanisms and facilitate enhancements i n process chemistry. Our efforts to date have relied on a combination of classical chemistry techniques, infrared (IR) spectroscopy, and nuclear magnetic resonance (NMR) spectroscopy to identify and explain the structures formed in the organic phase, elucidate the operative chemical mechanisms, and evaluate the diluent effects on extraction properties.

  12. Actinide metal processing

    DOEpatents

    Sauer, N.N.; Watkin, J.G.

    1992-03-24

    A process for converting an actinide metal such as thorium, uranium, or plutonium to an actinide oxide material by admixing the actinide metal in an aqueous medium with a hypochlorite as an oxidizing agent for sufficient time to form the actinide oxide material and recovering the actinide oxide material is described together with a low temperature process for preparing an actinide oxide nitrate such as uranyl nitrate. Additionally, a composition of matter comprising the reaction product of uranium metal and sodium hypochlorite is provided, the reaction product being an essentially insoluble uranium oxide material suitable for disposal or long term storage.

  13. Actinide metal processing

    DOEpatents

    Sauer, Nancy N.; Watkin, John G.

    1992-01-01

    A process of converting an actinide metal such as thorium, uranium, or plnium to an actinide oxide material by admixing the actinide metal in an aqueous medium with a hypochlorite as an oxidizing agent for sufficient time to form the actinide oxide material and recovering the actinide oxide material is provided together with a low temperature process of preparing an actinide oxide nitrate such as uranyl nitrte. Additionally, a composition of matter comprising the reaction product of uranium metal and sodium hypochlorite is provided, the reaction product being an essentially insoluble uranium oxide material suitable for disposal or long term storage.

  14. Zirconia Inert Matrix Fuel for Plutonium and Minor Actinides Management in Reactors and as an Ultimate Waste Form

    SciTech Connect

    Degueldre, Claude; Wiesenack, Wolfgang

    2008-07-01

    An yttria stabilised zirconia doped with plutonia and erbia has been selected as inert matrix fuel (IMF) at PSI. The results of experimental irradiation tests on yttria-stabilised zirconia doped with plutonia and erbia pellets in the Halden research reactor as well as a study of zirconia solubility are presented. Zirconia must be stabilised by yttria to form a solid solution such as MAz(Y,Er){sub y}Pu{sub x}Zr{sub 1-y}O{sub 2-{xi}} where minor actinides (MA) oxides are also soluble. (Er,Y,Pu,Zr)O{sub 2-{xi}} (with Pu containing 5% Am) was successfully prepared at PSI and irradiated in the Halden reactor. Emphasis is given on the zirconia- IMF properties under in-pile irradiation, on the fuel material centre temperatures and on the fission gas release. The retention of fission products in zirconia may be stronger at similar temperature, compared to UO{sub 2}. The outstanding behaviour of plutonia-zirconia inert matrix fuel is compared to the classical (U,Pu)O{sub 2} fuels. The properties of the spent fuel pellets are presented focusing on the once-through strategy. For this strategy, low solubility of the inert matrix is required for geological disposal. This parameter was studied in detail for a range of solutions corresponding to groundwater under near field conditions. Under these conditions the IMF solubility is about 109 times smaller than glass, several orders of magnitude lower than UO{sub 2} in oxidising conditions (Yucca Mountain) and comparable in reducing conditions, which makes the zirconia material very attractive for deep geological disposal. The behaviour of plutonia-zirconia inert matrix fuel is discussed within a 'burn and bury' strategy. (authors)

  15. Evaluation of New Inorganic Sorbents for Strontium and Actinide Removal from High-Level Nuclear Waste Solutions

    SciTech Connect

    Hobbs, D.T.; Nyman, M.; Medvedev, D.G.; Tripathi, A.; Clearfield, A.

    2004-03-28

    Monosodium titanate (MST), a hydrous metal oxide sorbent, is the baseline material for the removal of 90Sr and alpha-emitting radionuclides (principally 238Pu, 239Pu, 240Pu and 237Np) from alkaline waste solutions generated during the processing of irradiated nuclear materials at the Savannah River Site. This material exhibits excellent performance characteristics for strontium removal. Plutonium removal is also good, but problematic at the estimated bonding concentration. We are currently developing new inorganic materials for improved sorption characteristics. These materials include sodium nonatitanates, pharmacosiderites and heteropolyniobates. We will present results evaluating the performance of these materials with simulated and actual high level nuclear waste solutions.

  16. 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

  17. 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.

  18. 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.

  19. Near-quantitative recovery of actinides from nitric acid waste streams by solvent extraction using DHDECMP (dihexyl-N,N-diethylcarbamoylmethylphosphonate)

    SciTech Connect

    Marsh, S.F.; Yarbro, S.L.

    1988-01-01

    The more-than-adequate extraction of actinides from high nitrate solutions and of efficient back-extraction from low nitrate solutions make DHDECMP the preferred extractant for this application. Isopar-diluted DHDECMP extraction data are presented herein. Comparative extraction data for Am(III) Pu(IV), and U(VI) are also presented. The behavior of these three actinides can be assumed to represent the general behavior of other actinides in their trivalent, tetravalent, and hexavalent oxidation states. 4 refs., 5 figs.

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

    PubMed

    Krings, Thomas; Mauerhofer, Eric

    2012-07-01

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

  1. 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.

  2. 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.

  3. Tracing source and migration of Pb during waste incineration using stable Pb isotopes.

    PubMed

    Li, Yang; Zhang, Hua; Shao, Li-Ming; He, Pin-Jing

    2017-04-05

    Emission of Pb is a significant environmental concern during solid waste incineration. To target Pb emission control strategies effectively, the major sources of Pb in the waste incineration byproducts must be traced and quantified. However, identifying the migration of Pb in each waste component is difficult because of the heterogeneity of the waste. This study used a laboratory-scale incinerator to simulate the incineration of municipal solid waste (MSW). The Pb isotope ratios of the major waste components ((207)Pb/(206)Pb=0.8550-0.8627 and (208)Pb/(206)Pb=2.0957-2.1131) and their incineration byproducts were measured to trace sources and quantify the Pb contribution of each component to incineration byproducts. As the proportions of food waste (FW), newspaper (NP), and polyethylene bag (PE) in the artificial MSW changed, the contribution ratios of FW and PE to Pb in fly ash changed accordingly, ranging from 31.2% to 50.6% and from 35.0% to 41.8%, respectively. The replacement of PE by PVC significantly increased the partitioning and migration ratio of Pb. The use of Pb isotope ratios as a quantitative tool for tracing Pb from raw waste to incineration byproducts is a feasible means for improving Pb pollution control.

  4. 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.

  5. Laboratory Optimization Tests of Decontamination of Cs, Sr, and Actinides from Hanford Waste Treatment Plant Low Activity Waste Off-Gas Condensate Simulant

    SciTech Connect

    Taylor-Pashow, K.; Nash, C.; McCabe, D.

    2015-01-06

    The Hanford Waste Treatment and Immobilization Plant (WTP) Low Activity Waste (LAW) vitrification facility will generate an aqueous condensate recycle stream (LAW Off-Gas Condensate) from the off-gas system. The baseline plan for disposition of this stream is to send it to the WTP Pretreatment Facility, where it will be blended with LAW, concentrated by evaporation and recycled to the LAW vitrification facility. Alternate disposition of this stream would eliminate recycling of problematic components, and would enable less integrated operation of the LAW melter and the Pretreatment Facilities. Eliminating this stream from recycling within WTP would also substantially decrease the LAW vitrification mission duration and quantity of glass waste.

  6. Positron Spectroscopy of Hydrothermally Grown Actinide Oxides

    DTIC Science & Technology

    2014-03-27

    In this method, the powdered material is placed in a solution which contains extremely powerful mineralizers, such as cesium fluoride for actinide...the isotope that acts as a positron source is sodium -22, which has a relatively short half-life (2.6 y) and emits a characteristic gamma photon (at

  7. 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.

  8. Actinide Spectroscopy Workshop

    SciTech Connect

    Tobin, J.G.; Shuh, D.K.

    2004-12-05

    Actinide materials present an extreme scientific challenge to the materials research community. The complex electronic structures of actinide materials result in many unusual and unique properties that have yet to be fully understood. The difficulties in handling, preparing, and characterizing actinide materials has frequently precluded investigations and has the limited the detailed understanding of these relevant, complex materials. However, modern experiments with actinide materials have the potential to provide key, fundamental information about many long-standing issues concerning actinide materials. This workshop focused on the scientific and technical challenges posed by actinide materials and the potential that synchrotron radiation approaches available at the ALS can contribute to improving the fundamental understanding of actinides materials. Fundamental experimental approaches and results, as well as theoretical modeling and computational simulations, were part of the workshop program.

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

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

  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. 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.

  12. 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.

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

    SciTech Connect

    Bliss, Mary; Stave, Jean A.

    2012-10-01

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

  14. "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

  15. Propagation of Isotopic Bias and Uncertainty to Criticality Safety Analyses of PWR Waste Packages

    SciTech Connect

    Radulescu, Georgeta

    2010-06-01

    Burnup credit methodology is economically advantageous because significantly higher loading capacity may be achieved for spent nuclear fuel (SNF) casks based on this methodology as compared to the loading capacity based on a fresh fuel assumption. However, the criticality safety analysis for establishing the loading curve based on burnup credit becomes increasingly complex as more parameters accounting for spent fuel isotopic compositions are introduced to the safety analysis. The safety analysis requires validation of both depletion and criticality calculation methods. Validation of a neutronic-depletion code consists of quantifying the bias and the uncertainty associated with the bias in predicted SNF compositions caused by cross-section data uncertainty and by approximations in the calculational method. The validation is based on comparison between radiochemical assay (RCA) data and calculated isotopic concentrations for fuel samples representative of SNF inventory. The criticality analysis methodology for commercial SNF disposal allows burnup credit for 14 actinides and 15 fission product isotopes in SNF compositions. The neutronic-depletion method for disposal criticality analysis employing burnup credit is the two-dimensional (2-D) depletion sequence TRITON (Transport Rigor Implemented with Time-dependent Operation for Neutronic depletion)/NEWT (New ESC-based Weighting Transport code) and the 44GROUPNDF5 crosssection library in the Standardized Computer Analysis for Licensing Evaluation (SCALE 5.1) code system. The SCALE 44GROUPNDF5 cross section library is based on the Evaluated Nuclear Data File/B Version V (ENDF/B-V) library. The criticality calculation code for disposal criticality analysis employing burnup credit is General Monte Carlo N-Particle (MCNP) Transport Code. The purpose of this calculation report is to determine the bias on the calculated effective neutron multiplication factor, k{sub eff}, due to the bias and bias uncertainty associated with

  16. High-resolution profiling of the stable isotopes of water in unsaturated coal waste rock

    NASA Astrophysics Data System (ADS)

    Barbour, S. Lee; Hendry, M. Jim; Carey, Sean K.

    2016-03-01

    Characterization of the rate of water migration through unsaturated mine waste rock dumps is an essential element in assessing the chemical loading from these landforms; yet our understanding of how water moves into, through and out of waste rock is incomplete. To further understand the rates and magnitude of percolation through waste rock, deep high-resolution (every 0.1-4.5 m) depth profiles of the stable isotopes of water (δ2H and δ18O) at two coal waste rock dumps and a natural alluvial deposit down-gradient of one of the dumps were collected in the Elk Valley, British Columbia, Canada. The profiles were generated using vapor equilibrium techniques applied to continuous core samples collected using dry sonic drilling methods. Elevated core temperatures (up to 80 °C) were measured during sonic coring. The isotopic values of pore waters measured in the core samples were corrected for water loss to the atmosphere attributed to the elevated core temperatures. The average isotopic composition of the core samples were compared to water collected from rock drains discharging from the base of the dumps. The results indicate that high-resolution profiles of δ2H and δ18O can be measured to depths of 86 m in coal waste rock dumps and, based on the seasonal cycles in the isotopic composition of recharging water, can be used to characterize the migration of recharge water within these dumps. These profiles also suggest that recharge into these dumps occurs from both rain as well as snow melt and may be as high as 400-600 mm/yr (60-75% of annual precipitation). Combined with the relatively low volumetric water contents of these dumps (5-10%) the rates of water migration through the dumps are tens of meters each year.

  17. Irradiation of Metallic Fuels with Rare Earth Additions for Actinide Transmutation in the ATR. Experiment Description for AFC-2A and AFC-2B

    SciTech Connect

    S. L. Hayes; D. J. Utterbeck; T. A. Hyde

    2007-03-01

    The U.S. Advanced Fuel Cycle Initiative (AFCI), now within the broader context of the Global Nuclear Energy Partnership (GNEP), seeks to develop and demonstrate the technologies needed to transmute the long-lived transuranic actinide isotopes contained in spent nuclear fuel into shorter-lived fission products, thereby dramatically decreasing the volume of material requiring disposal and the long-term radio-toxicity and heat load of high-level waste sent to a geologic repository. One important component of the technology development is actinide-bearing metallic transmutation fuel forms containing plutonium, neptunium, americium (and possibly curium) isotopes. The proposed AFC-2A and AFC-2B irradiation experiments are a continuation of the metallic fuel test series in progress in the ATR. This report documents the experiment description and test matrix of the proposed experiments and the Post Irradiation Examination (PIE) and fabrication schedule.

  18. Irradiation of Metallic Fuels with Rare Earth Additions for Actinide Transmutation in the Advanced Test Reactor. Experiment Description for AFC-2A and AFC-2B

    SciTech Connect

    Hayes, Steven L.

    2006-12-01

    The U.S. Advanced Fuel Cycle Initiative (AFCI), now within the broader context of the Global Nuclear Energy Partnership (GNEP), seeks to develop and demonstrate the technologies needed to transmute the long-lived transuranic actinide isotopes contained in spent nuclear fuel into shorter-lived fission products, thereby dramatically decreasing the volume of material requiring disposal and the long-term radio-toxicity and heat load of high-level waste sent to a geologic repository. One important component of the technology development is actinide-bearing metallic transmutation fuel forms containing plutonium, neptunium, americium (and possibly curium) isotopes. The proposed AFC-2A and AFC-2B irradiation experiments are a continuation of the metallic fuel test series in progress in the ATR. This report documents the experiment description and test matrix of the proposed experiments and the Post Irradiation Examination (PIE) and fabrication schedule.

  19. Irradiation of Metallic Fuels with Rare Earth Additions for Actinide Transmutation in the ATR. Experiment Description for AFC-2A and AFC-2B

    SciTech Connect

    S. L. Hayes; D. J. Utterbeck; T. A. Hyde

    2006-11-01

    The U.S. Advanced Fuel Cycle Initiative (AFCI), now within the broader context of the Global Nuclear Energy Partnership (GNEP), seeks to develop and demonstrate the technologies needed to transmute the long-lived transuranic actinide isotopes contained in spent nuclear fuel into shorter-lived fission products, thereby dramatically decreasing the volume of material requiring disposal and the long-term radio-toxicity and heat load of high-level waste sent to a geologic repository. One important component of the technology development is actinide-bearing metallic transmutation fuel forms containing plutonium, neptunium, americium (and possibly curium) isotopes. The proposed AFC-2A and AFC-2B irradiation experiments are a continuation of the metallic fuel test series in progress in the ATR. This report documents the experiment description and test matrix of the proposed experiments and the Post Irradiation Examination (PIE) and fabrication schedule.

  20. Stable isotope signatures for characterising the biological stability of landfilled municipal solid waste

    SciTech Connect

    Wimmer, Bernhard; Hrad, Marlies; Huber-Humer, Marion; Watzinger, Andrea; Wyhlidal, Stefan; Reichenauer, Thomas G.

    2013-10-15

    Highlights: ► The isotopic signature of δ{sup 13}C-DIC of leachates is linked to the reactivity of MSW. ► Isotopic signatures of leachates depend on aerobic/anaerobic conditions in landfills. ► In situ aeration of landfills can be monitored by isotope analysis in leachate. ► The isotopic analysis of leachates can be used for assessing the stability of MSW. ► δ{sup 13}C-DIC of leachates helps to define the duration of landfill aftercare. - Abstract: Stable isotopic signatures of landfill leachates are influenced by processes within municipal solid waste (MSW) landfills mainly depending on the aerobic/anaerobic phase of the landfill. We investigated the isotopic signatures of δ{sup 13}C, δ{sup 2}H and δ{sup 18}O of different leachates from lab-scale experiments, lysimeter experiments and a landfill under in situ aeration. In the laboratory, columns filled with MSW of different age and reactivity were percolated under aerobic and anaerobic conditions. In landfill simulation reactors, waste of a 25 year old landfill was kept under aerobic and anaerobic conditions. The lysimeter facility was filled with mechanically shredded fresh waste. After starting of the methane production the waste in the lysimeter containments was aerated in situ. Leachate and gas composition were monitored continuously. In addition the seepage water of an old landfill was collected and analysed periodically before and during an in situ aeration. We found significant differences in the δ{sup 13}C-value of the dissolved inorganic carbon (δ{sup 13}C-DIC) of the leachate between aerobic and anaerobic waste material. During aerobic degradation, the signature of δ{sup 13}C-DIC was mainly dependent on the isotopic composition of the organic matter in the waste, resulting in a δ{sup 13}C-DIC of −20‰ to −25‰. The production of methane under anaerobic conditions caused an increase in δ{sup 13}C-DIC up to values of +10‰ and higher depending on the actual reactivity of the MSW

  1. Small-scale studies of roasted ore waste reveal extreme ranges of stable mercury isotope signatures

    NASA Astrophysics Data System (ADS)

    Smith, Robin S.; Wiederhold, Jan G.; Jew, Adam D.; Brown, Gordon E.; Bourdon, Bernard; Kretzschmar, Ruben

    2014-07-01

    Active and closed Hg mines are significant sources of Hg contamination to the environment, mainly due to large volumes of mine waste material disposed of on-site. The application of Hg isotopes as source tracer from such contaminated sites requires knowledge of the Hg isotope signatures of different materials potentially released to the environment. Previous work has shown that calcine, the waste residue of the on-site ore roasting process, can exhibit distinct Hg isotope signatures compared with the primary ore. Here, we report results from a detailed small-scale study of Hg isotope variations in calcine collected from the closed New Idria Hg mine, San Benito County, CA, USA. The calcine samples exhibited different internal layering features which were investigated using optical microscopy, micro X-ray fluorescence, micro X-ray absorption spectroscopy (μ-XAS), and stable Hg isotope analysis. Significant Fe, S, and Hg concentration gradients were found across the different internal layers. Isotopic analyses revealed an extreme variation with pronounced isotopic gradients across the internal layered features. Overall, δ202Hg (±0.10‰, 2 SD) describing mass-dependent fractionation (MDF) ranged from -5.96 to 14.49‰, which is by far the largest range of δ202Hg values reported for any environmental sample. In addition, Δ199Hg (±0.06‰, 2 SD) describing mass-independent fractionation (MIF) ranged from -0.17 to 0.21‰. The μ-XAS analyses suggested that cinnabar and metacinnabar are the dominant Hg-bearing phases in the calcine. Our results demonstrate that the incomplete roasting of HgS ores in Hg mines can cause extreme mass-dependent Hg isotope fractionations at the scale of individual calcine pieces with enrichments in both light and heavy Hg isotopes relative to the primary ore signatures. This finding has important implications for the application of Hg isotopes as potential source tracers for Hg released to the environment from closed Hg mines and

  2. The zinc stable isotope signature of waste rock drainage in Arctic Canada

    NASA Astrophysics Data System (ADS)

    Matthies, Romy; Blowes, David

    2014-05-01

    Leachate emerging from a pilot-scale waste rock pile of the Diavik diamond mine, Northwest Territories, was monitored. The well-characterized waste rock consists of granite, pegmatitic granite and biotite schist with an average total sulfur and carbonate carbon concentration of 0.053 and 0.027 wt. %, respectively. During the field seasons of 2011 and 2012, the Zn stable isotope footprint was characterized alongside standard monitoring parameters. pH ranged between 4.3 and 6.8 and carbonate alkalinity was low or undetectable. Al and Fe concentrations averaged 6.78 mg L-1 and 175 µg L-1, respectively. The pH and metal mobility were governed by sulfide oxidation and sorption and co-precipitation onto iron and aluminium hydroxides. The main processes controlling zinc mobility in the range of 0.4 and 4.7 mg L-1 was the oxidative dissolution of sphalerite (ZnS) in the biotite schist and the attenuation of zinc onto secondary iron and aluminium hydroxides and desorption upon the pH declining below the pHpzc. The isotope ratios between -0.16 and +0.19 ‰ (δ66Zn, avg = +0.05 ‰, n = 43) are consistent with values reported from other sphalerite containing deposits. Zn isotope ratios and concentrations were largely uncorrelated suggesting that the processes affecting Zn mobility had little or no impact on the Zn isotope signature. Data indicate, that the Zn isotope ratios of the waste rock leachate may be used as a fingerprint to track anthropogenic, mine-derived Zn sources under varying environmental conditions.

  3. Trends in actinide processing at Hanford

    SciTech Connect

    Harmon, H.D.

    1993-09-01

    In 1989, the mission at the Hanford Site began a dramatic and sometimes painful transition. The days of production--as we used to know it--are over. Our mission officially has become waste management and environmental cleanup. This mission change didn`t eliminate many jobs--in fact, budgets have grown dramatically to support the new mission. Most all of the same skilled crafts, engineers, and scientists are still required for the new mission. This change has not eliminated the need for actinide processing, but it has certainly changed the focus that our actinide chemists and process engineers have. The focus used to be on such things as increasing capacity, improving separations efficiency, and product purity. Minimizing waste had become a more important theme in recent years and it is still a very important concept in the waste management and environmental cleanup arena. However, at Hanford, a new set of words dominates the actinide process scene as we work to deal with actinides that still reside in a variety of forms at the Hanford Site. These words are repackage, stabilize, remove, store and dispose. Some key activities in each of these areas are described in this report.

  4. 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.

  5. 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.

  6. Isotope production potential at Sandia National Laboratories: Product, waste, packaging, and transportation

    SciTech Connect

    Trennel, A.J.

    1995-12-31

    The U.S. Congress directed the U.S. Department of Energy to establish a domestic source of molybdenum-99, an essential isotope used in nuclear medicine and radiopharmacology. An Environmental Impact Statement for production of {sup 99}Mo at one of four candidate sites is being prepared. As one of the candidate sites, Sandia National Laboratories is developing the Isotope Production Project. Using federally approved processes and procedures now owned by the U.S. Department of Energy, and existing facilities that would be modified to meet the production requirements, the Sandia National Laboratories` Isotope Project would manufacture up to 30 percent of the U.S. market, with the capacity to meet 100 percent of the domestic need if necessary. This paper provides a brief overview of the facility, equipment, and processes required to produce isotopes. Packaging and transportation issues affecting both product and waste are addressed, and the storage and disposal of the four low-level radioactive waste types generated by the production program are considered. Recommendations for future development are provided.

  7. 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.

  8. 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.

  9. 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

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 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.

  15. 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)

  16. Recovery of transplutonium elements from nuclear reactor waste

    DOEpatents

    Campbell, David O.; Buxton, Samuel R.

    1977-05-24

    A method of separating actinide values from nitric acid waste solutions resulting from reprocessing of irradiated nuclear fuels comprises oxalate precipitation of the major portion of actinide and lanthanide values to provide a trivalent fraction suitable for subsequent actinide/lanthanide partition, exchange of actinide and lanthanide values in the supernate onto a suitable cation exchange resin to provide an intermediate-lived raffinate waste stream substantially free of actinides, and elution of the actinide values from the exchange resin. The eluate is then used to dissolve the trivalent oxalate fraction prior to actinide/lanthanide partition or may be combined with the reprocessing waste stream and recycled.

  17. 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.

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

    SciTech Connect

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

    1982-03-01

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

  19. Spectroscopic investigation of actinide speciation in concentrated chloride solution

    SciTech Connect

    Runde, W.; Neu, M.P.; Conradson, S.D.; Clark, D.L.; Palmer, P.D.; Reilly, S.D.; Scott, B.L.; Tait, C.D.

    1997-12-31

    The proposed disposal of nuclear waste in geological salt formations, e.g., the Waste Isolation Pilot Plant (USA) and the Gorleben site (Germany), raises a fundamental question: To what degree actinides will be solubilized and mobilized upon interaction with chloride ions? Actinide solubilities in highly concentrated chloride solutions are about one order of magnitude higher than in similar inert electrolyte (NaClO{sub 4}) solutions. This increased solubility is due to interactions between actinide and chloride ions. Contradictory results exist regarding the interaction mechanism between actinide and chloride ions. Specifically, both inner-sphere complex formation and ion pair association have been implicated in the interpretation of spectrophotometric and extraction data. To address this controversy, the authors investigated the interaction between actinide ions in the (III), (IV), (V) and (VI) oxidation states and chloride ions using a multi-method approach. Spectroscopic techniques (TRLFS, Raman, UV-Vis absorption, EXAFS) were used to distinguish between changes in the inner coordination sphere of the actinide ion and effects of ion pairing, X-ray absorption spectroscopy and single crystal X-ray diffraction were used to determine structural details of the actinide chloro complexes formed in solution and solid states.

  20. 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.

  1. 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.

  2. 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.

  3. Use of tracers and isotopes to evaluate vulnerability of water in domestic wells to septic waste

    USGS Publications Warehouse

    Verstraeten, Ingrid M.; Fetterman, G.S.; Meyer, M.J.; Bullen, T.; Sebree, S.K.

    2005-01-01

    In Nebraska, a large number (>200) of shallow sand-point and cased wells completed in coarse alluvial sediments along rivers and lakes still are used to obtain drinking water for human consumption, even though construction of sand-point wells for consumptive uses has been banned since 1987. The quality of water from shallow domestic wells potentially vulnerable to seepage from septic systems was evaluated by analyzing for the presence of tracers and multiple isotopes. Samples were collected from 26 sand-point and perforated, cased domestic wells and were analyzed for bacteria, coliphages, nitrogen species, nitrogen and boron isotopes, dissolved organic carbon (DOC), prescription and nonprescription drugs, or organic waste water contaminants. At least 13 of the 26 domestic well samples showed some evidence of septic system effects based on the results of several tracers including DOC, coliphages, NH4+, NO3-, N2, ?? 15N[NO3-] and boron isotopes, and antibiotics and other drugs. Sand-point wells within 30 m of a septic system and <14 m deep in a shallow, thin aquifer had the most tracers detected and the highest values, indicating the greatest vulnerability to contamination from septic waste. Copyright ?? 2005 National Ground Water Association.

  4. Research in actinide chemistry

    SciTech Connect

    Not Available

    1991-01-01

    This report contains research results on studies of inorganic and organic complexes of actinide and lanthanide elements. Special attention is given to complexes of humic acids and to spectroscopic studies.

  5. 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)

  6. 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.

  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. 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.

  9. 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.

  10. 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)

  11. Measurement of trace uranium-235 and plutonium-239, 240 in waste tank material at the Savannah River Site

    SciTech Connect

    Mahannah, F.N.; Maxwell, S.L. III.

    1992-01-01

    At the Savannah River Site (SRS), large quantities of radioactive liquid waste are evaporated to reduce volume before eventual processing through the In-Tank Precipitation process. Actinides in the liquid waste are only slightly soluble in the highly alkaline waste solution. Since some of the actinide isotopes are fissionable, the quantities being processed through the evaporator system are of interest. To better quantify the concentration and mass of fissionable material entering the evaporator system and eventually deposited as salt, analysis of the actinide elements were necessary. The predominant fissionable actinide isotopes of interest are U{sup 235} and Pu{sup 239}. To enable the reliable measurement of these radionuclides, the Central Laboratory has developed high speed separation techniques to measure U{sup 235} content by Isotope Dilution Mass Spectrometry and Pu{sup 239,240} by alpha spectrometry. Due to the high radioactivity levels in the samples all separations are performed in shielded analytical cells. Uranium is purified and concentrated using a high speed extraction chromatography technique that employs applied vacuum and columns containing tri (2-ethylene) phosphate solvent coated on a small particle inert support. The uranium method enables measurement of U{sup 235} concentrations to 1 {times} 10{sup {minus}4} g/L. Plutonium is purified and concentrated using a high speed anion exchange technique. The Pu method enables measurements of Pu{sup 239,240} to 2 {times} 10{sup {minus}6} g/L.

  12. Measurement of trace uranium-235 and plutonium-239, 240 in waste tank material at the Savannah River Site

    SciTech Connect

    Mahannah, F.N.; Maxwell, S.L. III

    1992-08-01

    At the Savannah River Site (SRS), large quantities of radioactive liquid waste are evaporated to reduce volume before eventual processing through the In-Tank Precipitation process. Actinides in the liquid waste are only slightly soluble in the highly alkaline waste solution. Since some of the actinide isotopes are fissionable, the quantities being processed through the evaporator system are of interest. To better quantify the concentration and mass of fissionable material entering the evaporator system and eventually deposited as salt, analysis of the actinide elements were necessary. The predominant fissionable actinide isotopes of interest are U{sup 235} and Pu{sup 239}. To enable the reliable measurement of these radionuclides, the Central Laboratory has developed high speed separation techniques to measure U{sup 235} content by Isotope Dilution Mass Spectrometry and Pu{sup 239,240} by alpha spectrometry. Due to the high radioactivity levels in the samples all separations are performed in shielded analytical cells. Uranium is purified and concentrated using a high speed extraction chromatography technique that employs applied vacuum and columns containing tri (2-ethylene) phosphate solvent coated on a small particle inert support. The uranium method enables measurement of U{sup 235} concentrations to 1 {times} 10{sup {minus}4} g/L. Plutonium is purified and concentrated using a high speed anion exchange technique. The Pu method enables measurements of Pu{sup 239,240} to 2 {times} 10{sup {minus}6} g/L.

  13. Inductively Coupled Plasma/Mass Spectrometric Isotopic Determination of Nuclear Wastes Sources Associated with Hanford Tank Leaks

    SciTech Connect

    Evans, John C.; Dresel, P. Evan; Farmer, Orville T.

    2007-11-01

    The subsurface distribution of a nuclear waste tank leak on the U.S. Department of Energy’s Hanford Site was sampled by slant drilling techniques in order to characterize the chemical and radiological characteristics of the leaked material and assess geochemical transport properties of hazardous constituents. Sediment core samples recovered from the borehole were subjected to distilled water and acid leaching procedures with the resulting leachates analyzed for isotopic and chemical signatures. High-sensitivity inductively coupled plasma/mass spectrometry (ICP/MS) techniques were used for determination of isotopic ratios for Cs, I, Mo. Analysis of the isotopic patterns of I and Mo combined with associated chemical data showed evidence for at least two separate intrusions of nuclear waste into the subsurface. Isotopic data for Cs was inconclusive with respect to a source attribution signature.

  14. Measurement of enhanced radium isotopes in oil production wastes in Turkey.

    PubMed

    Parmaksız, A; Ağuş, Y; Bulgurlu, F; Bulur, E; Öncü, T; Özkök, Y Ö

    2015-03-01

    Gamma dose rates of oil production equipment and wastes were measured externally by survey meter. They were found to be between 0.2 μSv h(-1) and 25.7 μSv h(-1). Activity concentrations of radium isotopes in crude oil, scale, sludge, contaminated soil and water samples were determined by gamma spectrometric method. Activity concentrations of (224)Ra, (226)Ra and (228)Ra in samples varied from MDA to 132,000 Bq kg(-1). Radium isotopes enriched up to 14,667 times in scale samples. The highest value of (226)Ra was found to be 35,122 ± 1,983 Bq kg(-1) for sludge samples. Activity concentrations of a considerable number of samples were found to be higher than the exemption level recommended by IAEA. Measurement results revealed that oil production wastes caused soil contamination up to 70,483 Bq kg(-1). They may pose a radiological risk for workers and members of the public.

  15. 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.

  16. Identifying source correlation parameters for hydrocarbon wastes using compound-specific isotope analysis.

    PubMed

    Hough, Rupert L; Whittaker, Martin; Fallick, Anthony E; Preston, Tom; Farmer, John G; Pollard, Simon J T

    2006-10-01

    A preliminary evaluation of compound-specific isotope analysis (CSIA) as a novel, alternative method for identifying source correlation compounds in soils contaminated with residual heavy or weathered petroleum wastes is presented. Oil-contaminated soil microcosms were established using soil (sandy-loam, non-carbonaceous cley) amended with ballast-, crude- or No.6 fuel oil. Microcosms were periodically sampled over 256 days and delta(13)C values (which express the ratio of (13)C to (12)C) determined at each time point for five n-alkanes and the isoprenoid norpristane using gas chromatography-isotope ratio mass spectrometry (GC-IRMS). Although some temporal variation was observed, no significant temporal shifts in the delta(13)C values for the five n-alkanes were measured in all three oils. Isoprenoid isotope ratios (delta(13)C) appeared to be least affected by biotransformation, especially in the No.6 fuel oil. The research suggests that the delta(13)C of isoprenoids such as norpristane, may be of use as source correlation parameters.

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

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  18. 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.

  19. 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.

  20. 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.

  1. Enhancing VVER Annular Proliferation Resistance Fuel with Minor Actinides

    SciTech Connect

    G. S. Chang

    2007-06-01

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

  2. Nitrous oxide and methane emissions and nitrous oxide isotopic composition from waste incineration in Switzerland

    SciTech Connect

    Harris, Eliza; Zeyer, Kerstin; Kegel, Rainer; Müller, Beat; Emmenegger, Lukas; Mohn, Joachim

    2015-01-15

    Highlights: • N{sub 2}O emissions from waste incineration with SNCR NO{sub x} removal are 51.5 ± 10.6 g t{sup −1}. • This is significantly lower than the reported Swiss emission factor of 120 g t{sup −1} (FOEN, 2013). • N{sub 2}O contributes <0.3% and ≈2.5% of GHG emissions from SCR and SNCR plants. • Measured isotopic SP of 17.7‰ is likely characteristic for N{sub 2}O emissions from SNCR. • CH{sub 4} emitted by waste incineration is negligible, contributing <0.01% to total GHGs. - Abstract: Solid waste incineration accounts for a growing proportion of waste disposal in both developed and developing countries, therefore it is important to constrain emissions of greenhouse gases from these facilities. At five Swiss waste incineration facilities with grate firing, emission factors for N{sub 2}O and CH{sub 4} were determined based on measurements of representative flue gas samples, which were collected in Tedlar bags over a one year period (September 2010–August 2011) and analysed with FTIR spectroscopy. All five plants burn a mixture of household and industrial waste, and two of the plants employ NO{sub x} removal through selective non-catalytic reduction (SNCR) while three plants use selective catalytic reduction (SCR) for NO{sub x} removal. N{sub 2}O emissions from incineration plants with NO{sub x} removal through selective catalytic reduction were 4.3 ± 4.0 g N{sub 2}O tonne{sup −1} waste (wet) (hereafter abbreviated as t{sup −1}) (0.4 ± 0.4 g N{sub 2}O GJ{sup −1}), ten times lower than from plants with selective non-catalytic reduction (51.5 ± 10.6 g N{sub 2}O t{sup −1}; 4.5 ± 0.9 g N{sub 2}O GJ{sup −1}). These emission factors, which are much lower than the value of 120 g N{sub 2}O t{sup −1} (10.4 g N{sub 2}O GJ{sup −1}) used in the 2013 Swiss national greenhouse gas emission inventory, have been implemented in the most recent Swiss emission inventory. In addition, the isotopic composition of N{sub 2}O emitted from the two

  3. The OSMOSE program for the qualification of integral cross sections of actinides: Preliminary results in a PWR-UOx spectrum

    SciTech Connect

    Hudelot, J. P.; Antony, M.; Bernard, D.; Fougeras, P.

    2006-07-01

    The need for improved nuclear data for minor actinides has been stressed by various organizations throughout the world - especially for studies relating to plutonium management, waste incineration, transmutation of waste, and Pu burning in future nuclear concepts. Several international programs have indicated a strong desire to obtain accurate integral reaction rate data for improving the major and minor actinides cross sections. Data on major actinides (i.e. {sup 235}U, {sup 236}U, {sup 238}U, {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu and {sup 241}Am) are reasonably well-known and available in the Evaluated Nuclear Data Files (JEFF, JENDL, ENDF-BX However information on the minor actinides (i.e. {sup 232}Th, {sup 233}U, {sup 237}Np, {sup 238}Pu, {sup 242}Am, {sup 243}Am, {sup 243}Cm, {sup 235}Cm, {sup 244}Cm, {sup 245}Cm, {sup 246}Cm and {sup 247}Cm) is less well-known and considered to be relatively poor in some cases, having to rely on model and extrapolation of few data points. In this framework, the ambitious OSMOSE program between the Commissariat a l'Energie Atomique (CEA), Electricite de France (EDF) and the U.S. Dept. of Energy (DOE) has been undertaken with the aim of measuring the integral absorption rate parameters of actinides in the MINERVE experimental facility located at the CEA Cadarache Research Center. The OSMOSE Program (Oscillation in Minerve of isotopes in 'Eupraxic' Spectra) includes a complete analytical program associated with the experimental measurement program and aims at understanding and resolving potential discrepancies between calculated and measured values. In the OSMOSE program, the reactivity worth of samples containing separated actinides are measured in different neutron spectra using an oscillation technique with an overall expected accuracy better than 3%. Reactivity effects of less than 10 pcm (0.0001 or approximately 1.5 cents) are measured and compared with calibrations to determine the differential reactivity

  4. The Transmutation of Nuclear Waste in the Two-Zone Subcritical System Driven by High- Intensity Neutron Generator - 12098

    SciTech Connect

    Babenko, V.O.; Gulik, V.I.; Pavlovych, V.M.

    2012-07-01

    The main problems of transmutation of high-level radioactive waste (minor actinides and long-lived fission products) are considered in our work. The range of radioactive waste of nuclear power is analyzed. The conditions under which the transmutation of radioactive waste will be most effective are analyzed too. The modeling results of a transmutation of the main radioactive isotopes are presented and discussed. The transmutation of minor actinides and long-lived fission products are modeled in our work (minor actinides - Np-237, Am-241, Am-242, Am-243, Cm-244, Cm-245; long-lived fission products - I-129, Tc-99). The two-zone subcritical system is calculated with help of different neutron-physical codes (MCNP, Scale, Montebarn, Origen). The ENDF/B-VI nuclear data library used in above calculations. Thus, radioactive wastes can be divided into two main groups that need to be transmuted. The minor actinides form the first group and the long-lived fission products form the second one. For the purpose of effective transmutation these isotopes must be extracted from the spent nuclear fuel with the help of either PUREX technology or pyrometallurgical technology. The two-zone reactor system with fast and thermal regions is more effective for nuclear waste transmutation than the one-zone reactor. Modeling results show that nearly all radioactive wastes can be transmuted in the two-zone subcritical system driven by a high-intensity neutron generator with the external neutron source strength of 1.10{sup 13} n/sec. Obviously, transmutation rate will increase with a rise of the external neutron source strength. From the results above we can also see that the initial loading of radioactive isotopes into the reactor system should exceed by mass those isotopes that are finally produced. (authors)

  5. MICELLE FORMATION AND SURFACE INTERATIONS IN SUPERCRITICAL CO. FUNDAMENTAL STUDIES FOR THE EXTRACTION OF ACTINIDES FROM CONTAMINATED SURFACES.

    SciTech Connect

    McCleskey, T Mark

    2001-06-01

    We are examining the potential of water in CO? microemulsions as a new medium for the extraction of metal ions from contaminated surfaces with the ultimate goal of extracting actinides from heterogeneous waste to aid in decontamination and waste reduction,

  6. 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.

  7. A Summary of Actinide Enrichment Technologies and Capability Gaps

    SciTech Connect

    Patton, Bradley D.; Robinson, Sharon M.

    2017-01-01

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

  8. Phosphorus dynamics in soils irrigated with reclaimed waste water or fresh water - A study using oxygen isotopic composition of phosphate

    USGS Publications Warehouse

    Zohar, I.; Shaviv, A.; Young, M.; Kendall, C.; Silva, S.; Paytan, A.

    2010-01-01

    Transformations of phosphate (Pi) in different soil fractions were tracked using the stable isotopic composition of oxygen in phosphate (??18Op) and Pi concentrations. Clay soil from Israel was treated with either reclaimed waste water (secondary, low grade) or with fresh water amended with a chemical fertilizer of a known isotopic signature. Changes of ??18Op and Pi within different soil fractions, during a month of incubation, elucidate biogeochemical processes in the soil, revealing the biological and the chemical transformation impacting the various P pools. P in the soil solution is affected primarily by enzymatic activity that yields isotopic equilibrium with the water molecules in the soil solution. The dissolved P interacts rapidly with the loosely bound P (extracted by bicarbonate). The oxides and mineral P fractions (extracted by NaOH and HCl, respectively), which are considered as relatively stable pools of P, also exhibited isotopic alterations in the first two weeks after P application, likely related to the activity of microbial populations associated with soil surfaces. Specifically, isotopic depletion which could result from organic P mineralization was followed by isotopic enrichment which could result from preferential biological uptake of depleted P from the mineralized pool. Similar transformations were observed in both soils although transformations related to biological activity were more pronounced in the soil treated with reclaimed waste water compared to the fertilizer treated soil. ?? 2010 Elsevier B.V.

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

    SciTech Connect

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

    2010-02-18

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

  10. Liquid centrifugation for nuclear waste partitioning

    SciTech Connect

    Bowman, C.D.

    1992-03-11

    The performance of liquid centrifugation for nuclear waste partitioning is examined for the Accelerator Transmutation of Waste Program currently under study at the Los Alamos National Laboratory. Centrifugation might have application for the separation of the LiF-BeF{sub 2} salt from heavier radioactive materials fission product and actinides in the separation of fission product from actinides, in the isotope separation of fission-product cesium before transmutation of the {sup 137}Cs and {sup 135}Cs, and in the removal of spallation product from the liquid lead target. It is found that useful chemical separations should be possible using existing materials for the centrifuge construction for all four cases with the actinide fraction in fission product perhaps as low as 1 part in 10{sup 7} and the fraction of {sup 137}CS in {sup 133}Cs being as low as a few parts in 10{sup 5}. A centrifuge cascade has the advantage that it can be assembled and operated as a completely closed system without a waste stream except that associated with maintenance or replacement of centrifuge components.

  11. 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.

  12. 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.

  13. 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.

  14. Physics studies of higher actinide consumption in an LMR

    SciTech Connect

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

    1990-01-01

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

  15. 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.

  16. Conjugates of Actinide Chelator-Magnetic Nanoparticles for Used Fuel Separation Technology

    SciTech Connect

    Qiang, You; Paszczynski, Andrzej; Rao, Linfeng

    2011-10-30

    The actinide separation method using magnetic nanoparticles (MNPs) functionalized with actinide specific chelators utilizes the separation capability of ligand and the ease of magnetic separation. This separation method eliminated the need of large quantity organic solutions used in the liquid-liquid extraction process. The MNPs could also be recycled for repeated separation, thus this separation method greatly reduces the generation of secondary waste compared to traditional liquid extraction technology. The high diffusivity of MNPs and the large surface area also facilitate high efficiency of actinide sorption by the ligands. This method could help in solving the nuclear waste remediation problem.

  17. 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.

  18. Analyzing Nuclear Fuel Cycles from Isotopic Ratios of Waste Products Applicable to Measurement by Accelerator Mass Spectrometry

    SciTech Connect

    Biegalski, S R; Whitney, S M; Buchholz, B

    2005-08-24

    An extensive study was conducted to determine isotopic ratios of nuclides in spent fuel that may be utilized to reveal historical characteristics of a nuclear reactor cycle. This forensic information is important to determine the origin of unknown nuclear waste. The distribution of isotopes in waste products provides information about a nuclear fuel cycle, even when the isotopes of uranium and plutonium are removed through chemical processing. Several different reactor cycles of the PWR, BWR, CANDU, and LMFBR were simulated for this work with the ORIGEN-ARP and ORIGEN 2.2 codes. The spent fuel nuclide concentrations of these reactors were analyzed to find the most informative isotopic ratios indicative of irradiation cycle length and reactor design. Special focus was given to long-lived and stable fission products that would be present many years after their creation. For such nuclides, mass spectrometry analysis methods often have better detection limits than classic gamma-ray spectroscopy. The isotopic ratios {sup 151}Sm/{sup 146}Sm, {sup 149}Sm/{sup 146}Sm, and {sup 244}Cm/{sup 246}Cm were found to be good indicators of fuel cycle length and are well suited for analysis by accelerator mass spectroscopy.

  19. Detection of Septic System Waste in the Groundwaters of Southern California Using Emerging Contaminants and Isotopic Tracers

    NASA Astrophysics Data System (ADS)

    Huang, W.; Conkle, J.; Sickman, J. O.; Lucero, D.; Pang, F.; Gan, J.

    2011-12-01

    In California, groundwater supplies 30-40% of the State's water and in rapidly growing regions like the Inland Empire, groundwater makes up 80-90% of the municipal water supply. However, anthropogenic contamination could adversely affect groundwater quality and thereby reduce available supplies. Appropriate tracers are needed to identify groundwater contamination and protect human health. Stable isotopes δ15N and δ 18O offer unique information about the importance of nitrate sources and processes affecting nitrate in aquifers. We investigated the influence of septic systems on groundwater quality in and around the city of Beaumont, CA during 2010-11. Groundwater samples were collected from 38 active wells and 10 surface water sites in the region (urban and natural streams, agricultural drainage and groundwater recharge basins supplied by the California State Water Project). Stable isotopes and pharmaceuticals and personal care products (PPCPs) were analyzed for all the water samples. The variations of δ15N and δ 18O of nitrate were 2 - 21 per mil and -4 - 9 per mil respectively. δ15N-NO3 values greater than 10 per mil have been associated with nitrate inputs from sewage and animal waste, but in the Beaumont wells, PPCP concentrations were at or below the detection limit in most wells with high isotope ratios. We also observed a strong linear relationship between δ15N and δ 18O of nitrate (slope of~ 0.5) in the vast majority of our samples including those with high isotope ratios. Our results suggest that denitrification was widespread in the Beaumont aquifer and strongly affected the isotope composition of nitrate. In some wells, PPCPs (carbamazepine, sulfamethoxazole, primidone, meprobamate and diuron) and isotope measurements indicated inputs from human waste, but these sites were affected primarily by local waste-water treatment plant effluent. A mixing model was developed using multiple tracers to determine sources and contributions of groundwater

  20. 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

  1. Enhancing BWR Proliferation Resistance Fuel with Minor Actinides

    SciTech Connect

    Gray S. Chang

    2009-03-01

    To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced light water reactor- LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides (237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu/Pu. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO2 fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate-term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm3) to the top (0.35 g/cm3) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. The concept of MARA, which involves the use of transuranic nuclides (237Np and/or 241Am), significantly increases the 238Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms

  2. Environmental behavior of actinides

    NASA Astrophysics Data System (ADS)

    Choppin, G. R.

    2006-01-01

    Since the plutonium concentration in ocean waters is quite low, most of the plutonium deposited in marine waters has been sorbed onto plants and sediments. Actinides in natural waters usually are not in a state of thermodynamic equilibrium for long time periods as their solubility and migration behavior is strongly related to the form in which the nuclides are introduced initially into the aquatic system for long time periods. Their solubility depends on pH (hydrolysis), E H (oxidation state), reaction with complexants (e.g., carbonate, phosphate, humic acid, etc.), sorption to surfaces of minerals and/or colloids, etc. The primary variable is the oxidation state of the actinide cation. Actinides can be present in more than one oxidation state which complicates modeling actinide environmental behavior. Np(V)O 2 + and Pu(V)O 2 + are weakly complexing and resistant to hydrolysis and subsequent precipitation, but both can undergo reduction to the IV oxidation state. The solubility of NpO 2 + can be as high as 10-4M, while that of PuO 2 + is more limited as the very low solubility of Pu(OH)4 promotes reduction to Pu(IV). The solubility of hexavalent UO 2 2+ in sea water is limited by hydrolysis, but has a relatively high concentration due to carbonate complexation. Americium(III) hydroxocarbonate, Am(CO3)(OH), is the limiting species for the solubility of Am(III) in sea water. Thorium has a very low solubility due to the formation of Th(OH)4.

  3. Combined Extraction of Cesium, Strontium, and Actinides from Alkaline Media: An Extension of the Caustic-Side Solvent Extraction (CSSX) Process Technology

    SciTech Connect

    Kenneth Raymond

    2004-11-03

    The wastes present at DOE long-term storage sites are usually highly alkaline, and because of this, much of the actinides in these wastes are in the sludge phase. Enough actinide materials still remain in the supernatant liquid that they require separation followed by long-term storage in a geological repository. The removal of these metals from the liquid waste stream would permit their disposal as low-level waste and dramatically reduce the volume of high-level wastes.

  4. 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.

  5. Applications of UThPb isotope systematics to the problems of radioactive waste disposal

    USGS Publications Warehouse

    Stuckless, J.S.

    1986-01-01

    mobility can be obtained through the use of isotopic studies. Such information can be extremely important in the search for favorable hosts for containment of radioactive waste. Rocks such as the Go??temar Granite have undergone considerable rock-water interaction, most of which occurred ??? 400 Myr. ago and little in recent times. Thus a search for zones that have experienced only a little interaction with water may provide a misleading prediction as to the ability of such zones to shield radioactive wastes from the modern biosphere. From an isotopic point of view, an ideal candidate for evaluation as a host rock for radioactive wastes would have the following characteristics: (1) a high ratio (> 2) of radiogenic to common Pb in order to optimize precision of the results; (2) a simple two-stage geologic history so that results could be interpreted without multiple working hypotheses; and (3) an originally high percentage (> 50%) of labile U so that the results would be highly sensitive to even small amount of rock-water interaction. These characteristics should produce rocks with marked radioactive disequilibrium in surface samples. The disequilibrium should grade to radioactive equilibrium with increasing depth until zones in which water has not circulated are found. Extensive regions of such zones must exist because UThPb systematics of most analyzed granitoids demonstrate closed-system behavior for almost all of their history except for their recent history in the near-surface environment. ?? 1986.

  6. 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.

  7. Emissions of molecular hydrogen (H2) and its isotopic signature from residential heaters and waste incinerators

    NASA Astrophysics Data System (ADS)

    Vollmer, M. K.; Walter, S.; Mohn, J.; Steinbacher, M.; Bond, S. W.; Roeckmann, T.; Reimann, S.

    2011-12-01

    Atmospheric molecular hydrogen (H2) has recently received increased interest in the scientific community because of a potential shift to a global hydrogen energy economy which could potentially alter the atmospheric budget of H2 due to substantial leakage. This calls for an improved understanding of the present day's atmospheric H2 budget. One of the major sources of H2 are emissions from incomplete combustion of fossil fuel. While emissions of H2 from car exhaust have been studied extensively, those from fossil fuel based heating systems have remained a matter of speculation. Here we present results from measurements of a variety of residential heating systems covering oil, gas, and wood heating with various burner capacities. For oil and gas heating systems we surprisingly find no net H2 emissions, i.e. the exhaust air contains H2 at or below the mole fractions of the intake air (approx. 0.5 ppm). While H2 emissions are virtually absent, those of carbon monoxide (CO) are not. As a consequence, caution has to be exercised when modeling H2 emissions based on assumed H2/CO ratios and using CO emission inventories. We also find that the molecular hydrogen in the approx. 0.5 ppm exhaust air is isotopically strongly depleted (-20 permil to -200 permil) compared to the ambient air (+130 permil). This suggests that H2 is involved in the combustion processes, and therefore the H2 of the intake air is not the same H2 in the exhaust air. Exhausts from waste incinerator plants are generally also depleted in H2 mole fractions and in their H/D isotopic composition.

  8. Radioactive waste disposal via electric propulsion

    NASA Technical Reports Server (NTRS)

    Burns, R. E.

    1975-01-01

    It is shown that space transportation is a feasible method of removal of radioactive wastes from the biosphere. The high decay heat of the isotopes powers a thermionic generator which provides electrical power for ion thrust engines. The massive shields (used to protect ground and flight personnel) are removed in orbit for subsequent reuse; the metallic fuel provides a shield for the avionics that guides the orbital stage to solar system escape. Performance calculations indicate that 4000 kg. of actinides may be removed per Shuttle flight. Subsidiary problems - such as cooling during ascent - are discussed.

  9. 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.

  10. Isotopic variability of mercury in ore, mine-waste calcine, and leachates of mine-waste calcine from areas mined for mercury

    USGS Publications Warehouse

    Stetson, S.J.; Gray, J.E.; Wanty, R.B.; Macalady, D.L.

    2009-01-01

    The isotopic composition of mercury (Hg) was determined in cinnabar ore, mine-waste calcine (retorted ore), and leachates obtained from water leaching experiments of calcine from two large Hg mining districts in the U.S. This study is the first to report significant mass-dependent Hg isotopic fractionation between cinnabar ore and resultant calcine. Data indicate that ??202Hg values relative to NIST 3133 of calcine (up to 1.52???) in the Terlingua district, Texas, are as much as 3.24??? heavier than cinnabar (-1.72???) prior to retorting. In addition, ??202Hg values obtained from leachates of Terlingua district calcines are isotopically similar to, or as much as 1.17??? heavier than associated calcines, most likely due to leaching of soluble, byproduct Hg compounds formed during ore retorting that are a minor component in the calcines. As a result of the large fractionation found between cinnabar and calcine, and because calcine is the dominant source of Hg contamination from the mines studied, ??202Hg values of calcine may be more environmentally important in these mined areas than the primary cinnabar ore. Measurement of the Hg isotopic composition of calcine is necessary when using Hg isotopes for tracing Hg sources from areas mined for Hg, especially mine water runoff. ?? 2009 American Chemical Society.

  11. Isotopic variability of mercury in ore, mine-waste calcine, and leachates of mine-waste calcine from areas mined for mercury.

    PubMed

    Stetson, Sarah J; Gray, John E; Wanty, Richard B; Macalady, Donald L

    2009-10-01

    The isotopic composition of mercury (Hg) was determined in cinnabar ore, mine-waste calcine (retorted ore), and leachates obtained from water leaching experiments of calcine from two large Hg mining districts in the U.S. This study is the first to report significant mass-dependent Hg isotopic fractionation between cinnabar ore and resultant calcine. Data indicate that delta202Hg values relative to NIST 3133 of calcine (up to 1.52 per thousand) in the Terlingua district, Texas, are as much as 3.24 per thousand heavier than cinnabar (-1.72 per thousand) prior to retorting. In addition, delta202Hg values obtained from leachates of Terlingua district calcines are isotopically similar to, or as much as 1.17 per thousand heavier than associated calcines, most likely due to leaching of soluble, byproduct Hg compounds formed during ore retorting that are a minor component in the calcines. As a result of the large fractionation found between cinnabar and calcine, and because calcine is the dominant source of Hg contamination from the mines studied, delta202Hg values of calcine may be more environmentally important in these mined areas than the primary cinnabar ore. Measurement of the Hg isotopic composition of calcine is necessary when using Hg isotopes for tracing Hg sources from areas mined for Hg, especially mine water runoff.

  12. 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.

  13. A glass-encapsulated calcium phosphate wasteform for the immobilization of actinide-, fluoride-, and chloride-containing radioactive wastes from the pyrochemical reprocessing of plutonium metal

    NASA Astrophysics Data System (ADS)

    Donald, I. W.; Metcalfe, B. L.; Fong, S. K.; Gerrard, L. A.; Strachan, D. M.; Scheele, R. D.

    2007-03-01

    Chloride-containing radioactive wastes are generated during the pyrochemical reprocessing of Pu metal. Immobilization of these wastes in borosilicate glass or Synroc-type ceramics is not feasible due to the very low solubility of chlorides in these hosts. Alternative candidates have therefore been sought including phosphate-based glasses, crystalline ceramics and hybrid glass/ceramic systems. These studies have shown that high losses of chloride or evolution of chlorine gas from the melt make vitrification an unacceptable solution unless suitable off-gas treatment facilities capable of dealing with these corrosive by-products are available. On the other hand, both sodium aluminosilicate and calcium phosphate ceramics are capable of retaining chloride in stable mineral phases, which include sodalite, Na 8(AlSiO 4) 6Cl 2, chlorapatite, Ca 5(PO 4) 3Cl, and spodiosite, Ca 2(PO 4)Cl. The immobilization process developed in this study involves a solid state process in which waste and precursor powders are mixed and reacted in air at temperatures in the range 700-800 °C. The ceramic products are non-hygroscopic free-flowing powders that only require encapsulation in a relatively low melting temperature phosphate-based glass to produce a monolithic wasteform suitable for storage and ultimate disposal.

  14. 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.

  15. Disposition of nuclear waste using subcritical accelerator-driven systems

    SciTech Connect

    Venneri, F.; Li, N.; Williamson, M.; Houts, M.; Lawrence, G.

    1998-12-31

    Spent fuel from nuclear power plants contains large quantities of Pu, other actinides, and fission products (FP). This creates challenges for permanent disposal because of the long half-lives of some isotopes and the potential for diversion of the fissile material. Two issues of concern for the US repository concept are: (1) long-term radiological risk peaking tens-of-thousands of years in the future; and (2) short-term thermal loading (decay heat) that limits capacity. An accelerator-driven neutron source can destroy actinides through fission, and can convert long-lived fission products to shorter-lived or stable isotopes. Studies over the past decade have established that accelerator transmutation of waste (ATW) can have a major beneficial impact on the nuclear waste problem. Specifically, the ATW concept the authors are evaluating: (1) destroys over 99.9% of the actinides; (2) destroys over 99.9% of the Tc and I; (3) separates Sr-90 and Cs-137; (4) separates uranium from the spent fuel; (5) produces electric power.

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

    NASA Astrophysics Data System (ADS)

    Warin, Dominique

    2010-03-01

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

  17. Silicon isotope ratio measurements by inductively coupled plasma tandem mass spectrometry for alteration studies of nuclear waste glasses.

    PubMed

    Gourgiotis, Alkiviadis; Ducasse, Thomas; Barker, Evelyne; Jollivet, Patrick; Gin, Stéphane; Bassot, Sylvain; Cazala, Charlotte

    2017-02-15

    High-level, long-lived nuclear waste arising from spent fuel reprocessing is vitrified in silicate glasses for final disposal in deep geologic formations. In order to better understand the mechanisms driving glass dissolution, glass alteration studies, based on silicon isotope ratio monitoring of (29)Si-doped aqueous solutions, were carried out in laboratories. This work explores the capabilities of the new type of quadrupole-based ICP-MS, the Agilent 8800 tandem quadrupole ICP-MS/MS, for accurate silicon isotope ratio determination for alteration studies of nuclear waste glasses. In order to avoid silicon polyatomic interferences, a new analytical method was developed using O2 as the reaction gas in the Octopole Reaction System (ORS), and silicon isotopes were measured in mass-shift mode. A careful analysis of the potential polyatomic interferences on SiO(+) and SiO2(+) ion species was performed, and we found that SiO(+) ion species suffer from important polyatomic interferences coming from the matrix of sample and standard solutions (0.5M HNO3). For SiO2(+), no interferences were detected, and thus, these ion species were chosen for silicon isotope ratio determination. A number of key settings for accurate isotope ratio analysis like, detector dead time, integration time, number of sweeps, wait time offset, memory blank and instrumental mass fractionation, were considered and optimized. Particular attention was paid to the optimization of abundance sensitivity of the quadrupole mass filter before the ORS. We showed that poor abundance sensitivity leads to a significant shift of the data away from the Exponential Mass Fractionation Law (EMFL) due to the spectral overlaps of silicon isotopes combined with different oxygen isotopes (i.e. (28)Si(16)O(18)O(+), (30)Si(16)O(16)O(+)). The developed method was validated by measuring a series of reference solutions with different (29)Si enrichment. Isotope ratio trueness, uncertainty and repeatability were found to be <0

  18. 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.

  19. 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

  20. 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)

  1. 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.

  2. 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.

  3. 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.

  4. 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)

  5. Proliferation Resistance Evaluation of ACR-1000 Fuel with Minor Actinides

    SciTech Connect

    Gray S. Chang

    2008-09-01

    The Global Nuclear Energy Partnership (GNEP) program is to significantly advance the science and technology of nuclear energy systems and to enhance the spent fuel proliferation resistance. It consists of both innovative nuclear reactors and innovative research in separation and transmutation. The merits of nuclear energy are high-density energy, with low environmental impacts (i.e. almost zero greenhouse gas emission). Planned efforts involve near-term and intermediate-term improvements in fuel utilization and recycling in current light water reactors (LWRs) as well as the longer-term development of new nuclear energy systems that offer much improved fuel utilization and proliferation resistance, along with continued advances in operational safety. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. MAs can play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In this work, an Advanced CANDU Reactor (ACR) fuel unit lattice cell model with 43 UO2 fuel rods will be used to investigate the effectiveness of a Minor Actinide Reduction Approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance. The main MARA objective is to increase the 238Pu / Pu isotope ratio by using the transuranic nuclides (237Np and 241Am) in the high burnup fuel and thereby increase the proliferation resistance even for a very low fuel burnup. As a result, MARA is a very effective approach to enhance the proliferation resistance for the on power refueling ACR system nuclear fuel. The MA transmutation characteristics at different MA loadings were compared and their impact on neutronics

  6. Reflections on the criticality of special actinide elements

    SciTech Connect

    Clayton, E.D.

    1987-04-01

    During recent years, the list of nuclides known to be capable of supporting a chain reaction has substantially increased. Since the criticality aspects for some of these nuclides differ in important respects from those of the most common fissile nuclides, /sup 235//sub 92/U, and /sup 239//sub 94/Pu, a new term, ''fissible'' was recently proposed in nuclear engineering to help distinguish differences. Activation energies for fission have been calculated for 41 of the actinide isotopes which are grouped according to four types of nuclides, those with even-Z, even-N, odd-Z, odd-N, odd-Z, even-N, and even-Z, odd-N. With the possible exception of /sup 237//sub 92/U, all fissible isotopes listed have even N. The activation energy for fission is less in the case of the even-Z, even-N isotopes, but almost without eception it is the odd-N isotopes that undergo fission with thermal neutrons and which constitute the principal criticality problem. This paper reviews the criticality and fissionability aspects of the fissile and fissible actinide isotopes. The criticality of aqueous mixtures of fissile and fissible isotopes also is briefly discussed, including limits for criticality control.

  7. Purification of alkaline solutions and wastes from actinides and technetium by coprecipitation with some carriers using the method of appearing reagents: Final Report

    SciTech Connect

    Peretrukhin, V.F.; Silin, V.I.; Kareta, A.V.; Gelis, A.V.; Shilov, V.P.; German, K.E.; Firsova, E.V.; Maslennikov, A.G.; Trushina, V.E.

    1998-09-01

    The coprecipitation of transuranium elements (TRU) and technetium from alkaline solutions and from simulants of Hanford Site tank wastes has been studied in reducing and oxidizing conditions on uranium(IV,VI) hydroxocompounds, tetraalkylammonium perrhenate and perchlorate, and on hydroxides of Fe(III), Co(III), Mn(II), and Cr(III) using the method of appearing reagents (MAR). Coprecipitations in alkaline solution have been shown to give high decontamination factors (DF) at low content of carrier and in the presence of high salt concentrations. Uranium(IV) hydroxide in concentrations higher than 3 {times} 10{sup {minus}3} M coprecipitates Pu and Cm in any oxidation state from 0.2 to 4 M NaOH with DFs of 110 to 1000 and Np and Tc with DFs of 51 to 176. Technetium (VII) coprecipitates with (5 to 8) {times} 10{sup {minus}4} M tetrabutylammonium (TBA) perrhenate in 0.01 to 0.02 M TBA hydroxide from 0.5 to 1.5 M NaOH to give DFs of 150 to 200. Coprecipitations of Np and Pu with Co(OH){sub 3}, Fe(OH){sub 3}, Cr(OH){sub 3}, and Mn(OH){sub 2} obtained by the MAR from precursors in the range from pH 10.5 to 0.4 M NaOH give DFs from 80 to 400.

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

    PubMed

    Rao, Linfeng

    2007-06-01

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

  9. Actinide-lanthanide separation with solvents on the base of amides of heterocyclic diacids

    SciTech Connect

    Babain, V.A.; Alyapyshev, M.Y.; Tkachenko, L.I.

    2013-07-01

    The separation of actinides from lanthanides with a particular emphasis on Am(III) from Eu(III) with amides of heterocyclic dicarboxylic diacids was reviewed. It was shown that the di-amides of the 2,2'-dipyridyl-6,6'-dicarboxylic acid are the most promising ligands for the simultaneous selective recovery of actinides from HLLW (high level radioactive liquid waste) within the GANEX concept. (author)

  10. 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)

  11. Actinide transmutation in nuclear reactors

    SciTech Connect

    Ganev, I.K.; Lopatkin, A.V.; Naumov, V.V.; Tocheny, L.V.

    1993-12-31

    Of some interest is the comparison between the actinide nuclide burning up (fission) rates such as americium 241, americium 242, curium 244, and neptunium 237, in the reactors with fast or thermal neutron spectra.

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

    SciTech Connect

    Kenneth L. Nash

    2009-09-22

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

  13. 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

  14. Isotopic identification of the source of methane in subsurface sediments of an area surrounded by waste disposal facilities

    USGS Publications Warehouse

    Hackley, Keith C.; Liu, Chao-Li; Trainor, D.

    1999-01-01

    The major source of methane (CH4) in subsurface sediments on the property of a former hazardous waste treatment facility was determined using isotopic analyses measured on CH4 and associated groundwater. The site, located on an earthen pier built into a shallow wetland lake, has had a history of waste disposal practices and is surrounded by landfills and other waste management facilities. Concentrations of CH4 up to 70% were found in the headspace gases of several piezometers screened at 3 different depths (ranging from 8 to 17 m) in lacustrine and glacial till deposits. Possible sources of the CH4 included a nearby landfill, organic wastes from previous impoundments and microbial gas derived from natural organic matter in the sediments. Isotopic analyses included ??13C, ??D, 14C, and 3H on select CH4 samples and ??D and ??18O on groundwater samples. Methane from the deepest glacial till and intermediate lacustrine deposits had ??13C values from -79 to -82???, typical of natural 'drift gas' generated by microbial CO2-reduction. The CH4 from the shallow lacustrine deposits had ??13C values from -63 to -76???, interpreted as a mixture between CH4 generated by microbial fermentation and the CO2-reduction processes within the subsurface sediments. The ??D values of all the CH4 samples were quite negative ranging from -272 to -299???. Groundwater sampled from the deeper zones also showed quite negative ??D values that explained the light ??D observed for the CH4. Radiocarbon analyses of the CH4 showed decreasing 14C activity with depth, from a high of 58 pMC in the shallow sediments to 2 pMC in the deeper glacial till. The isotopic data indicated the majority of CH4 detected in the fill deposits of this site was microbial CH4 generated from naturally buried organic matter within the subsurface sediments. However, the isotopic data of CH4 from the shallow piezometers was more variable and the possibility of some mixing with oxidized landfill CH4 could not be completely

  15. 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.

  16. 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

  17. 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.

  18. 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.

  19. 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.

  20. 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.

  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. Isotopic Tracers for Waste Fluid Tracking and Fluid-Soil Interactions: Hanford, Washington

    SciTech Connect

    DePaolo, Donald J.

    2005-06-01

    The objective of this research is to develop and advance isotopic methods for characterizing fluid flow and chemical transport through the vadose zone to groundwater. Previous research has been concentrated on developing and comparing different isotopic systems (e.g., hydrogen, oxygen and strontium isotopes) for determining fluid infiltration rates and pathways in the vadose zone (e.g., Maher et al., 2003; DePaolo et al., 2004; Singleton et al., in press). The focus of our current efforts is on using the isotopic compositions of different chemical phases (e.g., uranium, nitrate) to track their movement through the vadose zone. Preliminary results indicate that this will be a powerful tool for assessing environmental risks associated with vadose zone contamination.

  3. Developing the Sandia National Laboratories transportation infrastructure for isotope products and wastes

    SciTech Connect

    Trennel, A.J.

    1995-12-31

    Certain radioactive isotopes for North American and especially the United States` needs are enormously important to the medical community and their numerous patients. The most important medical isotope is {sup 99}Mo, which is currently manufactured by Nordion International Inc. in a single, aging reactor operated by Atomic Energy of Canada, Ltd. The reactor`s useful life is expected to end at the turn of the century. Production loss because of reactor shutdown possibilities prompted the US Congress to direct the DOE to provide for a US backup source for this crucial isotope. The SNL Annular Core Research Reactor (ACRR) was evaluated as a site to provide {sup 99}Mo initially and other isotopes that can be economically extracted from the process. Medical isotope production at SNL is a new venture in manufacturing. Should SNL be selected and the project reach the manufacturing stage, SNL would expect to service up to 30% of the US market under normal circumstances as a backup to the Canadian supply with the capability to service 100% should the need arise. The demand for {sup 99}Mo increases each year; hence, the proposed action accommodates growth in demand to meet this increase. The proposed project would guarantee the supply of medical isotopes would continue if either the irradiation or processing activities in Canada were interrupted.

  4. Actinides and Life's Origins

    NASA Astrophysics Data System (ADS)

    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 uranium- and 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 3rd 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. 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

  6. Measurement of uranium and plutonium in solid waste by passive photon or neutron counting and isotopic neutron source interrogation

    SciTech Connect

    Crane, T.W.

    1980-03-01

    A summary of the status and applicability of nondestructive assay (NDA) techniques for the measurement of uranium and plutonium in 55-gal barrels of solid waste is reported. The NDA techniques reviewed include passive gamma-ray and x-ray counting with scintillator, solid state, and proportional gas photon detectors, passive neutron counting, and active neutron interrogation with neutron and gamma-ray counting. The active neutron interrogation methods are limited to those employing isotopic neutron sources. Three generic neutron sources (alpha-n, photoneutron, and /sup 252/Cf) are considered. The neutron detectors reviewed for both prompt and delayed fission neutron detection with the above sources include thermal (/sup 3/He, /sup 10/BF/sub 3/) and recoil (/sup 4/He, CH/sub 4/) proportional gas detectors and liquid and plastic scintillator detectors. The instrument found to be best suited for low-level measurements (< 10 nCi/g) is the /sup 252/Cf Shuffler. The measurement technique consists of passive neutron counting followed by cyclic activation using a /sup 252/Cf source and delayed neutron counting with the source withdrawn. It is recommended that a waste assay station composed of a /sup 252/Cf Shuffler, a gamma-ray scanner, and a screening station be tested and evaluated at a nuclear waste site. 34 figures, 15 tables.

  7. 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.

  8. 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

  9. Developing the Sandia National Laboratories transportation infrastructure for isotope products and wastes

    SciTech Connect

    Trennel, A.J.

    1997-11-01

    The US Department of Energy (DOE) plans to establish a medical isotope project that would ensure a reliable domestic supply of molybdenum-99 ({sup 99}Mo) and related medical isotopes (Iodine-125, Iodine-131, and Xenon-133). The Department`s plan for production will modify the Annular Core Research Reactor (ACRR) and associated hot cell facility at Sandia National Laboratories (SNL)/New Mexico and the Chemistry and Metallurgy Research facility at Los Alamos National Laboratory (LANL). Transportation activities associated with such production is discussed.

  10. 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.

  11. 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.

  12. Estimating evolution of δ13CH4 during methanization of cellulosic waste based on stoichiometric chemical reactions, microbial dynamics and stable carbon isotope fractionation.

    PubMed

    Vavilin, V A

    2012-04-01

    A change in δ(13)CH(4) during mesophilic methanization of cellulosic waste (paper and cardboard) was described using a mathematical model based on stoichiometric chemical reactions, microbial dynamics and the equation for the (13)C isotope accumulation in products including isotope fractionation. In this study, experimental data, previously obtained by Qu et al. (2009), was used to model metabolic pathways of cellulose transformation. A significant change in δ(13)CH(4) occurred in time during cellulosic waste methanization which was in accordance with the model. It was explained by the change in input of acetoclastic and hydrogenotrophic methanogenesis as well as by fractionation of stable carbon isotopes (13)C and (12)C which was much higher for hydrogenotrophic methanogenesis when compared to acetoclastic methanogenesis.

  13. Molecular models for actinide speciation

    SciTech Connect

    Clark, D.L.; Watkin, J.G.; Morris, D.E.; Berg, J.M.

    1994-06-01

    Much effort has been devoted to the development of sensitive spectroscopic techniques for the study of actinide speciation based on the sensitivity of f-f electronic absorption bands to oxidation state and ligation of the actinide ions. These efforts assume that data obtained in such studies will be interpretable in terms of changes in complexation of the metal center. However, the current understanding of 5f electronic structure is based on data from solid state doped single crystals. In those studies, the local coordination geometry about the central actinide ion is maintained in an almost perfect high-symmetry environment and will have little relevance for species in solution where deviations from perfect high symmetry tend to be the rule rather than the exception. The authors have developed a vigorous research program in the systematic preparation and spectroscopic characterization of synthetic actinide complexes (Th, U, Np, and Pu) in which they can control nuclearity, oxidation state, and molecular structure. These complexes have been used to determine how observable electronic transitions are perturbed in response to structural changes in the complex in solution. From the spectra obtained for these model complexes, the authors have found that the f-f transitions naturally fall into obvious groupings by coordination number and symmetry by which they can now differentiate between monomeric, dimeric, and trimeric species in solution. The study of radionuclide speciation is fundamentally important to the determination of radionuclide solubility in the groundwater at Yucca Mountain.

  14. 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

  15. Method for recovery of actinides from refractory oxides thereof using O.sub. F.sub.2

    DOEpatents

    Asprey, Larned B.; Eller, Phillip G.

    1988-01-01

    Method for recovery of actinides from nuclear waste material containing sintered and other oxides thereof 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 destroyed by high temperature reactions with the walls of the reaction vessel. Dioxygen difluoride is readily prepared, stored and transferred to the place of reaction.

  16. Micelle Formation and Surface Interactions in Supercritical CO2. Fundamental Studies for the Extraction of Actinides from Contaminated Surfaces.

    SciTech Connect

    McCleskey, T Mark; Birnbaum, Eva R.

    2000-09-01

    We are examining the potential of water in CO2 microemulsions as a new medium for the extraction of metal ions from contaminated surfaces with the ultimate goal of extracting actinides from heterogeneous waste to aid in decontamination and waste reduction.

  17. Selective Gaseous Extraction: Research, Development and Training for Isotope Production, Final Technical Report

    SciTech Connect

    Bertch, Timothy C,

    2014-03-31

    General Atomics and the University of Missouri Research Reactor (MURR) completed research and development of selective gaseous extraction of fission products from irradiated fuel, which included training and education of MURR students. The process used porous fuel and after irradiation flowed product gases through the fuel to selectively removed desired fission products with the primary goal of demonstrating the removal of rhodium 105. High removal rates for the ruthenium/rhodium (Ru/Rh), tellurium/iodine (Te/I) and molybdenum/technetium (Mo/Tc) series were demonstrated. The success of this research provides for the reuse of the target for further production, significantly reducing the production of actinide wastes relative to processes that dissolve the target. This effort was conducted under DOE funding (DE-SC0007772). General Atomics objective of the project was to conduct R&D on alternative methods to produce a number of radioactive isotopes currently needed for medical and industry applications to include rhodium-105 and other useful isotopes. Selective gaseous extraction was shown to be effective at removing radioisotopes of the ruthenium/rhodium, tellurium/iodine and molybdenum/technetium decay chains while having trace to no quantities of other fission products or actinides. This adds a new, credible method to the area of certain commercial isotope production beyond current techniques, while providing significant potential reduction of process wastes. Waste reduction, along with reduced processing time/cost provides for superior economic feasibility which may allow domestic production under full cost recovery practices. This provides the potential for improved access to domestically produced isotopes for medical diagnostics and treatment at reduced cost, providing for the public good.

  18. Crystalline matrices for the immobilization of plutonium and actinides

    SciTech Connect

    Anderson, E.B.; Burakov, E.E.; Galkin, Ya.B.; Starchenko, V.A.; Vasiliev, V.G.

    1996-05-01

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

  19. The EBR-II X501 Minor Actinide Burning Experiment

    SciTech Connect

    Jon Carmack; S. L. Hayes; M. K. Meyer; H. Tsai

    2008-06-01

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

  20. Innovations in the Assay of Un-Segregated Multi-Isotopic Grade TRU Waste Boxes with SuperHENC and FRAM Technology

    SciTech Connect

    Simpson, A. P.; Barber, S.; Abdurrahman, N. M.

    2006-07-01

    The Super High Efficiency Neutron Coincidence Counter (SuperHENC) was originally developed by BIL Solutions Inc., Los Alamos National Laboratory (LANL) and Rocky Flats Environmental Technology Site (RFETS) for assay of transuranic (TRU) waste in Standard Waste Boxes (SWB) at Rocky Flats. This mobile system was a key component in the shipment of over 4,000 SWBs to the Waste Isolation Pilot Plant (WIPP) in Carlsbad, New Mexico. The system was WIPP certified in 2001 and operated at the site for four years. The success of this system, a passive neutron coincidence counter combined with high resolution gamma spectroscopy, led to the order of two new units, delivered to Hanford in 2004. Several new challenges were faced at Hanford: For example, the original RFETS system was calibrated for segregated waste streams such that metals, plastics, wet combustibles and dry combustibles were separated by 'Item Description Codes' prior to assay. Furthermore, the RFETS mission of handling only weapons grade plutonium, enabled the original SuperHENC to benefit from the use of known Pu isotopics. Operations at Hanford, as with most other DOE sites, generate un-segregated waste streams, with a wide diversity of Pu isotopics. Consequently, the new SuperHENCs are required to deal with new technical challenges. The neutron system's software and calibration methodology have been modified to encompass these new requirements. In addition, PC-FRAM software has been added to the gamma system, providing a robust isotopic measurement capability. Finally a new software package has been developed that integrates the neutron and gamma data to provide a final assay results and analysis report. The new system's performance has been rigorously tested and validated against WIPP quality requirements. These modifications, together with the mobile platform, make the new SuperHENC far more versatile in handling diverse waste streams and allow for rapid redeployment around the DOE complex. (authors)

  1. Specific sequestering agents for iron and the actinides

    SciTech Connect

    Raymond, K.N.

    1983-06-01

    The transuranium actinide ions represent one unique environmental hazard associated with the waste of the nuclear power industry. A major component associated with that waste and a potential hazard is plutonium. The synthesis of metal-ion-specific complexing agents for ions such as Pu(IV) potentially represents a powerful new approach to many of the problems posed by waste treatment. This document is a progress report of a rational approach to the synthesis of such chelating agents based on the similarities of Pu(IV) and Fe(III), the structures of naturally-occurring complexing agents which are highly specific for Fe(III), and the incorporation of the same kinds of ligating groups present in the iron complexes to make octadentate complexes highly specific for plutonium. Both thermodynamic and animal test results indicate that a relatively high degree of success has already been achieved in this aim.

  2. Determination of long-lived Nb isotopes in nuclear power plant wastes.

    PubMed

    Osváth, Szabolcs; Vajda, Nóra; Molnár, Zsuzsa

    2008-01-01

    (94)Nb and (93m)Nb are long-lived radionuclides, produced by thermal and fast neutrons from (93)Nb that is a major component of the Zr alloys used in nuclear reactors. A radiochemical method for the determination of these nuclides has been developed. The separation is based on the insolubility of Nb oxides and the retention of the fluoric complexes on anion exchange resin. The Nb sources are detected by gamma- and X-ray spectrometries. Activity concentrations determined in radioactive waste samples of a nuclear power plant are presented.

  3. Carbon isotopic evidence for biodegradation of organic contaminants in the shallow vadose zone of the radioactive waste management complex

    SciTech Connect

    Conrad, Mark E.; DePaolo, Donald J.

    2003-09-04

    Waste material buried in drums in the shallow subsurface at the Radioactive Waste Management Facility (RWMC) of the Idaho National Engineering and Environmental Laboratory (INEEL) contained significant amounts of organic compounds including lubricating oils and chlorinated solvents. CO{sub 2} concentrations in pore gas samples from monitoring wells in the vicinity of the disposal pits are 3 to 5 times higher than the concentrations in nearby background wells. The stable carbon isotope ratios ({delta}{sup 13}C values) of CO{sub 2} from the disposal pits averaged 2.4. less than CO{sub 2} from the background wells, indicating that the elevated CO{sub 2} concentrations around the pits were derived from source materials with {delta}{sup 13}C values in the range of -24{per_thousand} to -29{per_thousand}. These {delta}{sup 13}C values are typical of lubricating oils, but higher than most solvents. The radiocarbon ({sup 14}C) contents of CO{sub 2} across most of the site were significantly elevated above modern concentrations due to reactor blocks buried in a subsurface vault at the site. However, several samples collected from the high-CO{sub 2} zone on the far side of the RWMC from the reactor blocks had very low {sup 14}C contents (less than 0.13 times modern), confirming production from lubricating oils manufactured from fossil hydrocarbons. The magnitude of the CO{sub 2} anomaly observed at the site is consistent with intrinsic biodegradation rates on the order of 0.5 to 3.0 metric tons of carbon per year.

  4. Method for extracting lanthanides and actinides from acid solutions by modification of Purex solvent

    DOEpatents

    Horwitz, E.P.; Kalina, D.G.

    1984-05-21

    A process has been developed for the extraction of multivalent lanthanide and actinide values from acidic waste solutions, and for the separation of these values from fission product and other values, which utilizes a new series of neutral bi-functional extractants, the alkyl(phenyl)-N, N-dialkylcarbamoylmethylphosphine oxides, in combination with a phase modifier to form an extraction solution. The addition of the extractant to the Purex process extractant, tri-n-butylphosphate in normal paraffin hydrocarbon diluent, will permit the extraction of multivalent lanthanide and actinide values from 0.1 to 12.0 molar acid solutions.

  5. Ion exchange in the atomic energy industry with particular reference to actinide and fission product separation

    SciTech Connect

    Jenkins, I.L.

    1984-01-01

    Reviewed are some of the uses of ion exchange processes used by the nuclear industry for the period April, 1978 to April, 1983. The topics dealt with are: thorium, protactinium, uranium, neptunium, plutonium, americium, cesium and actinide-lanthanide separations; the higher actinides - Cm, Bk, Cf, Es and Fm; fission products; ion exchange in the geological disposal of radioactive waste. Consideration is given to safety in the use of ion exchangers and in safe methods of disposal of such materials. Full scale and pilot plant process descriptions are included as well as summaries of laboratory studies. 130 references.

  6. DEVELOPMENT OF AN IMPROVED SODIUM TITANATE FOR THE PRETREATMENT OF NUCLEAR WASTE AT THE SAVANNAH RIVER SITE

    SciTech Connect

    Hobbs, D

    2008-01-22

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove Cs-137, Sr-90 and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes planned at SRS include sorption of Sr-90 and alpha-emitting radionuclides onto monosodium titanate (MST) and caustic side solvent extraction, for Cs-137 removal. The MST and separated Cs-137 will be encapsulated into a borosilicate glass waste form for eventual entombment at the federal repository. The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes Pu-238, Pu-239 and Pu-240. This paper describes recent results to produce an improved sodium titanate material that exhibits increased removal kinetics and capacity for Sr-90 and alpha-emitting radionuclides compared to the baseline MST material.

  7. 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.

  8. 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)

  9. Estimating evolution of δ(13)CH(4) during methanization of municipal solid waste based on chemical reactions, isotope accumulation in products and microbial ecology.

    PubMed

    Vavilin, V A

    2012-01-01

    Natural isotopic composition in substrate may be used to reveal the metabolic pathways of substrate transformation by microbial community. In this paper, a change in δ(13)CH(4) during methanization of reconstituted municipal solid waste was described using a mathematical model based on stoichiometric chemical reactions, equation for the (13)C isotope accumulation in products at the low natural C(13)/C(12) ratio and microbial ecology. A set of experimental data used in the model was taken from Qu et al. (2009a). According to the model, during mesophilic municipal solid waste methanization initially hydrogenotrophic and further aceticlastic methanogenesis dominated. At the final stage hydrogenotrophic methanogenesis followed by acetate oxidation dominated again. In spite of rather high measured values of δ(13)C for CO(2) above -21‰, a sharp decrease in δ(13)CH(4) from -20‰ to -60‰ at the final stage was explained by a larger fractionation against (13)C during methanogenesis from H(2)/H(2)CO(3) due to a kinetic isotope effect when hydrogenotrophic methanogens preferentially take down light (12)C. The model also confirmed that in thermophilic conditions a comparatively stable value of δ(13)CH(4) about -60‰ measured earlier (Qu et al. 2009b) was due to a dominance of hydrogenotrophic methanogenesis during all methanization process of cardboard waste.

  10. Using S and Pb isotope ratios to trace leaching of toxic substances from an acid-impacted industrial-waste landfill (Pozdatky, Czech Republic).

    PubMed

    Novak, Martin; Pacherova, Petra; Erbanova, Lucie; Veron, Alain J; Buzek, Frantisek; Jackova, Ivana; Paces, Tomas; Rukavickova, Lenka; Blaha, Vladimir; Holecek, Jan

    2012-10-15

    Slightly elevated concentrations of toxic species in waters sampled in the surroundings of a leaky landfill may be both a sign of an approaching contaminant plume, or a result of water-rock interaction. Isotopes can be instrumental in distinguishing between anthropogenic and geogenic species in groundwater. We studied sulfur and lead isotope ratios at an abandoned industrial-waste landfill, located in a densely populated part of Central Europe. Stable isotope variability in space and time was used to follow the movement of a groundwater plume, contaminated with toxic metals (Cd, Cr, Be), in fractured granitoids. Toxic metals had been mobilized from industrial waste by a strong pulse of sulfuric acid, also deposited in the landfill. Both tracers exhibited a wide range of values (δ(34)S between +2.6 and +18.9‰; (206)Pb/(207)Pb between 1.16 and 1.39), which facilitated identification of mixing end-members, and made it possible to assess the sources of the studied species. In situ fractionations did not hinder source apportionment. Influx of contaminated groundwater was observed neither in irrigation wells in a nearby village, nor at distances greater than 300 m from the landfill. Combination of stable isotope tracers can be used as part of an early-warning system in landscapes affected by landfills.

  11. 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.

  12. Prompt fission neutron spectra of actinides

    DOE PAGES

    Capote, R.; Chen, Y. -J.; Hambsch, F. -J.; ...

    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.

  13. Prompt fission neutron spectrum of actinides

    SciTech Connect

    Capote, R.; Chen, Y. -J.; Hambsch, F. J.; Jurado, B.; Lestone, J. P.; Litaize, O.; Morillon, B.; Neudecker, D.; Oberstedt, S.; Ohsawa, T.; Otuka, N.; Pronyaev, V. G.; Saxena, A.; Schmidt, K. H.; Shcherbakov, O. A.; Shu, N. -C.; Smith, D. L.; Talou, P.; Trkov, A.; Tudora, A. C.; Vogt, R.; Vorobyev, A. S.

    2016-01-06

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

  14. 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.

  15. Interactions of microbial exopolymers with actinides

    NASA Astrophysics Data System (ADS)

    Johnson, Mitchell T.; Chitwood, Dawn J.; He, Lee; Neu, Mary P.

    2000-07-01

    The development of viable bioremediation strategies for radionuclide contaminated soils, sediments and ground waters at DOE sites is a formidable challenge. Ubiquitous microorganisms can absorb, oxidize, reduce and/or precipitate actinides and thereby affect the speciation, solubility, bioavailability, and migration of these toxic metals. Actinides can interact directly with microorganisms, i.e., via sorption to the cell wall, and indirectly via reaction with their byproducts, such as extracellular polymers. However, very little is known about the fundamental chemistry of any microbial-actinide interactions or their impact on environmental processes. Our goal is to fully characterize specific microbial-actinide interactions and determine how they may be exploited to effect environmental actinide mobility/immobility and remediation efforts.

  16. 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.

  17. 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.

  18. Fission fragment angular distributions in pre-actinide nuclei

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

  19. 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).

  20. 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.

  1. 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.

  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. Accurate determination of Curium and Californium isotopic ratios by inductively coupled plasma quadrupole mass spectrometry (ICP-QMS) in 248Cm samples for transmutation studies

    SciTech Connect

    Gourgiotis, A.; Isnard, H.; Aubert, M.; Dupont, E.; AlMahamid, I.; Cassette, P.; Panebianco, S.; Letourneau, A.; Chartier, F.; Tian, G.; Rao, L.; Lukens, W.

    2011-02-01

    The French Atomic Energy Commission has carried out several experiments including the mini-INCA (INcineration of Actinides) project for the study of minor-actinide transmutation processes in high intensity thermal neutron fluxes, in view of proposing solutions to reduce the radiotoxicity of long-lived nuclear wastes. In this context, a Cm sample enriched in {sup 248}Cm ({approx}97 %) was irradiated in thermal neutron flux at the High Flux Reactor (HFR) of the Laue-Langevin Institute (ILL). This work describes a quadrupole ICP-MS (ICP-QMS) analytical procedure for precise and accurate isotopic composition determination of Cm before sample irradiation and of Cm and Cf after sample irradiation. The factors that affect the accuracy and reproducibility of isotopic ratio measurements by ICP-QMS, such as peak centre correction, detector dead time, mass bias, abundance sensitivity and hydrides formation, instrumental background, and memory blank were carefully evaluated and corrected. Uncertainties of the isotopic ratios, taking into account internal precision of isotope ratio measurements, peak tailing, and hydrides formations ranged from 0.3% to 1.3%. This uncertainties range is quite acceptable for the nuclear data to be used in transmutation studies.

  4. Heavy actinide cross sections in the /sup 238/U + /sup 248/Cm reaction

    SciTech Connect

    Kratz, J V; Bruechle, W; Gaeggeler, H

    1981-01-01

    Cross sections for the production of Cf, Es, Fm, and Md isotopes in the reactions of 7.4 MeV/u /sup 238/U-ions with /sup 248/Cm targets are presented and discussed. Cross sections for the formation of heavy actinides in the reactions of 7.5 MeV/u /sup 136/Xe and /sup 238/U-projectiles with /sup 238/U-targets are presented for comparison. (WHK)

  5. 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.

  6. Soil and foliar nutrient and nitrogen isotope composition (δ(15)N) at 5 years after poultry litter and green waste biochar amendment in a macadamia orchard.

    PubMed

    Bai, Shahla Hosseini; Xu, Cheng-Yuan; Xu, Zhihong; Blumfield, Timothy J; Zhao, Haitao; Wallace, Helen; Reverchon, Frédérique; Van Zwieten, Lukas

    2015-03-01

    This study aimed to evaluate the improvement in soil fertility and plant nutrient use in a macadamia orchard following biochar application. The main objectives of this study were to assess the effects of poultry litter and green waste biochar applications on nitrogen (N) cycling using N isotope composition (δ(15)N) and nutrient availability in a soil-plant system at a macadamia orchard, 5 years following application. Biochar was applied at 10 t ha(-1) dry weight but concentrated within a 3-m diameter zone when trees were planted in 2007. Soil and leaf samples were collected in 2012, and both soil and foliar N isotope composition (δ(15)N) and nutrient concentrations were assessed. Both soil and foliar δ(15)N increased significantly in the poultry litter biochar plots compared to the green waste biochar and control plots. A significant relationship was observed between soil and plant δ(15)N. There was no influence of either biochars on foliar total N concentrations or soil NH4 (+)-N and NO3 (-)-N, which suggested that biochar application did not pose any restriction for plant N uptake. Plant bioavailable phosphorus (P) was significantly higher in the poultry litter biochar treatment compared to the green waste biochar treatment and control. We hypothesised that the bioavailability of N and P content of poultry litter biochar may play an important role in increasing soil and plant δ(15)N and P concentrations. Biochar application affected soil-plant N cycling and there is potential to use soil and plant δ(15)N to investigate N cycling in a soil-biochar-tree crop system. The poultry litter biochar significantly increased soil fertility compared to the green waste biochar at 5 years following biochar application which makes the poultry litter a better feedstock to produce biochar compared to green waste for the tree crops.

  7. 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.

  8. Development of Biodegradable Isosaccharinate-Containing Foams for Decontamination of Actinides: Thermodynamic and Kinetic Reactions between Isosaccharinate and Actinides on Metal and Concrete Surfaces

    SciTech Connect

    Rai, Dhanpat; Rao, Linfeng; Moore, Robert C.; Bontchev, Ranko; Holt, Kathleen

    2004-06-01

    Actinide contamination of steel and concrete surfaces is a major problem within the DOE complex. Almost all current decontamination technologies rely on removal of the contaminated surface layer by mechanical means or by chemical methods using harsh chemicals. Some of the technologies are ineffective. Others are expensive, labor intensive, and hazardous to workers. Still others create secondary mixed wastes that are not environmentally acceptable. This project seeks fundamental information that will lead to the development of a new and more environmentally acceptable technology for decontamination of actinides, especially Pu, on steel and concrete surfaces. The key component of this technology is isosaccharinate (ISA), a degradation product of cellulose materials that is biodegradable. Isosaccharinate will be incorporated into foams/gels for safe and easy use in decontamination of actinides from steel, concrete, and other surfaces. Thermodynamic data are being developed on ISA species as a function of pH and on ISA interactions with actinides and competing metals [e.g., Fe(III) and Ca(II)] under a wide range of conditions relevant to decontamination of steel and concrete. The efficiency of the ISA containing foams/gels/solutions for decontamination is also being tested. This project builds on capabilities at three different national laboratories, and represents a joint effort between PNNL, LBNL, and SNL.

  9. DEVELOPMENT OF BIODEGRADABLE ISOSACCHARINATE-CONTAINING FOAMS FOR DECONTAMINATION OF ACTINIDES: THERMODYNAMIC AND KINETIC REACTIONS BETWEEN ISOSACCHARINATE AND ACTINIDES ON METAL AND CONCRETE SURFACES

    SciTech Connect

    Rai, Dhanpat; Moore, Robert C.; Linfeng, Rao; Tucker, Mark D.

    2003-06-01

    Actinide contamination of steel and concrete surfaces is a major problem within the DOE complex. Almost all current decontamination technologies rely on removal of the contaminated surface layer by mechanical means or by chemical methods, using harsh chemicals. Some of the technologies are ineffective. Others are expensive, labor intensive, and hazardous to workers. Still others create secondary mixed wastes that are not environmentally acceptable. This project seeks fundamental information that will lead to the development of a new and more environmentally acceptable technology for decontamination of actinides, especially Pu, on steel and concrete surfaces. The key component of this technology is isosaccharinate (ISA), a degradation product of cellulose materials that is biodegradable. Isosaccharinate will be incorporated into foams/gels for safe and easy use in decontamination of actinides from steel, concrete, and other surfaces. Thermodynamic data are being developed on the interactions of ISA with actinides and competing metals [e.g., Fe(III) and Ca(II)] under a wide range of conditions relevant to decontamination of steel and concrete. The efficiency of the ISA containing foams/gels/solutions for decontamination is also being tested. This project builds on capabilities at three different national laboratories, and represents a joint effort between PNNL, LBNL, and SNL.

  10. 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.

  11. 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).

  12. 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.

  13. 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.

  14. DIAMIDE DERIVATIVES OF DIPICOLINIC ACID AS ACTINIDE AND LANTHANIDE EXTRACTANTS IN A VARIATION OF THE UNEX PROCESS

    SciTech Connect

    D. R. Peterman; R. S. Herbst; J. D. Law; R. D. Tillotson; T. G. Garn; T. A. Todd; V. N. Romanovskiy; V. A. Babain; M. Yu. Alyapyshev; I. V. Smirnov

    2007-09-01

    The Universal Extraction (UNEX) process has been developed for simultaneous extraction of cesium, strontium, and actinides from acidic solutions. This process utilizes an extractant consisting of 0.08 M chlorinated cobalt dicarbollide (HCCD), 0.007-0.02 M polyethylene glycol (PEG-400), and 0.02 M diphenyl-N,N-di-n-butylcarbamoylmethylphosphine oxide (Ph2CMPO) in the diluent trifluoromethylphenyl sulfone (CF3C6H5SO2, designated FS-13) and provides simultaneous extraction of Cs, Sr, actinides, and lanthanides from HNO3 solutions. The UNEX process is of limited utility for processing acidic solutions containing large quantities of lanthanides and/or actinides, such as dissolved spent nuclear fuel solutions. These constraints are primarily attributed to the limited concentrations of CMPO (a maximum of ~0.02 M) in the organic phase and limited solubility of the CMPO-metal complexes. As a result, alternative actinide and lanthanide extractants are being investigated for use with HCCD as an improvement for waste processing and for applications where higher concentrations of the metals are present. Our preliminary results indicate that diamide derivatives of dipicolinic acid may function as efficient actinide and lanthanide extractants. The results to be presented indicate that, of the numerous diamides studied to date, the tetrabutyldiamide of dipicolinic acid, TBDPA, shows the most promise as an alternative actinide/lanthanide extractant in the UNEX process.

  15. 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.

  16. 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)

  17. Predictive Modeling in Actinide Chemistry and Catalysis

    SciTech Connect

    Yang, Ping

    2016-05-16

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

  18. DEVELOPMENT OF AN IMPROVED SODIUM TITANATE FOR THE PRETREATMENT OF HIGH LEVEL NUCLEAR WASTE AT THE SAVANNAH RIVER SITE

    SciTech Connect

    Hobbs, D

    2007-11-15

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove Cs-137, Sr-90 and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes planned at SRS include sorption of Sr-90 and alpha-emitting radionuclides onto monosodium titanate (MST) and caustic side solvent extraction, for {sup 137}Cs removal. The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes Pu-238, Pu-239 and Pu-240. This paper describes recent results to produce an improved sodium titanate material that exhibits increased removal kinetics and capacity for Sr-90 and alpha-emitting radionuclides compared to the baseline MST material.

  19. DEVELOPMENT OF AN IMPROVED SODIUM TITANATE FOR THE PRETREATMENT OF HIGH LEVEL NUCLEAR WASTE AT THE SAVANNAH RIVER SITE

    SciTech Connect

    Hobbs D. T.; Poirier, M. R.; Barnes, M. J.; Stallings, M. E.; Nyman, M. D.

    2005-11-22

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 137}Cs, {sup 90}Sr and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes planned at SRS include caustic side solvent extraction, for {sup 137}Cs removal, and sorption of {sup 90}Sr and alpha-emitting radionuclides onto monosodium titanate (MST). The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes {sup 238}Pu, {sup 239}Pu and {sup 240}Pu. This paper describes recent results to produce an improved sodium titanate material that exhibits increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the baseline MST material.

  20. High-temperature vacuum distillation separation of plutonium waste salts

    SciTech Connect

    Garcia, E.

    1996-10-01

    In this task, high-temperature vacuum distillation separation is being developed for residue sodium chloride-potassium chloride salts resulting from past pyrochemical processing of plutonium. This process has the potential of providing clean separation of the salt and the actinides with minimal amounts of secondary waste generation. The process could produce chloride salt that could be discarded as low-level waste (LLW) or low actinide content transuranic (TRU) waste, and a concentrated actinide oxide powder that would meet long-term storage standards (DOE-DTD-3013-94) until a final disposition option for all surplus plutonium is chosen.

  1. 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.

  2. 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.

  3. Feasibility study for the processing of Hanford Site cesium and strontium isotopic sources in the Hanford Waste Vitrification Plant

    SciTech Connect

    Anantatmula, R.P.; Watrous, R.A.; Nelson, J.L.; Perez, J.M.; Peters, R.D.; Peterson, M.E.

    1991-09-01

    The final environmental impact statement for the disposal of defense-related wastes at the Hanford Site (Final Environmental Impact Statement: Disposal of Hanford Defense High-Level, Transuranic and Tank Wastes [HDW-EIS] [DOE 1987]) states that the preferred alternative for disposal of cesium and strontium wastes at the Hanford Site will be to package and ship these wastes to the commercial high-level waste repository. The Record of Decision for this EIS states that before shipment to a geologic repository, these wastes will be packaged in accordance with repository waste acceptance criteria. However, the high cost per canister for repository disposal and uncertainty about the acceptability of overpacked capsules by the repository suggest that additional alternative means of disposal be considered. Vitrification of the cesium and strontium salts in the Hanford Waste Vitrification Plant (HWVP) has been identified as a possible alternative to overpacking. Subsequently, Westinghouse Hanford Company`s (Westinghouse Hanford) Projects Technical Support Office undertook a feasibility study to determine if any significant technical issues preclude the vitrification of the cesium and strontium salts. Based on the information presented in this report, it is considered technically feasible to blend the cesium chloride and strontium fluoride salts with neutralized current acid waste (NCAW) and/or complexant concentrate (CC) waste feedstreams, or to blend the salts with fresh frit and process the waste through the HWVP.

  4. Chemical effects of lanthanides and actinides in glasses determined with electron energy loss spectroscopy

    SciTech Connect

    Fortner, J.A.; Buck, E.C.; Ellison, A.J.G.; Bates, J.K.

    1996-07-01

    Chemical and structural environments of f-electron elements in glasses are the origin of many of the important properties of materials with these elements; thus oxidation state and chemical coordination of lanthanides and actinides in host materials is an important design consideration in optically active glasses, magnetic materials, perovskite superconductors, and nuclear waste materials. We have made use of the line shapes of Ce to determine its oxidation state in alkali borosilicate glasses being developed for immobilization of Pu. Examination of several prototype waste glass compositions with EELS shows that the redox state of Ce doped to 7 wt% could be varied by suitable choice of alkali elements. EELS for a Pu-doped glass illustrate the small actinide N{sub 4}/N{sub 5} intensity ratio and show that the Pu-N{sub 4,5} white line cross section is comparable to that of Gd M{sub 4,5}.

  5. Georgia Institute of Technology research on the Gas Core Actinide Transmutation Reactor (GCATR)

    NASA Technical Reports Server (NTRS)

    Clement, J. D.; Rust, J. H.; Schneider, A.; Hohl, F.

    1976-01-01

    The program reviewed is a study of the feasibility, design, and optimization of the GCATR. The program is designed to take advantage of initial results and to continue work carried out on the Gas Core Breeder Reactor. The program complements NASA's program of developing UF6 fueled cavity reactors for power, nuclear pumped lasers, and other advanced technology applications. The program comprises: (1) General Studies--Parametric survey calculations performed to examine the effects of reactor spectrum and flux level on the actinide transmutation for GCATR conditions. The sensitivity of the results to neutron cross sections are to be assessed. Specifically, the parametric calculations of the actinide transmutation are to include the mass, isotope composition, fission and capture rates, reactivity effects, and neutron activity of recycled actinides. (2) GCATR Design Studies--This task is a major thrust of the proposed research program. Several subtasks are considered: optimization criteria studies of the blanket and fuel reprocessing, the actinide insertion and recirculation system, and the system integration. A brief review of the background of the GCATR and ongoing research is presented.

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

    NASA Astrophysics Data System (ADS)

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

    2015-09-01

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

  7. The EBR-II X501 Minor Actinide Burning Experiment

    SciTech Connect

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

    2008-01-01

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

  8. Actinide Solubility and Speciation in the WIPP [PowerPoint

    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.

  9. 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

  10. 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.

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

    SciTech Connect

    Bouineau, V.; Lainet, M.; Chauvin, N.; Pelletier, M.

    2013-07-01

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

  12. 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.

  13. Nuclear archeology in a bottle: evidence of pre-Trinity U.S. weapons activities from a waste burial site.

    PubMed

    Schwantes, Jon M; Douglas, Matthew; Bonde, Steven E; Briggs, James D; Farmer, Orville T; Greenwood, Lawrence R; Lepel, Elwood A; Orton, Christopher R; Wacker, John F; Luksic, Andrzej T

    2009-02-15

    During World War II, the Hanford Site in Washington became the location for U.S. plutonium production. In 2004, a bottle containing a sample of plutonium was recovered from a Hanford waste trench. Here, state-of-the-art instrumental analyses, reactor model simulations, and investigative science techniques were used to provide insights as to the origin of this unknown sample, a process collectively termed as nuclear archeology. Isotopic age dating conducted on the sample in 2007 indicated the sample was separated from the spent fuel 61.6 +/- 4.5 years earlier. The isotope (22)Na, a detectable product of a secondary nuclear reaction, proved useful as a powerful tool for nuclear forensic analysis as (1) an easily detectable signifier of the presence of alpha emitting actinides, (2) an indicator of sample splitting, and (3) a measure of the time since sample splitting. Analytical results of minor actinide isotopes and reactor model simulations confirmed the material originated from the X-10 reactor in Oak Ridge, TN. Corroborated by historical documents, we concluded this sample was part of the first batch of Pu separated at T-Plant, Hanford, the world's first industrial-scale reprocessing facility, on December 9, 1944. This sample represents the oldest known collection of man-made (239)Pu in the world.

  14. 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.

  15. 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.

  16. The use of alkaline hydrolysis as a novel strategy for chloroform remediation: the feasibility of using construction wastes and evaluation of carbon isotopic fractionation.

    PubMed

    Torrentó, Clara; Audí-Miró, Carme; Bordeleau, Geneviève; Marchesi, Massimo; Rosell, Mònica; Otero, Neus; Soler, Albert

    2014-01-01

    Laboratory and field-scale pilot experiments were performed to evaluate the feasibility of chloroform degradation by alkaline hydrolysis and the potential of δ(13)C values to assess this induced reaction process at contaminated sites. In batch experiments, alkaline conditions were induced by adding crushed concrete (pH 12.33 ± 0.07), a filtered concrete solution (pH 12.27 ± 0.04), a filtered cement solution (pH 12.66 ± 0.02) and a pH 12 buffer solution (pH 11.92 ± 0.11). The resulting chloroform degradation after 28 days was 94, 96, 99, and 72%, respectively. The experimental data were described using a pseudo-first-order kinetic model, resulting in pseudo-first-order rate constant values of 0.10, 0.12, 0.20, and 0.05 d(-1), respectively. Furthermore, the significant chloroform carbon isotopic fractionation associated with alkaline hydrolysis of chloroform (-53 ± 3‰) and its independence from pH in the admittedly limited tested pH range imply a great potential for the use of δ(13)C values for in situ monitoring of the efficacy of remediation approaches based on alkaline hydrolysis. The carbon isotopic fractionation obtained at the lab scale allowed the calculation of the percentage of chloroform degradation in field-scale pilot experiments where alkaline conditions were induced in two recharge water interception trenches filled with concrete-based construction wastes. A maximum of approximately 30-40% of chloroform degradation was achieved during the two studied recharge periods. Although further research is required, the treatment of chloroform in groundwater through the use of concrete-based construction wastes is proposed. This strategy would also imply the recycling of construction and demolition wastes for use in value-added applications to increase economic and environmental benefits.

  17. Subject bibliography of radioactive waste management publications at Pacific Northwest Laboratory, 1975-1978

    SciTech Connect

    Powell, J.A.

    1981-10-01

    This bibliography contains publications from 1975 to 1978 written by PNL staff. PNL translations are also announced in this document. The following areas are covered: actinides; airborne wastes; alternative waste forms; calcination; characterization; containers; decontamination; disposal; high-level wastes; liquid wastes; radionuclide migration; safety; separation processes; soils; solidification; storage; transport; transuranic waste; and vitrification.

  18. On the possibility of radiation equivalent waste disposal

    SciTech Connect

    Adamov, E.O.; Orlov, V.V.; Tocheny, L.V.

    1993-12-31

    The method of radiation equivalent waste disposal due to their long-term controlled cooling, actinides recycle, and burning up and a variety of other measures can be considered for large scale future nuclear power.

  19. FURTHER DEVELOPMENT OF MODIFIED MONOSODIUM TITANATE, AN IMPROVED SORBENT FOR PRETREATMENT OF HIGH LEVEL NUCLEAR WASTE AT THE SAVANNAH RIVER SITE

    SciTech Connect

    Taylor-Pashow, K.; Hobbs, D.; Fondeur, F.; Fink, S.

    2011-01-12

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove Cs-137, Sr-90, and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. Separation processes planned at SRS include caustic side solvent extraction, for Cs-137 removal, and sorption of Sr-90 and alpha-emitting radionuclides onto monosodium titanate (MST). The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes Pu-238, Pu-239, and Pu-240. This paper describes recent results from the development of an improved titanate material that exhibits increased removal kinetics and effective capacity for Sr-90 and alpha-emitting radionuclides compared to the baseline MST material.

  20. 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.

  1. 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.

  2. 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.

  3. Challenges in the quality assurance of elemental and isotopic analyses in the nuclear domain benefitting from high resolution ICP-OES and sector field ICP-MS.

    PubMed

    Krachler, Michael; Alvarez-Sarandes, Rafael; Van Winckel, Stefaan

    Accurate analytical data reinforces fundamentally the meaningfulness of nuclear fuel performance assessments and nuclear waste characterization. Regularly lacking matrix-matched certified reference materials, quality assurance of elemental and isotopic analysis of nuclear materials remains a challenging endeavour. In this context, this review highlights various dedicated experimental approaches envisaged at the European Commission-Joint Research Centre-Institute for Transuranium Elements to overcome this limitation, mainly focussing on the use of high resolution-inductively coupled plasma-optical emission spectrometry (HR-ICP-OES) and sector field-inductively coupled plasma-mass spectrometry (SF-ICP-MS). However, also α- and γ-spectrometry are included here to help characterise extensively the investigated actinide solutions for their actual concentration, potential impurities and isotopic purity.

  4. 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.

  5. Elevated concentrations of actinides in Mono Lake

    SciTech Connect

    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.

  6. 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.

  7. 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.

  8. 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.

  9. Iron (III) Matrix Effects on Mineralization and Immobilization of Actinides

    SciTech Connect

    Cynthia-May S. Gong; Tyler A. Sullens; Kenneth R. Czerwinski

    2006-01-01

    Abstract - A number of models for the Yucca Mountain Project nuclear waste repository use studies of actinide sorption onto well-defined iron hydroxide materials. In the case of a waste containment leak, however, a complex interaction between dissolved waste forms and failed containment vessel components can lead to immediate precipitation of migratory iron and uranyl in the silicate rich near-field environment. Use of the Fe(III) and UO22+ complexing agent acetohydroxamic acid (AHA) as a colorimetric agent for visible spectrophotometry is well-known. Using the second derivative of these spectra a distinct shift in iron complexation in the presence of silicate is seen that is not seen with uranyl or alone. Silica also decreases the ability of uranyl and ferric solutions to absorb hydroxide, hastening precipitation. These ferric silicate precipitates are highly amorphous and soluble. Precipitates formed in the presence of uranyl below ~1 mol% exhibit lower solubility than precipitates from up to 50 mol % and of uranyl silicates alone.

  10. Americium-241: the most useful isotope of the actinide elements

    SciTech Connect

    Navratil, J.D.

    1984-01-01

    Used extensively in nuclear gauges and in many other areas, this man-made element (Atomic Number 95) was first isolated in weighable amounts during World War II. Americium is now a very useful by-product of the nuclear industry and is produced in kilogram amounts by appropriate recovery, separation and purification processes. A review will be presented of its discovery, nuclear and chemical properties, and uses, with emphasis on its production process and separations chemistry.

  11. Utilization of Minor Actinides as a Fuel Component for Ultra-Long Life Bhr Configurations: Designs, Advantages and Limitations

    SciTech Connect

    Dr. Pavel V. Tsvetkov

    2009-05-20

    This project assessed the advantages and limitations of using minor actinides as a fuel component to achieve ultra-long life Very High Temperature Reactor (VHTR) configurations. Researchers considered and compared the capabilities of pebble-bed and prismatic core designs with advanced actinide fuels to achieve ultra-long operation without refueling. Since both core designs permit flexibility in component configuration, fuel utilization, and fuel management, it is possible to improve fissile properties of minor actinides by neutron spectrum shifting through configuration adjustments. The project studied advanced actinide fuels, which could reduce the long-term radio-toxicity and heat load of high-level waste sent to a geologic repository and enable recovery of the energy contained in spent fuel. The ultra-long core life autonomous approach may reduce the technical need for additional repositories and is capable to improve marketability of the Generation IV VHTR by allowing worldwide deployment, including remote regions and regions with limited industrial resources. Utilization of minor actinides in nuclear reactors facilitates developments of new fuel cycles towards sustainable nuclear energy scenarios.

  12. New developments at the INE-Beamline for actinide research at ANKA

    NASA Astrophysics Data System (ADS)

    Dardenne, K.; Brendebach, B.; Denecke, M. A.; Liu, X.; Rothe, J.; Vitova, T.

    2009-11-01

    The INE-Beamline for actinide research at the synchrotron source ANKA is operated by the Institut für Nukleare Entsorgung (INE) at the Forschungszentrum Karlsruhe. Experiments on radioactive samples with activities up to 106 times the limit of exemption inside a safe and flexible double containment concept are possible. One great advantage of the beamline is its close proximity to INE's active laboratories with its equipment for manipulation of actinide materials and state-of-the-art spectroscopic, analytical, and microscopic instrumentation. This constellation is unique in Europe. The INE-Beamline is built primarily to serve INE in-house research associated with safe disposal of high level nuclear waste such as actinide speciation or coordination-, redox-, and geo-chemistry of actinides. A wide energy range from around 2.1 keV to 25 keV covering the K-edges from P to Pd and the L3, L2, and L1 edges for actinides from Th to Cm can be used. The INE-Beamline is optimized for X-ray absorption spectroscopy techniques (XANES/EXAFS), but x-ray fluorescence (XRF) analysis and powder diffraction (XRD) are also possible, as well as surface sensitive measurements in grazing incidence geometry (GI-XAFS). Upgrades of instrumentation and extension of experimental capabilities at the INE-Beamline are driven by user needs. Two of the recent upgrades are presented: 1) installation of a microfocus option for spatially resolved studies (μ-XRF, μ-XANES, μ-XRD) and investigations of small volumes (e.g., heterogeneous natural samples and diamond anvil high pressure cells); 2) construction, and commissioning of a high resolution x-ray emission spectrometer (HRXES); 3) availability of an electrochemical cell for investigation of redox sensitive systems.

  13. Actinide ion extraction using room temperature ionic liquids: opportunities and challenges for nuclear fuel cycle applications.

    PubMed

    Mohapatra, Prasanta Kumar

    2017-02-14

    Studies on the extraction of actinide ions from radioactive feeds have great relevance in nuclear fuel cycle activities, mainly in the back end processes focused on reprocessing and waste management. Room temperature ionic liquid (RTIL) based diluents are becoming increasingly popular due to factors such as more efficient extraction vis-à-vis molecular diluents, higher metal loading, higher radiation resistance, etc. The fascinating chemistry of the actinide ions in RTIL based solvent systems due to complex extraction mechanisms makes it a challenging area of research. By the suitable tuning of the cationic and anionic parts of the ionic liquids, their physical properties such as density, dielectric constant and viscosity can be changed which are considered key parameters in metal ion extraction. Aqueous solubility of the RTILs, which can lead to significant loss in the solvent inventory, can be avoided by appending the extractant moieties onto the ionic liquid. While the low vapour pressure and non-flammability of the ionic liquids make them appear as 'green' diluents, their aqueous solubility raises concerns of environmental hazards. The present article gives a summary of studies carried out on actinide ion extraction and presents perspectives of its applications in the nuclear fuel cycle. The article discusses various extractants used for actinide ion extraction and at many places, comparison is made vis-à-vis molecular diluents which includes the nature of the extracted species and the mechanism of extraction. Results of studies on rare earth elements are also included in view of their similarities with the trivalent minor actinides.

  14. Rapid determination of actinides in urine by inductively coupled plasma mass spectrometry and alpha spectrometry: a hybrid approach.

    PubMed

    Maxwell, Sherrod L; Jones, Vernon D

    2009-11-15

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

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

    SciTech Connect

    Maxwell, S.; Jones, V.

    2009-05-27

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

  16. Oxyhydroxy Silicate Colloids: A New Type of Waterborne Actinide(IV) Colloids

    PubMed Central

    Weiss, Stephan; Hennig, Christoph; Brendler, Vinzenz; Ikeda‐Ohno, Atsushi

    2016-01-01

    Abstract At the near‐neutral and reducing aquatic conditions expected in undisturbed ore deposits or in closed nuclear waste repositories, the actinides Th, U, Np, and Pu are primarily tetravalent. These tetravalent actinides (AnIV) are sparingly soluble in aquatic systems and, hence, are often assumed to be immobile. However, AnIV could become mobile if they occur as colloids. This review focuses on a new type of AnIV colloids, oxyhydroxy silicate colloids. We herein discuss the chemical characteristics of these colloids and the potential implication for their environmental behavior. The binary oxyhydroxy silicate colloids of AnIV could be potentially more mobile as a waterborne species than the well‐known mono‐component oxyhydroxide colloids. PMID:27957406

  17. The Minor Actinide Transmutation-Incineration Potential Studies in High Intensity Neutron Fluxes

    SciTech Connect

    Letourneau, A.; Chabod, S.; Foucher, Y.; Marie, F.; Ridikas, D.; Veyssiere, Ch.; Blandin, Ch.

    2005-05-24

    In the framework of nuclear waste transmutation studies, the Mini-INCA project has been initiated at CEA/DSM with objectives to determine optimal conditions for transmutation and incineration of Minor Actinides (MA) in high intensity neutron fluxes. Our experimental tools based on alpha- and gamma-spectroscopy of irradiated samples and the development of fission micro-chambers could gather both microscopic information on nuclear reactions (total and partial cross sections for neutron capture and/or fission reactions) and macroscopic information on transmutation and incineration potentials. Cross sections of selected actinides (241Am, 242Am, 242Pu, 237Np, 238Np) have already been measured at ILL, showing some discrepancies when compared to evaluated data libraries but in overall good agreement with recent experimental data.

  18. Minor Actinides, Major Challenges, the Needs for and Benefits of International Collaboration

    NASA Astrophysics Data System (ADS)

    Plompen, A. J. M.

    2014-04-01

    The role of experiments for the determination of minor actinide nuclear data is presented as essential to meet the tight uncertainties requirements derived by sensitivity analyses for innovative systems designed to significantly reduce the amount of high level nuclear waste. Recent, ongoing and planned experiments are highlighted emphasizing international collaboration and the European context. Specifically, the role of the MANREAD CRP, the European projects ANDES, ERINDA and EURFRAT, and the NEA databank and WPEC subgroups will be addressed. For 241Am capture and 240Pu fission are used to illustrate the generic situation with minor actinide experimental data and the discrepancy between achieved and target uncertainties. The importance of new high quality experiments, high quality reporting, diversity, new techniques, methods and facilities is stressed.

  19. 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.

  20. Fusion transmutation of waste: design and analysis of the in-zinerator concept.

    SciTech Connect

    Durbin, S. M.; Cipiti, Benjamin B.; Olson, Craig Lee; Guild-Bingham, Avery (Texas A&M University, College Station, TX); Venneri, Francesco (General Atomics, San Diego, CA); Meier, Wayne; Alajo, A.B.; Johnson, T. R.; El-Guebaly, L. A.; Youssef, M. E.; Young, Michael F.; Drennen, Thomas E. (Hobart & William Smith College, Geneva, NY); Tsvetkov, Pavel Valeryevich (Texas A&M University, College Station, TX); Morrow, Charles W.; Turgeon, Matthew C.; Wilson, Paul (University of Wisconsin, Madison, WI); Phruksarojanakun, Phiphat (University of Wisconsin, Madison, WI); Grady, Ryan (University of Wisconsin, Madison, WI); Keith, Rodney L.; Smith, James Dean; Cook, Jason T.; Sviatoslavsky, Igor N. (University of Wisconsin, Madison, WI); Willit, J. L. (Argonne Mational Laboratory, Argonne, IL); Cleary, Virginia D.; Kamery, William; Mehlhorn, Thomas Alan; Rochau, Gary Eugene

    2006-11-01

    Due to increasing concerns over the buildup of long-lived transuranic isotopes in spent nuclear fuel waste, attention has been given in recent years to technologies that can burn up these species. The separation and transmutation of transuranics is part of a solution to decreasing the volume and heat load of nuclear waste significantly to increase the repository capacity. A fusion neutron source can be used for transmutation as an alternative to fast reactor systems. Sandia National Laboratories is investigating the use of a Z-Pinch fusion driver for this application. This report summarizes the initial design and engineering issues of this ''In-Zinerator'' concept. Relatively modest fusion requirements on the order of 20 MW can be used to drive a sub-critical, actinide-bearing, fluid blanket. The fluid fuel eliminates the need for expensive fuel fabrication and allows for continuous refueling and removal of fission products. This reactor has the capability of burning up 1,280 kg of actinides per year while at the same time producing 3,000 MWth. The report discusses the baseline design, engineering issues, modeling results, safety issues, and fuel cycle impact.

  1. Actinide nuclear data for reactor physics calculations

    SciTech Connect

    Brady, M.C.; Wright, R.Q. ); England, T.R. )

    1991-07-01

    Calculational methodologies and data sources used to predict and recommend fission-product yields and delayed neutron and prompt neutron data for a number of actinide nuclides are presented and discussed. This compilation of nuclear data is the result of a nearly three-year effort under the Japan/US Actinide Program (JUSAP) at Oak Ridge National Laboratory to provide nuclear data supporting the preliminary design of an actinide burner reactor. In this type of reactor, minor actinides are the major components of the fuel. Nuclear data for these minor actinides are, therefore, essential in the design of such reactors. Fission yield, delayed neutron, and prompt neutron data are presented in the report for the following nuclides: Neptumium-237, Plutonium-238, -240, and -242, Americium-241 and -243, and Curium-242, -243, -244, -246, and -248. Additionally, prompt neutron data are also presented for these nuclides (except Plutonium-240, -242 and Curium-242) and for Curium-245 and -247. As in all compilations of nuclear data, the information in this report is subject to change as newer data become available. Most of the data presented here are based on calculational methodologies and should be revised as experimental data become available. The release of Version 6 of the Evaluated Nuclear Data Files (ENDF/B-6) is expected to be completed in 1991 and should replace this evaluation in areas of overlap although no serious discrepancies are expected between this compilation and ENDF/B-6. Because of the large amount of data comprising this compilation and limitations in publishing such a voluminous report, a complete listing of the explicit data is not included in this report. The data are, however, available from the authors on 5 {1/2}-in. high-density (1.2-Mbyte) diskettes. The file contents and formats are described in the text, and examples are given in the appendices. 34 refs., 18 tabs.

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

    SciTech Connect

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

    2008-05-30

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

  3. 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.

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

    SciTech Connect

    Allender, Jeffrey S.; Bridges, Nicholas J.; Loftin, Bradley M.; Dunsmuir, Michael D.

    2015-07-14

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

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

    SciTech Connect

    Pagano, Justin

    2016-01-08

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

  6. 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.

  7. In situ subterranean determination of actinides by high-resolution gamma-ray spectrometry

    SciTech Connect

    Brodzinski, R. L.

    1981-04-01

    A system utilizing high resolution germanium diode gamma-ray spectroscopy for the simple, safe, and economical in situ determination of actinides is described. Six isotopes, /sup 235/U, /sup 238/U, /sup 237/Np, /sup 239/Pu, /sup 241/Pu, and /sup 241/Am, can be simultaneously measured at the 10 nCi g/sup -1/ level in less than 7 minutes. Collimators provide for measurement of horizontal strata as thin as 1 cm or solid angles as small as 0.1 steradians. Information obtainable with the system is discussed and compared to that obtainable with neutron activation/detection systems.

  8. Systematic calculation of the fission mode characteristics of the light actinides

    SciTech Connect

    Hambsch, F.-J.; Dematte, L.; Oberstedt, S.

    1998-10-26

    A systematic calculation of the fission mode characteristics of the light actinides in the frame of the multi-modal random neck-rupture model has been started. In particular the isotopes {sup 220,226,232}Th and {sup 220,226}Ac are under investigation. A clear competition between the outer barrier heights of the asymmetric standard and the symmetric superlong fission mode has been found. Their systematic variation with the compound nuclear mass might explain the drastic changes in the nuclear charge distributions recently observed at GSI. The current status will be reported and discussed in the light of the experimental results.

  9. Preparation of higher-actinide burnup and cross section samples. [LMFBR

    SciTech Connect

    Adair, H.L.; Kobisk, E.H.; Quinby, T.C.; Thomas, D.K.; Dailey, J.M.

    1981-01-01

    A joint research program involving the United States and the United Kingdom was instigated about four years ago for the purpose of studying burnup of higher actinides using in-core irradiation in the fast reactor at Dounreay, Scotland. Simultaneously, determination of cross sections of a wide variety of higher actinide isotopes was proposed. Coincidental neutron flux and energy spectral measurements were to be made using vanadium encapsulated dosimetry materials in the immediate region of the burnup and cross section samples. The higher actinide samples chosen for the burnup study were /sup 241/Am and /sup 244/Cm in the forms of Am/sub 2/O/sub 3/, Cm/sub 2/O/sub 3/, and Am/sub 6/ Cm(RE)/sub 7/O/sub 21/, where (RE) represents a mixture of lanthanide sesquioxides. It is the purpose of this paper to describe technology development and its application in the preparation of the fuel specimens and the cross section specimens that are being used in this cooperative program.

  10. Strontium Isotopes in Pore Water as an Indicator of Water Flux at the Proposed High-Level Radioactive Waste Repository, Yucca Mountain, Nevada

    SciTech Connect

    B. Marshall; K. Futa

    2004-02-19

    The proposed high-level radioactive waste repository at Yucca Mountain, Nevada, would be constructed in the high-silica rhyolite (Tptp) member of the Miocene-age Topopah Spring Tuff, a mostly welded ash-flow tuff in the {approx}500-m-thick unsaturated zone. Strontium isotope compositions have been measured in pore water centrifuged from preserved core samples and in leachates of pore-water salts from dried core samples, both from boreholes in the Tptp. Strontium isotope ratios ({sup 87}Sr/{sup 86}Sr) vary systematically with depth in the surface-based boreholes. Ratios in pore water near the surface (0.7114 to 0.7124) reflect the range of ratios in soil carbonate (0.7112 to 0.7125) collected near the boreholes, but ratios in the Tptp (0.7122 to 0.7127) at depths of 150 to 370 m have a narrower range and are more radiogenic due to interaction with the volcanic rocks (primarily non-welded tuffs) above the Tptp. An advection-reaction model relates the rate of strontium dissolution from the rocks with flow velocity. The model results agree with the low transport velocity ({approx}2 cm per year) calculated from carbon-14 data by I.C. Yang (2002, App. Geochem., v. 17, no. 6, p. 807-817). Strontium isotope ratios in pore water from Tptp samples from horizontal boreholes collared in tunnels at the proposed repository horizon have a similar range (0.7121 to 0.7127), also indicating a low transport velocity. Strontium isotope compositions of pore water below the proposed repository in core samples from boreholes drilled vertically downward from tunnel floors are more varied, ranging from 0.7112 to 0.7127. The lower ratios (<0.7121) indicate that some of the pore water in these boreholes was replaced by tunnel construction water, which had an {sup 87}Sr/{sup 86}Sr of 0.7115. Ratios lower than 0.7115 likely reflect interaction of construction water with concrete in the tunnel inverts, which had an {sup 87}Sr/{sup 86}Sr < 0.709. These low Sr ratios indicate penetration of

  11. 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

  12. Use of Information Theory Concepts for Developing Contaminated Site Detection Method: Case for Fission Product and Actinides Accumulation Modeling

    SciTech Connect

    Harbachova, N.V.; Sharavarau, H.A.

    2006-07-01

    Information theory concepts and their fundamental importance for environmental pollution analysis in light of experience of Chernobyl accident in Belarus are discussed. An information and dynamic models of the radionuclide composition formation in the fuel of the Nuclear Power Plant are developed. With the use of code DECA numerical calculation of actinides (58 isotopes are included) and fission products (650 isotopes are included) activities has been carried out and their dependence with the fuel burn-up of the RBMK-type reactor have been investigated. (authors)

  13. 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.

  14. Chemistry of the actinide elements. Second edition

    SciTech Connect

    Katz, J.J.; Seaborg, G.T.; Morss, L.R.

    1987-01-01

    This is an exhaustive, updated discourse on the chemistry of Actinides, Volume 1 contains a systematic coverage of the elements Ac, Th, Pa, U, Np, and Pu, which constitutes Part 1 of the work. The characterization of each element is discussed in terms of its nuclear properties, occurrence, preparation, atomic and metallic properties, chemistry of specific compounds, and solution chemistry. The first part of Volume 2 follows the same format as Volume 1 but is confined to the elements Am, Cm, Bk, Cf, and Es, plus a more condensed coverage of the Transeinsteinium elements (Fm, Md, No, Lw, and 104-109). Part 2 of this volume is devoted to a discussion of the actinide elements in general, with a specific focus on electronic spectra, thermodynamic and magnetic properties, the metallic state, structural chemistry, solution kinetics, organometallic chemistry for /sigma/- and /pi/-bonded compounds, and some concluding remarks on the superheavy elements.

  15. Measurement and calculation of high-actinide burnup in the prototype fast reactor

    SciTech Connect

    Broadhead, B.L.; Raman, S.; Dickens, J.K. )

    1991-01-01

    An agreement was signed in May 1979 as a part of a long-term cooperative program between the United Kingdom and the US under the liquid-metal fast breeder reactor agreement of 1976. This agreement included an experiment to carry out irradiations of physics specimens of fissile and fertile actinides to improve our knowledge of basic nuclear physics phenomena. Three fuel pins were prepared by the US to contain the actinide physics samples; two of these pins were irradiated at the Dounreay prototype fast reactor (PFR) for a total irradiation of 63 full-power days. The third pin has only recently been removed from the PFT, following an irradiation of > 500 full-power days. Each pin houses 35 capsules containing milligram quantities of actinide oxides of {sup 231}Pa, {sup 230}Th, {sup 232}Th, {sup 233}U, {sup 234}U, {sup 235}U, {sup 236}U, {sup 238}U, {sup 237}Np, {sup 238}Pu, {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu, {sup 244}Pu, {sup 241}Am, {sup 243}Am, {sup 243}Cm, {sup 244}Cm, {sup 246}Cm, and {sup 248}Cm. Following the return of the first fuel pin (FP-1) to the United States in May 1984, the actinide samples were prepared for studies of fission product yields, isotopics, and material concentrations. The measurements were repeated for the second fuel pin (FP-2) to remedy several problems encountered in the processing of the FP-1 pin. A brief description of the measured and calculated {sup 137}Cs yields for both FP-1 and FP-2 are included in this paper.

  16. 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.

  17. 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.

  18. Preparation of actinide specimens for the US/UK joint experiment in the Dounreay Prototype Fast Reactor

    SciTech Connect

    Quinby, T C; Adair, H L; Kobisk, E H

    1982-05-01

    A joint research program involving the United States and the United Kingdom was initiated about four years ago for the purpose of studying the fuel behavior of higher actinides using in-core irradiation in the fast reactor at Dounreay, Scotland. Simultaneously, determination of integral cross sections of a wide variety of higher actinide isotopes (physics specimens) was proposed. Coincidental neutron flux and energy spectral measurements were to be made using vanadium encapsulated dosimetry materials in the immediate region of the fuel pellets and physics samples. The higher actinide samples chosen for the fuel study were /sup 241/Am and /sup 244/Cm in the forms of Am/sub 2/O/sub 3/, Cm/sub 2/O/sub 3/, and Am/sub 6/Cm(RE)/sub 7/O/sub 21/, where (RE) represents a mixture of lanthanides. Milligram quantities of actinide oxides of /sup 248/Cm, /sup 246/Cm, /sup 244/Cm, /sup 243/Cm, /sup 243/Am, /sup 241/Am, /sup 244/Pu, /sup 242/Pu, /sup 241/Pu, /sup 240/Pu, /sup 239/Pu, /sup 238/Pu, /sup 237/Np, /sup 238/U, /sup 236/U, /sup 235/U, /sup 234/U, /sup 233/U, /sup 232/Th, /sup 230/Th, and /sup 231/Pa were encapsulated to obtain nuclear cross section and reaction rate data for these materials.

  19. 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.

  20. Actinide and lanthanide separation process (ALSEP)

    DOEpatents

    Guelis, Artem V.

    2013-01-15

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

  1. 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. JOWOG 22/2 - Actinide Chemical Technology (July 9-13, 2012)

    SciTech Connect

    Jackson, Jay M.; Lopez, Jacquelyn C.; Wayne, David M.; Schulte, Louis D.; Finstad, Casey C.; Stroud, Mary Ann; Mulford, Roberta Nancy; MacDonald, John M.; Turner, Cameron J.; Lee, Sonya M.

    2012-07-05

    The Plutonium Science and Manufacturing Directorate provides world-class, safe, secure, and reliable special nuclear material research, process development, technology demonstration, and manufacturing capabilities that support the nation's defense, energy, and environmental needs. We safely and efficiently process plutonium, uranium, and other actinide materials to meet national program requirements, while expanding the scientific and engineering basis of nuclear weapons-based manufacturing, and while producing the next generation of nuclear engineers and scientists. Actinide Process Chemistry (NCO-2) safely and efficiently processes plutonium and other actinide compounds to meet the nation's nuclear defense program needs. All of our processing activities are done in a world class and highly regulated nuclear facility. NCO-2's plutonium processing activities consist of direct oxide reduction, metal chlorination, americium extraction, and electrorefining. In addition, NCO-2 uses hydrochloric and nitric acid dissolutions for both plutonium processing and reduction of hazardous components in the waste streams. Finally, NCO-2 is a key team member in the processing of plutonium oxide from disassembled pits and the subsequent stabilization of plutonium oxide for safe and stable long-term storage.

  3. QUANTIFICATION OF ACTINIDE ALPHA-RADIATION DAMAGE IN MINERALS AND CERAMICS

    SciTech Connect

    Farnan, Ian E.; Cho, Herman M.; Weber, William J.

    2007-01-11

    There are large amounts of heavy alpha-emitters in nuclear waste and nuclear materials inventories stored in various sites around the world. These include plutonium and minor actinides such as americium and curium. In preparation for geological disposal there is a consensus that actinides that have been separated from spent nuclear fuel should be immobilised within mineral-based ceramics rather than glass. Over the long-term, the alpha-decay taking place in these ceramics will severely disrupt their crystalline structure and reduce their durability. A fundamental property in predicting cumulative radiation damage is the number of atoms permanently displaced per alpha–decay. Currently, this number is estimated as 1000-2000 atoms/alpha decay event. Here, we report nuclear magnetic resonance, spin-counting experiments that measure close to 5000 atoms/alpha decay event in radiation damaged natural zircons. New radiological NMR measurements on highly radioactive, 239Pu zircon show damage similar to that created by 238U and 232Th in mineral zircons at the same dose, indicating no significant effect of dose rate. Based on these measurements, the initially crystalline structure of a 10 wt% 239Pu zircon would be amorphous after only 1400 years in a geological repository. These measurements establish a basis for assessing the long-term structural durability of actinide-containing ceramics based on an atomistic understanding of the fundamental damage event.

  4. Long-term test results from a West Valley actinide-doped reference glass

    SciTech Connect

    Fortner, J.A.; Gerding, T.J.; Bates, J.K.

    1995-07-01

    Results from drip tests designed to simulate unsaturated conditions in the proposed Yucca Mountain Repository are reported for an actinide-doped glass (reference glass ATM-10) used as a model waste form. These tests have been ongoing for nearly 7 years, with data collected on solution composition (including transuranics), colloid formation and disposition, glass corrosion layers, and solid secondary phases. This test is unique because of its long elapsed time, high content of thorium and transuranics, use of actual groundwater from the proposed site area, use of contact between the glass and sensitized stainless steel in the test, and the variety of analytical procedures applied to the components. Some tests have been terminated, and scanning electron microscopy (SEM) and analytical transmission electron microscopy (AEM) were used to directly measure glass corrosion and identify secondary phases. Other tests remain ongoing, with periodic sampling of the water that had contacted the glass. The importance of integrated testing has been demonstrated, as complex interactions between the glass, the groundwater, and the sensitized stainless steel have been observed. Secondary phases include smectite clay, iron silicates, and brockite. Actinides, except neptunium, concentrate into stable secondary phases. The release of actinides is then controlled by the behavior of these phases.

  5. 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.

  6. Assessing the subsequent effect of nitrogen released from tobacco-waste on maize crop using a ¹⁵N isotope technique.

    PubMed

    Karaman, M Rüştü; Brohi, A Reşit

    2013-06-01

    The investigation of the residual effect of nitrogen (N) released from tobacco-waste (TW) using isotope techniques will provide valuable data for sustainable organic farming. For this aim, a pot experiment was conducted using the (15)N isotope technique. The experiment was based on a completely randomised design with four replications and was conducted on a calcareous ustochrepts soil. TW at levels of 0, 10, 20, 30 and 40 t ha(-1) and N fertiliser as (NH₄)₂SO₂ at levels of 0, 20, 40, 60 and 80 kg N ha(-1) were used for the Bezostaja-1 wheat variety. Concerning mineral N fertilisation with 20 and 80 kg N ha(-1), additional treatments with (15)N-labelled (NH₄)₂SO₂ (10 at.% exc.) have been applied. Following harvesting wheat plants, the Pioneer 3377 maize variety was used to see the residual effect of TW. After harvesting, dry matter yields were recorded and total N concentrations were determined. (15)N determinations and calculations were also made for (15)N treatments separately. TW had a significant residual effect on the growth of corn plant under the pot condition. Increasing rates of TW significantly increased the dry matter yield of corn plant following wheat from 3.31 t ha(-1) (at control) to 7.89 t ha(-1) (at the TW treatment of 40 t ha(-1)). The (15)N values derived from the (15)N fertiliser decreased with increasing TW application. The average values of N derived from N fertiliser (Ndff) varied from 2.14 to 3.09% at the rates of 20 and 80 kg N ha(-1), respectively. However, N derived from TW (Ndftw) significantly increased from 16.93 to 24.59% (at 20 kg N ha(-1)), and it also increased from 23.06 to 28.15% (at 80 kg N ha(-1)) with increasing TW applications from 20 to 40 t ha(-1), respectively.

  7. Application of gaseous core reactors for transmutation of nuclear waste

    NASA Technical Reports Server (NTRS)

    Schnitzler, B. G.; Paternoster, R. R.; Schneider, R. T.

    1976-01-01

    An acceptable management scheme for high-level radioactive waste is vital to the nuclear industry. The hazard potential of the trans-uranic actinides and of key fission products is high due to their nuclear activity and/or chemical toxicity. Of particular concern are the very long-lived nuclides whose hazard potential remains high for hundreds of thousands of years. Neutron induced transmutation offers a promising technique for the treatment of problem wastes. Transmutation is unique as a waste management scheme in that it offers the potential for "destruction" of the hazardous nuclides by conversion to non-hazardous or more manageable nuclides. The transmutation potential of a thermal spectrum uranium hexafluoride fueled cavity reactor was examined. Initial studies focused on a heavy water moderated cavity reactor fueled with 5% enriched U-235-F6 and operating with an average thermal flux of 6 times 10 to the 14th power neutrons/sq cm-sec. The isotopes considered for transmutation were I-129, Am-241, Am-242m, Am-243, Cm-243, Cm-244, Cm-245, and Cm-246.

  8. Supercritical Carbon Dioxide Ligands for Extracting Actinide Metal Ions from Porous Solids

    SciTech Connect

    Albert W. Herlinger; Dr. Mark L. Dietz

    2003-03-06

    Numerous types of actinide-bearing waste materials are found throughout the DOE complex. Most of these wastes consist of large volumes of non-hazardous materials contaminated with relatively small quantities of actinide elements. Separation of these wastes into their inert and radioactive components would dramatically reduce the costs of stabilization and disposal. For example, the DOE is responsible for decontaminating concrete within 7000 surplus contaminated buildings. The best technology now available for removing surface contamination from concrete involves removing the surface layer by grit blasting, which produces a large volume of blasting residue containing a small amount of radioactive material. Disposal of this residue is expensive because of its large volume and fine particulate nature. Considerable cost savings would result from separation of the radioactive constituents and stabilization of the concrete dust. Similarly, gas diffusion plants for uranium enrichment contain valuable high-purity nickel in the form of diffusion barriers. Decontamination is complicated by the extremely fine pores in these barriers, which are not readily accessible by most cleaning techniques. A cost-effective method for the removal of radioactive contaminants would release this valuable material for salvage.

  9. 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

  10. Molecular hydrogen (H2) combustion emissions and their isotope (D/H) signatures from domestic heaters, diesel vehicle engines, waste incinerator plants, and biomass burning

    NASA Astrophysics Data System (ADS)

    Vollmer, M. K.; Walter, S.; Mohn, J.; Steinbacher, M.; Bond, S. W.; Röckmann, T.; Reimann, S.

    2012-03-01

    Molecular hydrogen (H2), its stable isotope signature (δD), and the key combustion parameters carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were measured from various combustion processes. H2 in the exhaust of gas and oil-fired heaters and of waste incinerator plants was generally depleted compared to ambient intake air, while CO was significantly elevated. These findings contradict the often assumed co-occurring net H2 and CO emissions in combustion processes and suggest that previous H2 emissions from combustion may have been overestimated when scaled to CO emissions. For the heater exhausts, H2 and δD generally decrease with increasing fuel-to-air ratio, from ambient values of ∼0.5 ppm and +130‰ to 0.2 ppm and -206‰, respectively. These results are interpreted as a combination of an isotopically light H2 source from fossil fuel combustion and a D/H kinetic isotope fractionation of hydrogen in the advected ambient air during its partial removal during combustion. Diesel exhaust measurements from dynamometer test stand driving cycles show elevated H2 and CO emissions during cold-start and some acceleration phases. Their molar H2/CO ratios are <0.25, significantly smaller than those for gasoline combustion. Using H2/CO emission ratios, along with CO global emission inventories, we estimate global H2 emissions for 2000, 2005, and 2010. For road transportation (gasoline and diesel), we calculate 8.6 ± 2.1 Tg, 6.3 ± 1.5 Tg, and 4.1 ± 1.0 Tg, respectively, whereas the contribution from diesel vehicles has increased from 5% to 8% over this time. Other fossil fuel emissions are believed to be negligible but H2 emissions from coal combustion are unknown. For residential (domestic) emissions, which are likely dominated by biofuel combustion, emissions for the same years are estimated at 2.7 ± 0.7 Tg, 2.8 ± 0.7 Tg, and 3.0 ± 0.8 Tg, respectively. Our wood combustion measurements are combined with results from the literature to calculate

  11. Simulation of alpha decay of actinides in iron phosphate glasses by ion irradiation

    NASA Astrophysics Data System (ADS)

    Dube, Charu L.; Stennett, Martin C.; Gandy, Amy S.; Hyatt, Neil C.

    2016-03-01

    A surrogate approach of ion beam irradiation is employed to simulate alpha decay of actinides in iron phosphate nuclear waste glasses. Bismuth and helium ions of different energies have been selected for simulating glass matrix modification owing to radiolysis and ballistic damage due to recoil atoms. Structural modification and change in coordination number of network former were probed by employing Reflectance Fourier-Transform Infrared (FT-IR), and Raman spectroscopies as a consequence of ion irradiation. Depolymerisation is observed in glass sample irradiated at intermediate energy of 2 MeV. Helium blisters of micron size are seen in glass sample irradiated at low helium ion energy of 30 keV.

  12. 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.

  13. 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.

  14. French R and D program for minor actinide bearing fuel developments

    SciTech Connect

    Warin, Dominique; Brossard, Philippe; Nabot, Jean-Philippe

    2007-07-01

    One of the main objectives of future Generation IV fast neutron systems is the minimization of waste which will necessitate the recycling of the trans-uranium elements. In order to fulfill this objective, R and D work has to cope with the development of Minor Actinide bearing fuels and, in this context, this paper presents an overview of the results already obtained and the research program to be carried out in the future about fabrication and irradiation behavior at significant scale of such fuels. In France, the results have been obtained, for a large part, thanks to an important experimental irradiation programme using the Phenix fast reactor and the European HFR in Petten. Flux conditions of Phenix are well suited to allow the studies of irradiation damages of fuels and targets for transmutation under representative conditions of fast or partly moderated neutron flux, which are considered to be the most efficient for transmutation of MA. The fuels are now developed for sodium (more mature) and gas (alternative track) fast reactor with in both cases Minor Actinide recycling as a progressive approach in the future nuclear cycles of these reactors. This strategy is based upon the two possible recycling modes: - the homogeneous (using the so called 'GANEX' grouped Transuranics recovery treatment of the irradiated fuel) recycling of Minor Actinides, at low concentration in the standard U-Pu fuel of fast GEN IV systems, - the heterogeneous (using a partitioning process such as the French 'DIAMEX-SANEX') recycling with specific Minor Actinide bearing target in fast critical GEN IV reactors or fuel in sub critical system. (authors)

  15. Synthesis and Characterization of Templated Ion Exchange Resins for the Selective Complexation of Actinide Ions

    SciTech Connect

    Uy, O. Manual

    2001-03-01

    The purpose of this research is to develop a polymeric extractant for the selective complexation of uranyl ions (and subsequently other actinyl and actinide ions) from aqueous solutions (lakes, streams, waste tanks and even body fluids). Chemical insights into what makes a good complexation site will be used to synthesize reagents tailor-made for the complexation of uranyl and other actinide ions. These insights, derived from studies of molecular recognition include ion coordination number and geometry, ionic size and ionic shape, as well as ion to ligand thermodynamic affinity. Selectivity for a specific actinide ion will be obtained by providing the polymers with cavities lined with complexing ligands so arranged as to match the charge, coordination number, coordination geometry, and size of the actinide metal ion. These cavity-containing polymers will be produced by using a specific ion (or surrogate) as a template around which monomeric complexing ligands will be polymerized. The complexing ligands will be ones containing functional groups known to form stable complexes with a specific ion and less stable complexes with other cations. Prior investigator's approaches for making templated resins for metal ions have had marginal success. We have extended and amended these methodologies in our work with Pb(II) and uranyl ion, by changing the order of the steps, by the inclusion of sonication, by using higher complex loading, and the selection of functional groups with better complexation constants. This has resulted in significant improvements to selectivity. The unusual shape of the uranyl ion suggests that this approach will result in even greater selectivities than already observed for Pb(II). Preliminary data obtained for uranyl templated polymers shows unprecedented selectivity and has resulted in the first ion selective electrode for uranyl ion.

  16. Stable carbon ((12/13)C) and nitrogen ((14/15)N) isotopes as a tool for identifying the sources of cyanide in wastes and contaminated soils--a method development.

    PubMed

    Weihmann, Jenny; Mansfeldt, Tim; Schulte, Ulrike

    2007-01-23

    The occurrence of iron-cyanide complexes in the environment is of concern, since they are potentially hazardous. In order to determine the source of iron-cyanide complexes in contaminated soils and wastes, we developed a method based on the stable isotope ratios (13)C/(12)C and (15)N/(14)N of the complexed cyanide-ion (CN(-)). The method was tested on three pure chemicals and two industrials wastes: blast-furnace sludge (BFS) and gas-purifier waste (GPW). The iron-cyanide complexes were converted into the solid cupric ferrocyanide, Cu(2)[Fe(CN)(6)].7H(2)O, followed by combustion and determination of the isotope-ratios by continuous flow isotope ratio mass spectrometry. Cupric ferrocyanide was obtained from the materials by (i) an alkaline extraction with 1M NaOH and (ii) a distillate digestion. The [Fe(CN)(6)](4-) of the alkaline extraction was precipitated after adding Cu(2+). The CN(-) of the distillate digestion was at first complexed with Fe(2+) under inert conditions and then precipitated after adding Cu(2+). The delta(13)C-values obtained by the two methods differed slightly up to 1-3 per thousand for standards and BFS. The difference was larger for alkaline-extracted GPW (4-7 per thousand), since non-cyanide C was co-extracted and co-precipitated. Therefore the distillate digestion technique is recommended when determining the C isotope ratios in samples rich in organic carbon. Since the delta(13)C-values of BFS are in the range of -30 to -24 per thousand and of -17 to -5 per thousand for GPW, carbon seems to be a suitable tracer for identifying the source of cyanide in both wastes. However, the delta(15)N-values overlapped for BFS and GPW, making nitrogen unsuitable as a tracer.

  17. Preparations and mechanism of hydrolysis of ((8)annulene)actinide compounds. [Uranocene

    SciTech Connect

    Moore, R.M. Jr.

    1985-07-01

    The mechanism of hydrolysis for bis(8)annulene actinide and lanthanide complexes has been studied in detail. The uranium complex, uranocene, decomposes with good pseudo-first order kinetics (in uranocene) in 1 M degassed solutions of H/sub 2/O in THF. Decomposition of a series of aryl-substituted uranocenes demonstrates that the hydrolysis rate is dependent on the electronic nature of the substituent (Hammett rho value = 2.1, r/sup 2/ = 0.999), with electron-withdrawing groups increasing the rate. When D/sub 2/O is substituted for H/sub 2/O, kinetic isotope effects of 8 to 14 are found for a variety of substituted uranocenes. These results suggest a pre-equilibrium involving approach of a water molecule to the central metal, followed by rate determining proton transfer to the eight membered ring and rapid decomposition to products. Each of the four protonations of the complex has a significant isotope effect. The product ratio of cyclooctatriene isomers formed in the hydrolysis varies, depending on the central metal of the complex. However, the general mechanism of hydrolysis, established for uranocene, can be extended to the hydrolysis and alcoholysis of all the (8)annulene complexes of the lanthanides and actinides.

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

    SciTech Connect

    Raymond, K.; White, D.; Whisenhunt, D.

    1996-10-01

    The ultimate goal of this project is to develop new separation technologies to remove radioactive metal ions from contaminated DOE sites. To this end we are studying both the fundamental chemistry and the extractant properties of some chelators that are either found in nature or are closely related to natural materials. The work is a collaboration betwen Lawrence Berkeley National Laboratory-University of California, Berkeley, and the Glenn T. Seaborg Institute for Transactinium Science at Lawrence Livermore National Laboratory.

  19. Potential agents for removal of actinides from waste solutions

    SciTech Connect

    Romanovski, V.V.; Whisenhunt, D.W.; Veeck, A.C.; Andersen, W.A.; Hoffman, D.C.; Jide, X.; White, D.; Raymond, K.N.

    1996-07-01

    The uptake of Th(IV) from nitric acid and hydrochloric acid solutions by chelating ion exchange resins containing catechol, 1,2- hydroxypyridinone (1,2-HOPO) and 3,4-hydroxypyridinone (3,4-HOPO) functional groups, has been investigated. These polystyrene based materials show excellent kinetics for uptake of Th(IV) and have a high loading capacity. Liquid/liquid extractants have also been synthesized by addition of lipophilic side chains to the chelating groups (1,2-HOPO; 3,4-HOPO; 3,2-HOPO; catecholamide; terephthalamide). The initial evaluation of the extraction properties has been carried out.

  20. Monte-Carlo Application for Nondestructive Nuclear Waste Analysis

    NASA Astrophysics Data System (ADS)

    Carasco, C.; Engels, R.; Frank, M.; Furletov, S.; Furletova, J.; Genreith, C.; Havenith, A.; Kemmerling, G.; Kettler, J.; Krings, T.; Ma, J.-L.; Mauerhofer, E.; Neike, D.; Payan, E.; Perot, B.; Rossbach, M.; Schitthelm, O.; Schumann, M.; Vasquez, R.

    2014-06-01

    Radioactive waste has to undergo a process of quality checking in order to check its conformance with national regulations prior to its transport, intermediate storage and final disposal. Within the quality checking of radioactive waste packages non-destructive assays are required to characterize their radio-toxic and chemo-toxic contents. The Institute of Energy and Climate Research - Nuclear Waste Management and Reactor Safety of the Forschungszentrum Jülich develops in the framework of cooperation nondestructive analytical techniques for the routine characterization of radioactive waste packages at industrial-scale. During the phase of research and development Monte Carlo techniques are used to simulate the transport of particle, especially photons, electrons and neutrons, through matter and to obtain the response of detection systems. The radiological characterization of low and intermediate level radioactive waste drums is performed by segmented γ-scanning (SGS). To precisely and accurately reconstruct the isotope specific activity content in waste drums by SGS measurement, an innovative method called SGSreco was developed. The Geant4 code was used to simulate the response of the collimated detection system for waste drums with different activity and matrix configurations. These simulations allow a far more detailed optimization, validation and benchmark of SGSreco, since the construction of test drums covering a broad range of activity and matrix properties is time consuming and cost intensive. The MEDINA (Multi Element Detection based on Instrumental Neutron Activation) test facility was developed to identify and quantify non-radioactive elements and substances in radioactive waste drums. MEDINA is based on prompt and delayed gamma neutron activation analysis (P&DGNAA) using a 14 MeV neutron generator. MCNP simulations were carried out to study the response of the MEDINA facility in terms of gamma spectra, time dependence of the neutron energy spectrum

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

    NASA Astrophysics Data System (ADS)

    Brush, L. H.; Xiong, Y.

    2009-12-01

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

  2. 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.

  3. 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.

  4. 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.

  5. 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.

  6. The disposal of nuclear waste in space

    NASA Technical Reports Server (NTRS)

    Burns, R. E.

    1978-01-01

    The important problem of disposal of nuclear waste in space is addressed. A prior study proposed carrying only actinide wastes to space, but the present study assumes that all actinides and all fission products are to be carried to space. It is shown that nuclear waste in the calcine (oxide) form can be packaged in a container designed to provide thermal control, radiation shielding, mechanical containment, and an abort reentry thermal protection system. This package can be transported to orbit via the Space Shuttle. A second Space Shuttle delivers an oxygen-hydrogen orbit transfer vehicle to a rendezvous compatible orbit and the mated OTV and waste package are sent to the preferred destination. Preferred locations are either a lunar crater or a solar orbit. Shuttle traffic densities (which vary in time) are given and the safety of space disposal of wastes discussed.

  7. Autoradiographic study of actinide sorption on climax stock granite

    SciTech Connect

    Beall, G.W.; O'Kelley, G.D.; Allard, B.

    1980-06-01

    An autoradiographic technique that employed an arrangement for placing in firm contact Polaroid sheet film, a scintillator screen, and the radioactive face of a specimen was applied to a study of the sorption of americium, neptunium, plutonium, and uranium on Climax Stock granite under varying conditions of pH and Eh. Qualitative agreement was found between the sorption of americium on crushed, pure minerals and on the minerals comprising the specimen of Climax Stock granite. The observations also supported a mechanism for reduction of Np(V) to Np(IV) and Pu(VI) to Pu(IV) by Fe(II)-containing minerals. There was no evidence for reduction of U(VI) by the Fe(II)-containing minerals, although the uranium, assumed to be present as UO/sub 2//sup 2 +/, appeared to be the only actinide species to exhibit sorption by a simple, cation-exchange mechanism at particular mineral sites. Some implications of these results for nuclear waste isolation are discussed briefly.

  8. Actinide recycle potential in the IFR (Integral Fast Reactor)

    SciTech Connect

    Chang, Y.I.

    1989-01-01

    Rising concern about the greenhouse effect reinforces the need to reexamine the question of a next-generation reactor concept that can contribute significantly toward substitution for fossil-based energy generation. Even with only the nuclear capacity on-line today, world-wide reasonably assured uranium resources would last for only about 50 years. If nuclear is to make a significant contribution, breeding is a fundamental requirement. Uranium resources can then be extended by two orders of magnitude, making nuclear essentially a renewable energy source. The key technical elements of the IFR concept are metallic fuel and fuel cycle technology based on pyroprocessing. Pyroprocessing is radically different from the conventional PUREX reprocessing developed for the LWR oxide fuel. Chemical feasibility of pyroprocessing has been demonstrated. The next major step in the IFR development program will be the full-scale pyroprocessing demonstration to be carried out in conjunction with EBR-II. IFR fuel cycle closure based on pyroprocessing can also have a dramatic impact on the waste management options, and in particular on the actinide recycling. 6 figs.

  9. 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.

  10. Nuclear energy waste-space transportation and removal

    NASA Technical Reports Server (NTRS)

    Burns, R. E.

    1975-01-01

    A method for utilizing the decay heat of actinide wastes to power an electric thrust vehicle is proposed. The vehicle, launched by shuttle to earth orbit and to earth escape by a tug, obtains electrical power from the actinide waste heat by thermionic converters. The heavy gamma ray and neutron shielding which is necessary as a safety feature is removed in orbit and returned to earth for reuse. The problems associated with safety are dealt with in depth. A method for eliminating fission wastes via chemical propulsion is briefly discussed.

  11. 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.

  12. Vapor pressure and thermodynamics of actinide metals

    SciTech Connect

    Ward, J.W.; Kleinschmidt, P.D.; Haire, R.G.; Brown, D.

    1980-01-01

    Precise vapor pressure measurements by target collection/mass spectrometric Knudsen effusion techniques were combined with crystal entropy estimates to produce self-consistent free-enrgy functions, permitting calculation of heats, entropies and free energies from 298/sup 0/K to the highest temperatures of measurement. The vapor pressures and thermodyamics of vaporization of americium, curium, berkelium, and californium are compared in terms of electronic structure and bonding trends in the trans-plutonium elements. These resuslts are contrasted with the behavior of the early actinides, with attention to energy states and possible effects of f-electron bonding. 9 figures, 4 tables.

  13. 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.

  14. Colloid formation during waste form reaction: implications for nuclear waste disposal

    USGS Publications Warehouse

    Bates, J. K.; Bradley, J.; Teetsov, A.; Bradley, C. R.; ten Brink, Marilyn Buchholtz

    1992-01-01

    Insoluble plutonium- and americium-bearing colloidal particles formed during simulated weathering of a high-level nuclear waste glass. Nearly 100 percent of the total plutonium and americium in test ground water was concentrated in these submicrometer particles. These results indicate that models of actinide mobility and repository integrity, which assume complete solubility of actinides in ground water, underestimate the potential for radionuclide release into the environment. A colloid-trapping mechanism may be necessary for a waste repository to meet long-term performance specifications.

  15. Final Technical Progress Report Long term risk from actinides in the environment: Modes of mobility

    SciTech Connect

    Thomas B. Kirchner

    2002-03-22

    The key source of uncertainty in assessing actinide mobility is the relative importance of transport by: (1) wind erosion, (2) water erosion, and (3) vertical migration. Each of these three processes depends on several environmental factors and they compete with one another. A scientific assessment of the long-term risks associated with actinides in surface soils depends on better quantifying each of these three modes of mobility. The objective from our EMSP study was to quantify the mobility of soil actinides by wind erosion, water erosion, and vertical migration at three semiarid sites where actinide mobility is a key technical, social and legal issue. This EMSP project was the first to evaluate all three factors at a site. The approach has been to investigate both short- and long-term issues based on field and lab studies and model comparisons. Our results demonstrate the importance of incorporating threshold responses into a modeling framework that accounts for environmental factors and natural disturbances that trigger large changes in actinide mobility. The study measured erosional losses of sediment and fallout cesium (an actinide analogue) from field plots located near WIPP in 1998. The results highlight the large effect of burning as a disturbance on contaminant transport and mobility via runoff and erosion. The results show that runoff, erosion, and actinide transport are (1) strongly site specific-differences in radionuclide transport between WIPP and Rocky Flats differed by a factor of twelve because of soil and vegetation differences, and (2) are strongly impacted by disturbances such as fire, which can increase runoff, erosion, and actinide transport by more than an order of magnitude. In addition, a laboratory experiment using soil columns was conducted to investigate the vertical transport of contaminants in sandy soils. Nine columns of soil collected from the vicinity of the WIPP site were prepared. The column consisted of a piece of PVC pipe 20 cm

  16. Actinide electronic structure and atomic forces

    NASA Astrophysics Data System (ADS)

    Albers, R. C.; Rudin, Sven P.; Trinkle, Dallas R.; Jones, M. D.

    2000-07-01

    We have developed a new method[1] of fitting tight-binding parameterizations based on functional forms developed at the Naval Research Laboratory.[2] We have applied these methods to actinide metals and report our success using them (see below). The fitting procedure uses first-principles local-density-approximation (LDA) linear augmented plane-wave (LAPW) band structure techniques[3] to first calculate an electronic-structure band structure and total energy for fcc, bcc, and simple cubic crystal structures for the actinide of interest. The tight-binding parameterization is then chosen to fit the detailed energy eigenvalues of the bands along symmetry directions, and the symmetry of the parameterization is constrained to agree with the correct symmetry of the LDA band structure at each eigenvalue and k-vector that is fit to. By fitting to a range of different volumes and the three different crystal structures, we find that the resulting parameterization is robust and appears to accurately calculate other crystal structures and properties of interest.

  17. Design of an Actinide-Burning, Lead or Lead-Bismuth Cooled Reactor that Produces Low-Cost Electricity

    SciTech Connect

    Mac Donald, Philip Elsworth; Weaver, Kevan Dean; Davis, Cliff Bybee; MIT folks

    2000-07-01

    The purpose of this Idaho National Engineering and Environmental Laboratory (INEEL) and Massachusetts Institute of Technology (MIT) University Research Consortium (URC) project is to investigate the suitability of lead or lead-bismuth cooled fast reactors for producing low-cost electricity as well as for actinide burning. The goal is to identify and analyze the key technical issues in core neutronics, materials, thermal-hydraulics, fuels, and economics associated with the development of this reactor concept. Work has been accomplished in four major areas of research: core neutronic design, material compatibility, plant engineering, and coolant activation. In the area of core neutronic design, the reactivity vs. burnup and discharge isotopics of both non-fertile and fertile fuels were evaluated. An innovative core for pure actinide burning that uses streaming, fertile-free fuel assemblies was studied in depth. This particular core exhibits excellent reactivity performance upon coolant voiding, even for voids that occur in the core center, and has a transuranic (TRU) destruction rate that is comparable to the proposed accelerator transmutation of waste (ATW) facility. These studies suggest that a core can be designed to achieve a long life while maintaining safety and minimizing waste. In the area of material compatibility studies, an experimental apparatus for the investigation of the flow-assisted dissolution and precipitation (corrosion) of potential fuel cladding and structural materials has been designed and built at the INEEL. The INEEL forced-convection corrosion cell consists of a small heated vessel with a shroud and gas flow system. The corrosion cell is being used to test steel that is commercially available in the United States to temperatures above 650°C. Progress in plant engineering was made for two reactor concepts, one utilizing an indirect cycle with heat exchangers and the other utilizing a direct-contact steam cycle. The evaluation of the

  18. 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)

  19. Waste Isolation Pilot Plant Transuranic Waste Baseline inventory report. Volume 2. Revision 1

    SciTech Connect

    1995-02-01

    This document is the Baseline Inventory Report for the transuranic (alpha-bearing) wastes stored at the Waste Isolation Pilot Plant (WIPP) in New Mexico. Waste stream profiles including origin, applicable EPA codes, typical isotopic composition, typical waste densities, and typical rates of waste generation for each facility are presented for wastes stored at the WIPP.

  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. 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. 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.

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

    SciTech Connect

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

    2010-12-21

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 134,137}Cs, {sup 90}Sr, and alpha-emitting radionuclides (i.e., actinides) prior to disposal onsite as low level waste. An inorganic sorbent, monosodium titanate (MST), is currently used to remove {sup 90}Sr and alpha-emitting radionuclides, while a caustic-side solvent extraction process is used for removing {sup 134,137}Cs. A new peroxotitanate material, modified MST, or mMST, has recently been developed and has shown increased removal kinetics and capacity for {sup 90}Sr and alpha-emitting radionuclides compared to the current baseline material, MST. This paper describes recent results focused on further characterization of this material.

  4. Nuclear Archeology in a Bottle: Evidence of Pre-Trinity U.S. Weapons Activities from a Waste Burial Site

    SciTech Connect

    Schwantes, Jon M.; Douglas, Matthew; Bonde, Steven E.; Briggs, David; Farmer, Orville T.; Greenwood, Lawrence R.; Lepel, Elwood A.; Orton, Christopher R.; Wacker, John F.; Luksic, Andrzej T.

    2009-02-15

    During World War II, the Hanford Site in Washington was chosen for plutonium production. In 2004, a bottle containing a sample of plutonium was recovered from a Hanford waste trench. Isotopic age dating indicated the sample was separated from the fuel pellet 64 ±2.8 years earlier. Detectable products of secondary nuclear reactions, such as 22Na, proved useful as 1) a detectable analog for alpha emitting actinides, 2) an indicator of sample splitting, and 3) a measure of the time since sample splitting. The sample origin was identified as the X-10 reactor, Oak Ridge, TN. Corroborated by historical documents, we concluded this sample was part of the first batch of Pu separated at T-Plant, Hanford, the world’s first industrial-scale reprocessing facility, on December 9, 1944.

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

    SciTech Connect

    Leyba, J.D.

    1990-09-07

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

  6. Molecular hydrogen (H2) combustion emissions and their isotope (D/H) signatures from domestic heaters, diesel vehicle engines, waste incinerator plants, and biomass burning

    NASA Astrophysics Data System (ADS)

    Vollmer, M. K.; Walter, S.; Mohn, J.; Steinbacher, M.; Bond, S. W.; Röckmann, T.; Reimann, S.

    2012-07-01

    Molecular hydrogen (H2), its stable isotope signature (δD), and the key combustion parameters carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were measured from various combustion processes. H2 in the exhaust of gas and oil-fired heaters and of waste incinerator plants was generally depleted compared to ambient intake air, while CO was significantly elevated. These findings contradict the often assumed co-occurring net H2 and CO emissions in combustion processes and suggest that previous H2 emissions from combustion may have been overestimated when scaled to CO emissions. For the gas and oil-fired heater exhausts, H2 and δD generally decrease with increasing CO2, from ambient values of ~0.5 ppm and +130‰ to 0.2 ppm and -206‰, respectively. These results are interpreted as a combination of an isotopically light H2 source from fossil fuel combustion and a D/H kinetic isotope fractionation of hydrogen in the advected ambient air during its partial removal during combustion. Diesel exhaust measurements from dynamometer test stand driving cycles show elevated H2 and CO emissions during cold-start and some acceleration phases. While H2 and CO emissions from diesel vehicles are known to be significantly less than those from gasoline vehicles (on a fuel-energy base), we find that their molar H2/CO ratios (median 0.026, interpercentile range 0.12) are also significantly less compared to gasoline vehicle exhaust. Using H2/CO emission ratios, along with CO global emission inventories, we estimate global H2 emissions for 2000, 2005, and 2010. For road transportation (gasoline and diesel), we calculate 8.3 ± 2.2 Tg, 6.0 ± 1.5 Tg, and 3.8 ± 0.94 Tg, respectively, whereas the contribution from diesel vehicles is low (0.9-1.4%). Other fossil fuel emissions are believed to be negligible but H2 emissions from coal combustion are unknown. For residential (domestic) emissions, which are likely dominated by biofuel combustion, emissions for the same years are

  7. 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.

  8. Utilization of natural hematite as reactive barrier for immobilization of radionuclides from radioactive liquid waste.

    PubMed

    El Afifi, E M; Attallah, M F; Borai, E H

    2016-01-01

    Potential utilization of hematite as a natural material for immobilization of long-lived radionuclides from radioactive liquid waste was investigated. Hematite ore has been characterized by different analytical tools such as Fourier transformer infrared (FTIR), X-ray fluorescence (XRF), powder X-ray diffraction (XRD), thermogravimetry (TG) and differential thermal (DT) analysis, scanning electron microscopy (SEM) and BET-surface area. In this study, europium was used as REEs(III) and as a homolog of Am(III)-isotopes (such as (241)Am of 432.6 y, (242m)Am of 141 y and (243)Am of 7370 y). Micro particles of the hematite ore were used for treatment of radioactive waste containing (152+154)Eu(III). The results indicated that 96% (4.1 × 10(4) Bq) of (152+154)Eu(III) was efficiently retained onto hematite ore. Kinetic experiments indicated that the processes could be simulated by a pseudo-second-order model and suggested that the process may be chemisorption in nature. The applicability of Langmuir, Freundlich and Temkin models was investigated. It was found that Langmuir isotherm exhibited the best fit with the experimental results. It can be concluded that hematite is an economic and efficient reactive barrier for immobilization of long-lived radio isotopes of actinides and REEs(III).

  9. 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.

  10. 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.

  11. 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.

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

    SciTech Connect

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

    2010-01-01

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

  13. Understanding radioactive waste

    SciTech Connect

    Murray, R.L.

    1981-12-01

    This document contains information on all aspects of radioactive wastes. Facts are presented about radioactive wastes simply, clearly and in an unbiased manner which makes the information readily accessible to the interested public. The contents are as follows: questions and concerns about wastes; atoms and chemistry; radioactivity; kinds of radiation; biological effects of radiation; radiation standards and protection; fission and fission products; the Manhattan Project; defense and development; uses of isotopes and radiation; classification of wastes; spent fuels from nuclear reactors; storage of spent fuel; reprocessing, recycling, and resources; uranium mill tailings; low-level wastes; transportation; methods of handling high-level nuclear wastes; project salt vault; multiple barrier approach; research on waste isolation; legal requiremnts; the national waste management program; societal aspects of radioactive wastes; perspectives; glossary; appendix A (scientific American articles); appendix B (reference material on wastes). (ATT)

  14. 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.

  15. 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.

  16. Actinides in HD 101065 (Przybylski's Star)

    NASA Astrophysics Data System (ADS)

    Cowley, C. R.; Hubrig, S.; Bord, D. J.

    2003-05-01

    There are many strange things about the abundances in Przybylski's star (HD 101065). The most recent study (MN, 217, 299, 2000) finds that among the elements through copper, the abundances scatter with no apparent pattern. The largest deviations from solar are found for magnesium, which may be deficient by somewhat more than 1 dex, and cobalt, which appears to be in excess by about the same amount. The heavier elements especially those beyond barium, and continuing through the actinides uranium and thorium, show a clear pattern and a remarkable coherence. We plot solar and stellar abundances on a logarithmic plot vs. atomic number Z, and displace the solar points upward by some 3 dex. While individual points do not overlap, there is a remarkable similarity in the overall trends from Z = 58-80, including the maxima caused in the solar case by the third r-process peak. Points for the displaced solar actinides fall near their stellar counterparts. The processes that produced the large enhancements of these heavy elements have not caused large fractionations of adjacent elements. We have new spectra from the ESO UVES spectrograph on UT2. Resolution is 80,000 (blue) and 110,000 (red), with S/N > 300. This material, and new oscillator strengths (AA 381, 1090,2002; AA 382, 368, 2002), allow a more complete analysis of U and Th. We find abundances near +2.5 for both elements (log(H) = 12), but uncertainties at the moment are surely +/- 0.3 dex. We are currently working to improve the accuracy. Current errors preclude the use of these observations for accurate cosmochronometry, even if the chemical differentiation were not relevant. If a U/Th ratio of unity could be taken at face value, it would imply an r-process event some 103 years ago. Thanks to B. Pfeiffer help and advice.

  17. Archetypes for actinide-specific chelating agents

    SciTech Connect

    Smith, W.L.

    1980-01-01

    The complexes of uranium and thorium with monomeric hydroxamic acids can serve as archetypes for an optimized macrochelate designed for tetravalent actinides. The eight-coordinate complexes, Th(i-PrN(O)C(O)R)/sub 4/, where R = tert-butyl or R = neopentyl, have been synthesized and their structures have been determined by x-ray diffraction. The bulky alkyl substituents impart remarkable volatility and hydrocarbon solubility to these complexes, and the steric interactions of these substituents largely determine the structures. When R = tert-butyl, the substituents occupy the corners of a tetrahedron and force the complex into a distorted cubic geometry with crystallographic S/sub 4/ symmetry. Insertion of a methylene group between the carbonyl carbon and the tert-butyl group relaxes the steric requirements, and the coordination polyhedron of the neopentyl derivative is close to the mmmm isomer of the trigonal-faced dodecahedron. Uranium tetrachloride was quantitatively oxidized via an oxygen transfer reaction with two equivalents of N-phenylbenzohydroxamic acid anion (PBHA) in tetrahydrofuran (THF) to form UO/sub 2/ Cl(PBHA)(THF)/sub 2/ and benzanilide. The structure of the uranyl complex has been determined from x-ray diffraction data; the linear uranyl ion is surrounded by a planar pentagonal array composed of two hydroxamate oxygen atoms, a chloride ion and two THF oxygens, such that the chloride ion is opposite the hydroxamate group. That the THF and phenyl rings are twisted from this equatorial plane limits the molecular geometry to that of the C/sub 1/ point group. Some aspects of the chemistry of hydroxamic acids and of their incorporation into molecules that may serve as precursors of tetravalent actinide specific sequestering agents have also been investigated.

  18. 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.

  19. 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.

  20. 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.

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

    DOE PAGES

    Roberto, J.; Alexander, Charles W.; Boll, Rose Ann; ...

    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

    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.

  3. 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.

  4. 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.

  5. 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.

  6. Isotopic analyses by ICP-MS in clinical samples.

    PubMed

    Rodushkin, Ilia; Engström, Emma; Baxter, Douglas C

    2013-03-01

    This critical review focuses on inductively coupled plasma mass spectrometry (ICP-MS) based applications for isotope abundance ratio measurements in various clinical samples relevant to monitoring occupational or environmental exposure, human provenancing and reconstruction of migration pathways as well as metabolic research. It starts with a brief overview of recent advances in ICP-MS instrumentation, followed by selected examples that cover the fields of accurate analyte quantification using isotope dilution, tracer studies in nutrition and toxicology, and areas relying upon natural or man-made variations in isotope abundance ratios (Pb, Sr, actinides and stable heavy elements). Finally, some suggestions on future developments in the field are provided.

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

    SciTech Connect

    Heiken, J.H.; Lindberg, H.A.

    1984-05-01

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

  8. 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.

  9. The nature of chemical bonding in actinide and lanthanide ferrocyanides determined by X-ray absorption spectroscopy and density functional theory.

    PubMed

    Dumas, Thomas; Guillaumont, Dominique; Fillaux, Clara; Scheinost, Andreas; Moisy, Philippe; Petit, Sébastien; Shuh, David K; Tyliszczak, Tolek; Den Auwer, Christophe

    2016-01-28

    The electronic properties of actinide cations are of fundamental interest to describe intramolecular interactions and chemical bonding in the context of nuclear waste reprocessing or direct storage. The 5f and 6d orbitals are the first partially or totally vacant states in these elements, and the nature of the actinide ligand bonds is related to their ability to overlap with ligand orbitals. Because of its chemical and orbital selectivities, X-ray absorption spectroscopy (XAS) is an effective probe of actinide species frontier orbitals and for understanding actinide cation reactivity toward chelating ligands. The soft X-ray probes of the light elements provide better resolution than actinide L3-edges to obtain electronic information from the ligand. Thus coupling simulations to experimental soft X-ray spectral measurements and complementary quantum chemical calculations yields quantitative information on chemical bonding. In this study, soft X-ray XAS at the K-edges of C and N, and the L2,3-edges of Fe was used to investigate the electronic structures of the well-known ferrocyanide complexes K4Fe(II)(CN)6, thorium hexacyanoferrate Th(IV)Fe(II)(CN)6, and neodymium hexacyanoferrate KNd(III)Fe(II)(CN)6. The soft X-ray spectra were simulated based on quantum chemical calculations. Our results highlight the orbital overlapping effects and atomic effective charges in the Fe(II)(CN)6 building block. In addition to providing a detailed description of the electronic structure of the ferrocyanide complex (K4Fe(II)(CN)6), the results strongly contribute to confirming the actinide 5f and 6d orbital oddity in comparison to lanthanide 4f and 5d.

  10. 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.

  11. The influence of radioactive decay on actinide magnetic susceptibility measurements obtained using the Evans method.

    PubMed

    Autillo, Matthieu; Kaden, Peter; Geist, Andreas; Guerin, Laetitia; Moisy, Philippe; Berthon, Claude

    2014-05-14

    In order to explain the higher magnetic susceptibility of some aquo actinide ions than predicted by Hund's rules, the molar magnetic susceptibilities of two americium isotopes ((241)Am and (243)Am) were measured using the Evans method. The results obtained show a growing change in the magnetic susceptibility with α and also a β(-) activity increase in solution. β(-) particle effects appear to be stronger than radicals formed by α particles on the experimental values. The temperature dependence of Am(iii) magnetic susceptibility has been observed but from experiments carried out here, it appears to be difficult to prove whether this effect arises from radicals or β(-). Finally, magnetic susceptibilities of americium recorded in different media (HClO4, HCl, and HNO3) have been compared to alpha and beta emissions' impact.

  12. Actinide cross sections from the reaction of sup 13 C with sup 254 Es sup g

    SciTech Connect

    Moody, K.J.; Lougheed, R.W.; Dougan, R.J.; Hulet, E.K.; Wild, J.F.; Summerer, K.; Hahn, R.L.; Aarle, J.v.; Bethune, G.R. )

    1990-01-01

    We have measured cross sections for the formation of actinide transfer products in the reaction of 72-MeV {sup 13}C projectiles with {sup 254}Es{sup {ital g}} targets. The pattern of nuclide yields is similar to those observed in the reactions of heavier ions with {sup 254}Es{sup {ital g}}. We have constructed the primary element yields from these results and show that the total cross section for transfer reactions is 58 mb. The total reaction cross section is about 300 mb. Lawrencium isotopes are formed with larger cross sections than are consistent with the trends of the transfer-product distributions; we explain this in terms of massive transfer, and model the lawrencium yields with an evaporation code.

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

    PubMed

    Chang, G S; Ambrosek, R G

    2005-01-01

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

  14. Hardening Neutron Spectrum for Advanced Actinides Transmutation Experiments in the ATR

    SciTech Connect

    G. S. Chang; R. G. Ambrosek

    2004-05-01

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

  15. Dependence of Fission-Fragment Properties On Excitation Energy For Neutron-Rich Actinides

    NASA Astrophysics Data System (ADS)

    Ramos, D.; Rodríguez-Tajes, C.; Caamaño, M.; Farget, F.; Audouin, L.; Benlliure, J.; Casarejos, E.; Clement, E.; Cortina, D.; Delaune, O.; Derkx, X.; Dijon, A.; Doré, D.; Fernández-Domínguez, B.; de France, G.; Heinz, A.; Jacquot, B.; Navin, A.; Paradela, C.; Rejmund, M.; Roger, T.; Salsac, M. D.; Schmitt, C.

    2016-03-01

    Experimental access to full isotopic fragment distributions is very important to determine the features of the fission process. However, the isotopic identification of fission fragments has been, in the past, partial and scarce. A solution based on the use of inverse kinematics to study transfer-induced fission of exotic actinides was carried out at GANIL, resulting in the first experiment accessing the full identification of a collection of fissioning systems and their corresponding fission fragment distribution. In these experiments, a 238U beam at 6.14 AMeV impinged on a carbon target to produce fissioning systems from U to Am by transfer reactions, and Cf by fusion reactions. Isotopic fission yields of 250Cf, 244Cm, 240Pu, 239Np and 238U are presented in this work. With this information, the average number of neutrons as a function of the atomic number of the fragments is calculated, which reflects the impact of nuclear structure around Z=50, N=80 on the production of fission fragments. The characteristics of the Super Long, Standard I, Standard II, and Standard III fission channels were extracted from fits of the fragment yields for different ranges of excitation energy. The position and contribution of the fission channels as function of excitation energy are presented.

  16. Rapid Column Extraction Method for Actinides and Sr-89/90 in Water Samples

    SciTech Connect

    MAXWELL III, SHERROD L.

    2005-06-15

    The SRS Environmental Laboratory analyzes water samples for environmental monitoring, including river water and ground water samples. A new, faster actinide and strontium 89/90 separation method has been developed and implemented to improve productivity, reduce labor costs and add capacity to this laboratory. This method uses stacked TEVA Resin{reg_sign}, TRU Resin{reg_sign} and Sr-Resin{reg_sign} cartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium (Pu), neptunium (Np), uranium (U), americium (Am), curium (Cm) and thorium (Th) using a single multi-stage column combined with alpha spectrometry. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized. The method can be used for routine analysis or as a rapid method for emergency preparedness. Thorium and curium are often analyzed separately due to the interference of the daughter of Th-229 tracer, actinium (Ac)-225, on curium isotopes when measured by alpha spectrometry. This new method also adds a separation step using DGA Resin{reg_sign}, (Diglycolamide Resin, Eichrom Technologies) to remove Ac-225 and allow the separation and analysis of thorium isotopes and curium isotopes at the same time.

  17. Granulation and infiltration processes for the fabrication of minor actinide fuels, targets and conditioning matrices

    NASA Astrophysics Data System (ADS)

    Nästren, C.; Fernandez, A.; Haas, D.; Somers, J.; Walter, M.

    2007-05-01

    The impact of Pu and Am, two elements that potentially pose a long term hazard for the disposal of spent nuclear fuel, can be abated by their reintroduction into the fuel cycle for transmutation. Such transmutation targets can be fabricated by a sol gel method for the production of porous inactive beads, which are then infiltrated by Am solutions. Following calcination, compaction into pellets and sintering, the product is obtained. At its heart, the sol gel process relies on an ammonia precipitation, so that it is not universally applicable. Therefore, an alternative is sought not just to overcome this chemical limitation, but also to simplify the process and reduce waste streams. The new concept utilises powder metallurgy routes (compaction, crushing and sieving) to produce porous, almost, dust free granules, which are infiltrated with the actinide nitrate. The method has been developed using yttria stabilised zirconia and alumina, and has been demonstrated for the production of Al2O3-AmO2 targets for neutron capture investigations. The results are very promising and meet light water reactor fuel specifications. In addition, the process is ideally suited for the production of ceramic matrices for conditioning actinides for geological disposal.

  18. Selective sorption of actinides by titania nanoparticles covalently functionalized with simple organic ligands.

    PubMed

    Veliscek-Carolan, Jessica; Jolliffe, Katrina A; Hanley, Tracey L

    2013-11-27

    Although current and proposed reprocessing of used nuclear fuel is performed predominantly by solvent extraction processes, solid phase sorbent materials have many advantages including the ability to avoid production of large volumes of organic waste. Therefore, three titania nanoparticle based sorbent materials have been developed, functionalized with organic ligands designed to impart selectivity for elements relevant to important separations at the back end of the nuclear fuel cycle. A novel, simplified method of covalent functionalization to the titania surface has been utilized, and the resulting materials have been shown to be hydrolytically stable at pH 2. The sorption behavior of these organofunctionalized titania materials was investigated over a wide pH range with a selection of elements including fission products and actinides. Titania nanoparticles functionalized with an amine or phosphate moiety were able to demonstrate exclusive extraction of uranium under optimized conditions. Titania nanoparticles functionalized with a picolinamide moiety exhibited superior minor actinide sorption properties, in terms of both efficiency and selectivity, to solvent extraction processes using similar organic moieties. As such, organo-functionalized titania materials as solid phase sorbents show promise as a future alternative to solvent extraction processes for nuclear separations.

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

    SciTech Connect

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

    2007-06-29

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

  20. Review of the complexation of tetravalent actinides by ISA and gluconate under alkaline to hyperalkaline conditions.

    PubMed

    Gaona, X; Montoya, V; Colàs, E; Grivé, M; Duro, L

    2008-12-12

    Isosaccharinic (ISA) and gluconic acids (GLU) are polyhydroxy carboxylic compounds showing a high affinity to metal complexation. Both organic ligands are expected in the cementitious environments usually considered for the disposal of low- and intermediate-level radioactive wastes. The hyperalkaline conditions imposed by cementitious materials contribute to the formation of ISA through cellulose degradation, whereas GLU is commonly used as a concrete additive. Despite the high stability attributed to ISA/GLU complexes of tetravalent actinides, the number and reliability of available experimental studies is still limited. This work aims at providing a general and comprehensive overview of the state of the art regarding Th, U(IV), Np(IV), and Pu(IV) complexes with ISA and GLU. In the presence of ISA/GLU concentrations in the range 10(-5)-10(-2) M and absence of calcium, An(IV)(OH)x(L)y complexes (An(IV)=Th, U(IV), Np(IV), Pu(IV); L=ISA, GLU) are expected to dominate the aqueous speciation of tetravalent actinides in the alkaline pH range. There is a moderate agreement among their stability, although the stoichiometry of certain An(IV)-GLU complexes is still ill-defined. Under hyperalkaline conditions and presence of calcium, the species CaTh(OH)4(L)2(aq) has been described for both ISA and GLU, and similar complexes may be expected to form with other tetravalent actinides. In the present work, the available thermodynamic data for An(IV)-ISA/GLU complexes have been reviewed and re-calculated to ensure the internal consistency of the stability constants assessed. Further modelling exercises, estimations based on Linear Free-Energy Relationships (LFER) among tetravalent actinides, as well as direct analogies between ISA and GLU complexes have also been performed. This approach has led to the definition of a speciation scheme for the complexes of Th, U(IV), Np(IV) and Pu(IV) with ISA and GLU forming in alkaline to hyperalkaline pH conditions, both in the absence and

  1. Review of the complexation of tetravalent actinides by ISA and gluconate under alkaline to hyperalkaline conditions

    NASA Astrophysics Data System (ADS)

    Gaona, X.; Montoya, V.; Colàs, E.; Grivé, M.; Duro, L.

    2008-12-01

    Isosaccharinic (ISA) and gluconic acids (GLU) are polyhydroxy carboxylic compounds showing a high affinity to metal complexation. Both organic ligands are expected in the cementitious environments usually considered for the disposal of low- and intermediate-level radioactive wastes. The hyperalkaline conditions imposed by cementitious materials contribute to the formation of ISA through cellulose degradation, whereas GLU is commonly used as a concrete additive. Despite the high stability attributed to ISA/GLU complexes of tetravalent actinides, the number and reliability of available experimental studies is still limited. This work aims at providing a general and comprehensive overview of the state of the art regarding Th, U(IV), Np(IV), and Pu(IV) complexes with ISA and GLU. In the presence of ISA/GLU concentrations in the range 10 - 5 -10 - 2 M and absence of calcium, An(IV)(OH) x(L) y complexes (An(IV) = Th, U(IV), Np(IV), Pu(IV); L = ISA, GLU) are expected to dominate the aqueous speciation of tetravalent actinides in the alkaline pH range. There is a moderate agreement among their stability, although the stoichiometry of certain An(IV)-GLU complexes is still ill-defined. Under hyperalkaline conditions and presence of calcium, the species CaTh(OH) 4(L) 2(aq) has been described for both ISA and GLU, and similar complexes may be expected to form with other tetravalent actinides. In the present work, the available thermodynamic data for An(IV)-ISA/GLU complexes have been reviewed and re-calculated to ensure the internal consistency of the stability constants assessed. Further modelling exercises, estimations based on Linear Free-Energy Relationships (LFER) among tetravalent actinides, as well as direct analogies between ISA and GLU complexes have also been performed. This approach has led to the definition of a speciation scheme for the complexes of Th, U(IV), Np(IV) and Pu(IV) with ISA and GLU forming in alkaline to hyperalkaline pH conditions, both in the

  2. 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

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

    SciTech Connect

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

    2006-08-31

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

  4. 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.

  5. 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)

  6. Isotopic Biogeochemistry

    NASA Technical Reports Server (NTRS)

    Hayes, J. M.

    1985-01-01

    An overview is provided of the biogeochemical research. The funding, productivity, personnel and facilities are reviewed. Some of the technical areas covered are: carbon isotopic records; isotopic studies of banded iron formations; isotope effects in microbial systems; studies of organic compounds in ancient sediments; and development in isotopic geochemistry and analysis.

  7. Rapid determination of alpha emitters using Actinide resin.

    PubMed

    Navarro, N; Rodriguez, L; Alvarez, A; Sancho, C

    2004-01-01

    The European Commission has recently published the recommended radiological protection criteria for the clearance of building and building rubble from the dismantling of nuclear installations. Radionuclide specific clearance levels for actinides are very low (between 0.1 and 1 Bq g(-1)). The prevalence of natural radionuclides in rubble materials makes the verification of these levels by direct alpha counting impossible. The capability of Actinide resin (Eichrom Industries, Inc.) for extracting plutonium and americium from rubble samples has been tested in this work. Besides a strong affinity for actinides in the tri, tetra and hexavalent oxidation states, this extraction chromatographic resin presents an easy recovery of absorbed radionuclides. The retention capability was evaluated on rubble samples spiked with certified radionuclide standards (239Pu and 241Am). Samples were leached with nitric acid, passed through a chromatographic column containing the resin and the elution fraction was measured by LSC. Actinide retention varies from 60% to 80%. Based on these results, a rapid method for the verification of clearance levels for actinides in rubble samples is proposed.

  8. 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.

  9. 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

  10. 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.

  11. 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.

  12. 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.

  13. Recent progress on minor-actinide-bearing oxide fuel fabrication at CEA Marcoule

    NASA Astrophysics Data System (ADS)

    Lebreton, Florent; Prieur, Damien; Horlait, Denis; Delahaye, Thibaud; Jankowiak, Aurélien; Léorier, Caroline; Jorion, Frédéric; Gavilan, Elisabeth; Desmoulière, François

    2013-07-01

    Partitioning and transmutation (P&T) of minor actinides (MA: americium, neptunium and curium) in fast neutron reactors or accelerator-driven systems is a route envisaged to reduce nuclear waste inventory. Over the years, several modes of P&T were proposed, each being based on the use of dedicated fuels such as inert-matrix fuels, MA-bearing MOX or MA-bearing blankets. In this context, progress on the manufacturing of such fuels is a key-challenge in order to render P&T viable at the industrial scale. Here, MA-bearing oxide fuel fabrication and characterization conducted in the CEA Marcoule Atalante facility is reviewed. A particular attention is also given to the research conducted on uranium-americium mixed-oxides fuels, which are now considered the reference fuels for MA transmutation in France.

  14. Role of fast reactor and its cycle to reduce nuclear waste burden

    SciTech Connect

    Arie, Kazuo; Oomori, Takashi; Okita, Takeshi; Kawashima, Masatoshi; Kotake, Shoji; Fuji-ie, Yoichi

    2013-07-01

    The role of the metal fuel fast reactor with recycling of actinides and the five long-lived fission products based on the concept of the Self-Consistent Nuclear Energy System has been examined by evaluating the reduction of nuclear wastes during the transition period to this reactor system. The evaluation was done in comparison to an LWR once-through case and a conventional actinide recycling oxide fast reactor. As a result, it is quantitatively clarified that a metal fuel fast reactor with actinide and the five long-lived fission products (I{sup 129}, Tc{sup 99}, Zr{sup 93}, Cs{sup 135} and Sn{sup 126}) recycling could play a significant role in reducing the nuclear waste burden including the current LWR wastes. This can be achieved by using a fast neutron spectrum reactor enhanced with metal fuel that brings high capability as a 'waste burner'. (authors)

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

    SciTech Connect

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

    1995-12-01

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

  16. Isolation of Pu-isotopes from environmental samples using ion chromatography for accelerator mass spectrometry and alpha spectrometry.

    PubMed

    Chamizo, E; Jiménez-Ramos, M C; Wacker, L; Vioque, I; Calleja, A; García-León, M; García-Tenorio, R

    2008-01-14

    A radiochemical method for the isolation of plutonium-isotopes from environmental samples, based on the use of specific extraction chromatography resins for actinides (TEVA), Eichrom Industries, Inc.), has been set up in our laboratory and optimised for their posterior determination by alpha spectrometry (AS) or accelerator mass spectrometry (AMS). The proposed radiochemical method has replaced in our lab a well-established one based on the use of a relatively un-specific anion-exchange resin (AG) 1X8, Bio-rad Laboratories, Inc.), because it is clearly less time consuming, reduces the amounts and molarities of acid wastes produced, and reproducibly gives high radiochemical yields. In order to check the reliability of the proposed radiochemical method for the determination of plutonium-isotopes in different environmental matrixes, twin aliquots of a set of samples were prepared with TEVA and with AG 1X8 resins and measured by AS. Some samples prepared with TEVA resins were measured as well by AMS. As it is shown in the text, there is a comfortable agreement between AS and AMS, which adequately validates the method.

  17. 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

  18. Determination of actinides at the radiological and environmental sciences laboratory

    NASA Astrophysics Data System (ADS)

    Williams, R. L.; Grothaus, G. E.

    1984-06-01

    This article briefly describes some of the techniques and procedures that have been developed at the Radiological and Environmental Sciences Laboratory (RESL) to determine the actinides in environmental and biological samples. Dried or ashed samples are totally decomposed in high temperature fusions or with an acid dissolution method. Actinides of interest are coprecipitated from the sample matrix with barium sulfate, cerium fluoride, or a combination of ferrous phosphate and calcium fluoride precipitations. The precipitates are dissolved in perchloric acid and extracted with bis(2-ethylhexyl)phosphoric acid (HDEHP) or dissolved in acidic aluminum nitrate and extracted with Aliquat-336. Actinides in the stripped fractions are coprecipitated with 50 μg of cerium as cerium fluoride, filtered onto membrane filters and counted by alpha spectrometry. The described procedures enable an experienced analyst to prepare sixteen 1 g soil or twelve 5 g faecal ash samples for alpha spectrometry in 14 to 16 working-hours.

  19. 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.

  20. 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.

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

    NASA Astrophysics Data System (ADS)

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

    1987-04-01

    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.

  2. Systematic view of optical absorption spectra in the actinide series

    SciTech Connect

    Carnall, W.T.

    1985-01-01

    In recent years sufficient new spectra of actinides in their numerous valence states have been measured to encourage a broader scale analysis effort than was attempted in the past. Theoretical modelling in terms of effective operators has also undergone development. Well established electronic structure parameters for the trivalent actinides are being used as a basis for estimating parameters in other valence states and relationships to atomic spectra are being extended. Recent contributions to our understanding of the spectra of 4+ actinides have been particularly revealing and supportive of a developing general effort to progress beyond a preoccupation with modelling structure to consideration of the much broader area of structure-bonding relationships. We summarize here both the developments in modelling electronic structure and the interpretation of apparent trends in bonding. 60 refs., 9 figs., 1 tab.

  3. Actinide science with soft x-ray synchrotron radiation

    NASA Astrophysics Data System (ADS)

    Shuh, David K.

    2000-07-01

    The primary methods for the experimental investigation of actinide materials in the VUV/soft x-ray region are the complementary photoelectron spectroscopies, near-edge x-ray absorption fine structure (NEXAFS), and x-ray emission spectroscopy (XES) techniques. Resonant photoemission techniques capable of resolving the 5f electron contributions to actinide bonding along with angle-resolving measurements for band structure and surface structure determinations, have clear and immediate applications. Venerable angle-integrating core and valence band photoelectron spectroscopy are valuable for characterization and analytical purposes. Combined with results from NEXAFS measurements, these techniques will provide the information needed to develop improved understandings of the electronic structure of actinide materials and their surface chemistries/physics.

  4. 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)

  5. One-group fission cross sections for plutonium and minor actinides inserted in calculated neutron spectra of fast reactor cooled with lead-208 or lead-bismuth eutectic

    SciTech Connect

    Khorasanov, G. L.; Blokhin, A. I.

    2012-07-01

    The paper is dedicated to one-group fission cross sections of Pu and MA in LFRs spectra with the aim to increase these values by choosing a coolant which hardens neutron spectra. It is shown that replacement of coolant from Pb-Bi with Pb-208 in the fast reactor RBEC-M, designed in Russia, leads to increasing the core mean neutron energy. As concerns fuel Pu isotopes, their one-group fission cross sections become slightly changed, while more dramatically Am-241 one-group fission cross section is changed. Another situation occurs in the lateral blanket containing small quantities of minor actinides. It is shown that as a result of lateral blanket mean neutron energy hardening the one-group fission cross sections of Np-237, Am-241 and Am-243 increases up to 8-11%. This result allows reducing the time of minor actinides burning in FRs. (authors)

  6. 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.

  7. Actinide consumption: Nuclear resource conservation without breeding

    SciTech Connect

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

    1991-01-01

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

  8. Reference commercial high-level waste glass and canister definition.

    SciTech Connect

    Slate, S.C.; Ross, W.A.; Partain, W.L.

    1981-09-01

    This report presents technical data and performance characteristics of a high-level waste glass and canister intended for use in the design of a complete waste encapsulation package suitable for disposal in a geologic repository. The borosilicate glass contained in the stainless steel canister represents the probable type of high-level waste product that will be produced in a commercial nuclear-fuel reprocessing plant. Development history is summarized for high-level liquid waste compositions, waste glass composition and characteristics, and canister design. The decay histories of the fission products and actinides (plus daughters) calculated by the ORIGEN-II code are presented.

  9. Leap to explore the region of neutron-rich heavy element isotopes

    SciTech Connect

    Hoffman, D.C.

    1985-10-01

    The research aims of the Large Einsteinium Activation Program (LEAP) are described. This program is a major initiative to exploit currently existing expertise in heavy element research and the potential for producing very heavy actinide target materials such as 285-day /sup 254/Es at the High Flux Isotope Reactor at Oak Ridge National Laboratory. The stated aims of the program are to produce heavy element isotopes, to conduct chemical studies of these isotopes, to study the nuclear properties of such isotopes, and to produce a superheavy element (183 neutrons) by the using a /sup 254/Es target and /sup 48/Ca projectiles. 13 refs., 2 figs., 2 tabs. (DWL)

  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. 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.

  12. 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

  13. FUEL CYCLE ISOTOPE EVOLUTION BY TRANSMUTATION DYNAMICS OVER MULTIPLE RECYCLES

    SciTech Connect

    Samuel Bays; Steven Piet; Amaury Dumontier

    2010-06-01

    Because all actinides have the ability to fission appreciably in a fast neutron spectrum, these types of reactor systems are usually not associated with the buildup of higher mass actinides: curium, berkelium and californium. These higher actinides have high specific decay heat power, gamma and neutron source strengths, and are usually considered as a complication to the fuel manufacturing and transportation of fresh recycled transuranic fuel. This buildup issue has been studied widely for thermal reactor fuels. However, recent studies have shown that the transmutation physics associated with "gateway isotopes" dictates Cm-Bk-Cf buildup, even in fast burner reactors. Assuming a symbiotic fuel relationship with light water reactors (LWR), Pu-242 and Am-243 are formed in the LWRs and then are externally fed to the fast reactor as part of its overall transuranic fuel supply. These isotopes are created much more readily in a thermal than in fast spectrum systems due to the differences in the fast fission (i.e., above the fission threshold for non-fissile actinides) contribution. In a strictly breeding fast reactor this dependency on LWR transuranics would not exist, and thus avoids the introduction of LWR derived gateway isotopes into the fast reactor system. However in a transuranic burning fast reactor, the external supply of these gateway isotopes behaves as an external driving force towards the creation and build-up of Cm-Bk-Cf in the fuel cycle. It was found that though the Cm-Bk-Cf concentration in the equilibrium fuel cycle is dictated by the fast neutron spectrum, the time required to reach that equilibrium concentration is dictated by recycle, transmutation and decay storage dynamics.

  14. 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.

  15. 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)

  16. 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.

  17. Waste isolation safety assessment program. Task 4. Third contractor information meeting

    SciTech Connect

    Not Available

    1980-06-01

    The Contractor Information Meeting (October 14 to 17, 1979) was part of the FY-1979 effort of Task 4 of the Waste Isolation Safety Assessment Program (WISAP): Sorption/Desorption Analysis. The objectives of this task are to: evaluate sorption/desorption measurement methods and develop a standardized measurement procedure; produce a generic data bank of nuclide-geologic interactions using a wide variety of geologic media and groundwaters; perform statistical analysis and synthesis of these data; perform validation studies to compare short-term laboratory studies to long-term in situ behavior; develop a fundamental understanding of sorption/desorption processes; produce x-ray and gamma-emitting isotopes suitable for the study of actinides at tracer concentrations; disseminate resulting information to the international technical community; and provide input data support for repository safety assessment. Conference participants included those subcontracted to WISAP Task 4, representatives and independent subcontractors to the Office of Nuclear Waste Isolation, representatives from other waste disposal programs, and experts in the area of waste/geologic media interaction. Since the meeting, WISAP has been divided into two programs: Assessment of Effectiveness of Geologic Isolation Systems (AEGIS) (modeling efforts) and Waste/Rock Interactions Technology (WRIT) (experimental work). The WRIT program encompasses the work conducted under Task 4. This report contains the information presented at the Task 4, Third Contractor Information Meeting. Technical Reports from the subcontractors, as well as Pacific Northwest Laboratory (PNL), are provided along with transcripts of the question-and-answer sessions. The agenda and abstracts of the presentations are also included. Appendix A is a list of the participants. Appendix B gives an overview of the WRIT program and details the WRIT work breakdown structure for 1980.

  18. Thermodynamic stability of actinide pyrochlore minerals in deep geologic repository environments

    SciTech Connect

    WANG,YIFENG; XU,HUIFANG

    2000-03-14

    Crystalline phases of pyrochlore (e.g., CaPuTi{sub 2}O{sub 7}, CaUTi{sub 2}O{sub 7}) have been proposed as a durable ceramic waste form for disposal of high level radioactive wastes including surplus weapons-usable plutonium. In this paper, the authors use a linear free energy relationship to predict the Gibbs free energies of formation of pyrochlore phases (CaMTi{sub 2}O{sub 7}). The Pu-pyrochlore phase is predicted to be stable with respect to PuO{sub 2}, CaTiO{sub 3}, and TiO{sub 2} at room temperatures. Pu-pyrochlore is expected to be stable in a geologic repository where silica and carbonate components are absent or limited. The authors suggest that a repository in a salt formation be an ideal environment for disposal of high level, pyrochlore-based ceramic wastes. In such environment, adding CaO as a backfill will make pyrochlore minerals thermodynamically stable and therefore effectively prevent actinide release from these mineral phases.

  19. Improving the actinides recycling in closed fuel cycles, a major step towards nuclear energy sustainability

    SciTech Connect

    Poinssot, C.; Grandjean, S.; Masson, M.; Bouillis, B.; Warin, D.

    2013-07-01

    Increasing the sustainability of nuclear energy is a longstanding road that requires a stepwise approach to successively tackle the following 3 objectives. First of all, optimize the consumption of natural resource to preserve them for future generations and hence guarantee the energetic independence of the countries (no uranium ore is needed anymore). The current twice-through cycle of Pu implemented by France, UK, Japan and soon China is a first step in this direction and already allows the development and optimization of the relevant industrial processes. It also allows a major improvement regarding the conditioning of the ultimate waste in a durable and robust nuclear glass. Secondly, the recycling of americium could be an interesting option for the future with the deployment of FR fleet to save the repository resource and optimize its use by allowing a denser disposal. It would limit the burden towards the future generations and the need for additional repositories before several centuries. Thirdly, the recycling of the whole minor actinides inventory could be an interesting option for the far-future for strongly decreasing the waste long-term toxicity, down to a few centuries. It would bring the waste issue back within the human history, which should promote its acceptance by the social opinion.

  20. Evidence for a hypogene paleohydrogeological event at the prospective nuclear waste disposal site Yucca Mountain, Nevada, USA, revealed by the isotope composition of fluid-inclusion water

    NASA Astrophysics Data System (ADS)

    Dublyansky, Yuri V.; Spötl, Christoph

    2010-01-01

    Secondary calcite residing in open cavities in the unsaturated zone of Yucca Mountain has long been interpreted as the result of downward infiltration of meteoric water through open fractures. In order to obtain information on the isotopic composition (δD and δ 18O) of the mineral-forming water we studied fluid inclusions from this calcite. Water was extracted from inclusions by heated crushing and the δD values were measured using a continuous-flow isotope-ratio mass spectrometry method. The δ 18O values were calculated from the δ 18O values of the host calcite assuming isotopic equilibrium at the temperature of formation determined by fluid-inclusion microthermometry. The δD values measured in all samples range between - 110 and - 90‰, similar to Holocene meteoric water. Coupled δ 18O-δD values plot significantly, 2 to 8‰, to the right of the meteoric water line. Among the various processes operating at the topographic surface and/or in the unsaturated zone only two processes, evaporation and water-rock exchange, could alter the isotope composition of percolating water. Our analysis indicates, however, that none of these processes could produce the observed large positive δ 18O-shifts. The latter require isotopic interaction between mineral-forming fluid and host rock at elevated temperature (>100 °C), which is only possible in the deep-seated hydrothermal environment. The stable isotope data are difficult to reconcile with a meteoric origin of the water from which the secondary minerals at Yucca Mountain precipitated; instead they point to the deep-seated provenance of the mineral-forming waters and their introduction into the unsaturated zone from below, i.e. a hypogene origin.

  1. Investigation of microscopic radiation damage in waste forms using ODNMR and AEM techniques. (EMSP Project Final Report)

    SciTech Connect

    Liu, G.; Luo, J.; Beitz, J.; Li, S.; Williams, C.; Zhorin, V.

    2000-04-21

    This project seeks to understand the microscopic effects of radiation damage in nuclear waste forms. The authors' approach to this challenge encompasses studies of ceramics and glasses containing short-lived alpha- and beta-emitting actinides with electron microscopy, laser and X-ray spectroscopic techniques, and computational modeling and simulations. In order to obtain information on long-term radiation effects on waste forms, much of the effort is to investigate {alpha}-decay induced microscopic damage in 18-year old samples of crystalline yttrium and lutetium orthophosphates that initially contained {approximately} 1(wt)% of the alpha-emitting isotope {sup 244}Cm (18.1 y half life). Studies also are conducted on borosilicate glasses that contain {sup 244}Cm, {sup 241}Am, or {sup 249}Bk, respectively. The authors attempt to gain clear insights into the properties of radiation-induced structure defects and the consequences of collective defect-environment interactions, which are critical factors in assessing the long-term performance of high-level nuclear waste forms.

  2. 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).

  3. Radiation Effects in a Model Ceramic for Nuclear Waste Disposal

    SciTech Connect

    Devanathan, Ram; Weber, William J.

    2007-04-02

    The safe immobilization of nuclear waste in geological repositories is one of the major scientific challenges facing humanity today. Crystalline ceramics hold the promise of locking up actinides from nuclear fuel and excess weapons plutonium in their structure thereby isolating them from the environment. In this paper, we discuss the atomistic details of radiation damage in a model ceramic, zircon.

  4. Medical effects of internal contamination with actinides: further controversy on depleted uranium and radioactive warfare.

    PubMed

    Durakovic, Asaf

    2016-05-01

    The Nuclear Age began in 1945 with testing in New Mexico, USA, and the subsequent bombings of Hiroshima and Nagasaki. Regardless of attempts to limit the development of nuclear weapons, the current world arsenal has reached the staggering dimensions and presents a significant concern for the biosphere and mankind. In an explosion of a nuclear weapon, over 400 radioactive isotopes are released into the biosphere, 40 of which pose potential dangers including iodine, cesium, alkaline earths, and actinides. The immediate health effects of nuclear explosions include thermal, mechanical, and acute radiation syndrome. Long-term effects include radioactive fallout, internal contamination, and long-term genotoxicity. The current controversial concern over depleted uranium's somatic and genetic toxicity is still a subject of worldwide sustained research. The host of data generated in the past decades has demonstrated conflicting findings, with the most recent evidence showing that its genotoxicity is greater than previously considered. Of particular concern are the osteotropic properties of uranium isotopes due to their final retention in the crystals of exchangeable and nonexchangeable bone as well as their proximity to pluripotent stem cells. Depleted uranium remains an unresolved issue in both warfare and the search for alternative energy sources.

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

    SciTech Connect

    Metzger, R.L.; Jessop, B.H.; McDowell, B.L.

    1996-02-01

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

  6. Radiation Effects in Nuclear Waste Materials

    SciTech Connect

    Weber, William J.

    2005-09-30

    The objective of this project is to develop a fundamental understanding of radiation effects in glasses and ceramics, as well as the influence of solid-state radiation effects on aqueous dissolution kinetics, which may impact the performance of nuclear waste forms and stabilized nuclear materials. This work provides the underpinning science to develop improved glass and ceramic waste forms for the immobilization and disposition of high-level tank waste, excess plutonium, plutonium residues and scrap, other actinides, and other nuclear waste streams. Furthermore, this work is developing develop predictive models for the performance of nuclear waste forms and stabilized nuclear materials. Thus, the research performed under this project has significant implications for the immobilization of High-Level Waste (HLW) and Nuclear Materials, two mission areas within the Office of Environmental Management (EM). With regard to the HLW mission, this research will lead to improved understanding of radiation-induced degradation mechanisms and their effects on dissolution kinetics, as well as development of predictive models for waste form performance. In the Nuclear Materials mission, this research will lead to improvements in the understanding of radiation effects on the chemical and structural properties of materials for the stabilization and long-term storage of plutonium, highly-enriched uranium, and other actinides. The research uses plutonium incorporation, ion-beam irradiation, and electron-beam irradiation to simulate the effects of alpha decay and beta decay on relevant glasses and ceramics. The research under this project has the potential to result in improved glass and ceramic materials for the stabilization and immobilization of high-level tank waste, plutonium residues and scraps, surplus weapons plutonium, highly-enriched uranium, other actinides, and other radioactive materials.

  7. Radiation Effects in Nuclear Waste Materials

    SciTech Connect

    Weber, William J.

    2005-06-01

    The objective of this project is to develop a fundamental understanding of radiation effects in glasses and ceramics, as well as the influence of solid-state radiation effects on aqueous dissolution kinetics, which may impact the performance of nuclear waste forms and stabilized nuclear materials. This work provides the underpinning science to develop improved glass and ceramic waste forms for the immobilization and disposition of high-level tank waste, excess plutonium, plutonium residues and scrap, other actinides, and other nuclear waste streams. Furthermore, this work is developing develop predictive models for the performance of nuclear waste forms and stabilized nuclear materials. Thus, the research performed under this project has significant implications for the immobilization of High-Level Waste (HLW) and Nuclear Materials, two mission areas within the Office of Environmental Management (EM). With regard to the HLW mission, this research will lead to improved understanding of radiation-induced degradation mechanisms and their effects on dissolution kinetics, as well as development of predictive models for waste form performance. In the Nuclear Materials mission, this research will lead to improvements in the understanding of radiation effects on the chemical and structural properties of materials for the stabilization and long-term storage of plutonium, highly-enriched uranium, and other actinides. The research uses plutonium incorporation, ion-beam irradiation, and electron-beam irradiation to simulate the effects of alpha decay and beta decay on relevant glasses and ceramics. The research under this project has the potential to result in improved glass and ceramic materials for the stabilization and immobilization of high-level tank waste, plutonium residues and scraps, surplus weapons plutonium, highly-enriched uranium, other actinides, and other radioactive materials.

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

    NASA Astrophysics Data System (ADS)

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

    2015-01-01

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

  9. Minor Actinide Transmutation Physics for Low Conversion Ratio Sodium Fast Reactors

    SciTech Connect

    Mehdi Asgari; Samuel E. Bays; Benoit Forget; Rodolfo Ferrer

    2007-09-01

    The effects of varying the reprocessing strategy used in the closed cycle of a Sodium Fast Reactor (SNF) prototype are presented in this paper. The isotopic vector from the aqueous separation of transuranic (TRU) elements in Light Water Reactor (LWR) spent nuclear fuel (SNF) is assumed to also vary according to the reprocessing strategy of the closed fuel cycle. The decay heat, gamma energy, and neutron emission of the fuel discharge at equilibrium are found to vary depending on the separation strategy. The SFR core used in this study corresponds to a burner configuration with a conversion ratio of ~0.5 based on the Super-PRISM design. The reprocessing strategies stemming from the choice of either metal or oxide fuel for the SFR are found to have a large impact on the equilibrium discharge decay heat, gamma energy, and neutron emission. Specifically, metal fuel SFR with pyroprocessing of the discharge produces the largest amount of TRU consumption (166 kg per Effective Full Power Year or EFPY), but also the highest decay heat, gamma energy, and neutron emission. On the other hand, an oxide fuel SFR with PUREX reprocessing minimizes the decay heat and related parameters of interest to a minimum, even when compared to thermal Mixed Oxide (MOX) or Inert Matrix Fuel (IMF) on a per mass basis. On an assembly basis, however, the metal SFR discharge has a lower decay heat than an equivalent oxide SFR assembly for similar minor actinide consumptions (~160 kg/EFPY.) Another disadvantage in the oxide PUREX reprocessing scenario is that there is no consumption of americium and curium, since PUREX reprocessing separates these minor actinides (MA) and requires them to be disposed of externally.

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

    SciTech Connect

    D.S. Shafer; J. Gommes

    2009-02-03

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

  11. 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

  12. 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.

  13. 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.

  14. 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.

  15. 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)

  16. 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.

  17. Search for octupole deformation in neutron rich Xe isotopes

    SciTech Connect

    Bentaleb, M.; Schulz, N.; Lubkiewicz, E.

    1994-07-01

    A search for octupole deformation in neutron rich Xe isotopes has been conducted through gamma-ray spectroscopy of primary fragments produced in the spontaneous fission of {sup 248}Cm. The spectrometer consisted of the Eurogam array and a set of 5 LEPS detectors. Level schemes were constructed for Xe isotopes with masses ranging from 138 to 144. Except for {sup 139}Xe, none of them exhibit an alternating parity quasimolecular band, {alpha} feature usually encountered in octupole deformed nuclei. Substantial evidence for reflection asymmetric shape in the intrinsic system of the nucleus exists for the light actinide nuclei.

  18. FY06 ANNUAL REPORT FOR ENVIRONMENTAL MANAGEMENT SCIENCE PROGRAM PROJECT #95061STRATEGIC DESIGN AND OPTIMIZATION OF INORGANIC SORBENTSFOR CESIUM, STRONTIUM AND ACTINIDES

    SciTech Connect

    Hobbs, D

    2006-08-10

    The basic science goal in this project identifies structure/affinity relationships for selected radionuclides and existing sorbents. The task will apply this knowledge to the design and synthesis of new sorbents that will exhibit increased affinity for cesium, strontium and actinide separations. The target problem focuses on the treatment of high-level nuclear wastes. The general approach can likewise be applied to nonradioactive separations. During the fifth year of the project our studies focused along the following paths: (1) determination of Cs{sup +} ion exchange mechanism in sodium titanium silicates with sitinikite topology and the influence of crystallinity on ion exchange, (2) synthesis and characterization of novel peroxo-titanate materials for strontium and actinide separations, and (3) further refinements in computational models for the CST and polyoxoniobate materials.

  19. 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.

  20. Microbial Transformations of TRU and Mixed Wastes: Actinide Speciation and Waste Volume Reduction

    SciTech Connect

    Halada, Gary P.

    2005-06-01

    Cellosic samples were prepared 1/29/92 at BNL from various sources, including white and brown paper towel, and Kimwipes. The mixed cellulosics were cut into 1 cm x 1 cm squares and transferred to glass serum bottles and various treatments were conducted: unamended (U) samples were filled with nitrogen-purged brine from G-Seep (4.1 M Na+ and 5.1 Cl- with minor amounts of Mg, K, and Ca and 0.3 M sulfate (Brush, 1990)); unamended/inoculated (UI) samples were filled with bacteria-containing surface lake water, sediment, and halite from the underground at the WIPP site; amended/inoculated (AI) samples were inoculated in this fashion and amended with nutrients; and amended/inoculated/excess nitrate (AINO3) samples were inoculated with excess nitrate in the form of KNO3 (5 g L-1 (49.5 mM)). Further information on sample preparation is available. All samples were analyzed by Fourier transform infrared spectroscopy (FTIR) at SBU to identify any transformations in cellulosic material which may have occurred during treatment and storage.