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Sample records for actinides thorium uranium

  1. Minor actinide transmutation in thorium and uranium matrices in heavy water moderated reactors

    SciTech Connect

    Bhatti, Zaki; Hyland, B.; Edwards, G.W.R.

    2013-07-01

    The irradiation of Th{sup 232} breeds fewer of the problematic minor actinides (Np, Am, Cm) than the irradiation of U{sup 238}. This characteristic makes thorium an attractive potential matrix for the transmutation of these minor actinides, as these species can be transmuted without the creation of new actinides as is the case with a uranium fuel matrix. Minor actinides are the main contributors to long term decay heat and radiotoxicity of spent fuel, so reducing their concentration can greatly increase the capacity of a long term deep geological repository. Mixing minor actinides with thorium, three times more common in the Earth's crust than natural uranium, has the additional advantage of improving the sustainability of the fuel cycle. In this work, lattice cell calculations have been performed to determine the results of transmuting minor actinides from light water reactor spent fuel in a thorium matrix. 15-year-cooled group-extracted transuranic elements (Np, Pu, Am, Cm) from light water reactor (LWR) spent fuel were used as the fissile component in a thorium-based fuel in a heavy water moderated reactor (HWR). The minor actinide (MA) transmutation rates, spent fuel activity, decay heat and radiotoxicity, are compared with those obtained when the MA were mixed instead with natural uranium and taken to the same burnup. Each bundle contained a central pin containing a burnable neutron absorber whose initial concentration was adjusted to have the same reactivity response (in units of the delayed neutron fraction β) for coolant voiding as standard NU fuel. (authors)

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

    SciTech Connect

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

    2013-12-01

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

  3. 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.

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

    SciTech Connect

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

    2014-04-01

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

  5. Identification of hexanuclear Actinide(IV) carboxylates with Thorium, Uranium and Neptunium by EXAFS spectroscopy

    NASA Astrophysics Data System (ADS)

    Hennig, Christoph; Takao, Shinobu; Takao, Koichiro; Weiss, Stephan; Kraus, Werner; Emmerling, Franziska; Meyer, Michel; Scheinost, Andreas C.

    2013-04-01

    Hydrated actinide(IV) ions undergo hydrolysis and further polymerization and precipitation with increasing pH. The resulting amorphous and partly crystalline oxydydroxides AnOn(OH)4-2n·xH2O can usually be observed as colloids above the An(IV) solubility limit. The aging process of such colloids results in crystalline AnO2. The presence of carboxylates in the solution prevents the occurrence of such colloids by formation of polynuclear complexes through a competing reaction between hydrolysis and ligation. The majority of recently described carboxylates reveals a hexanuclear core of [An6(μ3-O)4(μ3-OH)4]12+ terminated by 12 carboxylate ligands. We found that the An(IV) carboxylate solution species remain often preserved in crystalline state. The An(IV) carboxylates show An-An distances which are ~ 0.03 Å shorter than the An-An distances in AnO2 like colloids. The difference in the distances could be used to identify such species in solution.

  6. ELECTROLYSIS OF THORIUM AND URANIUM

    DOEpatents

    Hansen, W.N.

    1960-09-01

    An electrolytic method is given for obtaining pure thorium, uranium, and thorium-uranium alloys. The electrolytic cell comprises a cathode composed of a metal selected from the class consisting of zinc, cadmium, tin, lead, antimony, and bismuth, an anode composed of at least one of the metals selected from the group consisting of thorium and uranium in an impure state, and an electrolyte composed of a fused salt containing at least one of the salts of the metals selected from the class consisting of thorium, uranium. zinc, cadmium, tin, lead, antimony, and bismuth. Electrolysis of the fused salt while the cathode is maintained in the molten condition deposits thorium, uranium, or thorium-uranium alloys in pure form in the molten cathode which thereafter may be separated from the molten cathode product by distillation.

  7. SEPARATION OF THORIUM FROM URANIUM

    DOEpatents

    Bane, R.W.

    1959-09-01

    A description is given for the separation of thorium from uranium by forming an aqueous acidic solution containing ionic species of thorium, uranyl uranium, and hydroxylamine, flowing the solution through a column containing the phenol-formaldehyde type cation exchange resin to selectively adsorb substantially all the thorium values and a portion of the uranium values, flowing a dilute solution of hydrochloric acid through the column to desorb the uranium values, and then flowing a dilute aqueous acidic solution containing an ion, such as bisulfate, which has a complexing effect upon thortum through the column to desorb substantially all of the thorium.

  8. SEPARATION OF URANIUM FROM THORIUM

    DOEpatents

    Hellman, N.N.

    1959-07-01

    A process is presented for separating uranium from thorium wherein the ratio of thorium to uranium is between 100 to 10,000. According to the invention the thoriumuranium mixture is dissolved in nitric acid, and the solution is prepared so as to obtain the desired concentration within a critical range of from 4 to 8 N with regard to the total nitrate due to thorium nitrate, with or without nitric acid or any nitrate salting out agent. The solution is then contacted with an ether, such as diethyl ether, whereby uranium is extracted into ihe organic phase while thorium remains in the aqueous phase.

  9. Uranium and Thorium

    ERIC Educational Resources Information Center

    Finch, Warren I.

    1978-01-01

    The results of President Carter's policy on non-proliferation of nuclear weapons are expected to slow the growth rate in energy consumption, put the development of the breeder reactor in question, halt plans to reprocess and recycle uranium and plutonium, and expand facilities to supply enriched uranium. (Author/MA)

  10. PRODUCTION OF URANIUM AND THORIUM COMPOUNDS

    DOEpatents

    Arden, T.V.; Burstall, F.H.; Linstead, R.P.; Wells, R.A.

    1955-12-27

    Compounds of Th and U are extracted with an organic solvent in the presence of an adsorbent substance which has greater retentivity for impurities present than for the uranium and/or thorium. The preferred adsorbent material is noted as being cellulose. The uranium and thoriumcontaining substances treated are preferably in the form of dissolved nitrates, and the preferred organic solvent is diethyl ether.

  11. SEPARATION OF THORIUM FROM URANIUM BY EXTRACTION

    DOEpatents

    Bohlmann, E.G.

    1959-07-28

    A method is presented for the recovery and separation of uranium and thorium values contained in an aqueous nitric acid solution which is more than 3 M in nitric acid. The uranium and thorium containing solution preferable about 7 M in nitric acid is contacted with tributyl phosphatekerosene mixture. Both U and Th are extracted by the immiscible organic. After phase separation the Th is selectively back extracted by contacting with an aqueous nitric acid solution preferably between 0.1 to 1.5 M in nitric acid. The uranium which is still in the organic extractant phase may be recovered by contacting with water.

  12. SEPARATION OF URANIUM FROM THORIUM AND PROTACTINIUM

    DOEpatents

    Musgrave, W.K.R.

    1959-06-30

    This patent relates to the separation of uranium from thorium and protactinium; such mixtures of elements usually being obtained by neutron irradiation of thorium. The method of separating the constituents has been first to dissolve the mixture of elements in concertrated nitric acid and then to remove the protactinium by absorption on manganese dioxide and the uranium by solvent extraction with ether. Prior to now, comparatively large amounts of thorium were extracted with the uranium. According to the invention this is completely prevented by adding sodium diethyldithiocarbamate to the mixture of soluble nitrate salts. The organic salt has the effect of reacting only with the uranyl nitrate to form the corresponding uranyl salt which can then be selectively extracted from the mixture with amyl acetate.

  13. Comparison of the radiological hazard of thorium and uranium spent fuels from VVER-1000 reactor

    NASA Astrophysics Data System (ADS)

    Frybort, Jan

    2014-11-01

    Thorium fuel is considered as a viable alternative to the uranium fuel used in the current generation of nuclear power plants. Switch from uranium to thorium means a complete change of composition of the spent nuclear fuel produced as a result of the fuel depletion during operation of a reactor. If the Th-U fuel cycle is implemented, production of minor actinides in the spent fuel is negligible. This is favourable for the spent fuel disposal. On the other hand, thorium fuel utilisation is connected with production of 232U, which decays via several alpha decays into a strong gamma emitter 208Tl. Presence of this nuclide might complicate manipulations with the irradiated thorium fuel. Monte-Carlo computation code MCNPX can be used to simulate thorium fuel depletion in a VVER-1000 reactor. The calculated actinide composition will be analysed and dose rate from produced gamma radiation will be calculated. The results will be compared to the reference uranium fuel. Dependence of the dose rate on time of decay after the end of irradiation in the reactor will be analysed. This study will compare the radiological hazard of the spent thorium and uranium fuel handling.

  14. Nitrite complexes of uranium and thorium.

    PubMed

    Dulong, Florian; Pouessel, Jacky; Thuéry, Pierre; Berthet, Jean-Claude; Ephritikhine, Michel; Cantat, Thibault

    2013-03-25

    The first examples of inorganic nitrite complexes of the natural actinides are described, including the structures of the homoleptic thorium(IV) [PPh(4)](2)[Th(NO(2))(6)] and the uranyl(VI) [PPh(4)](2)[UO(2)(NO(2))(4)] complexes; the nitrite ligand can adopt two different coordination modes in the coordination sphere of the uranyl ion and is unstable towards reduction.

  15. A method for the rapid radiochemical analysis of uranium and thorium isotopes in impure carbonates.

    PubMed

    Elyahyaoui, A; Zarki, R; Chiadli, A

    2003-01-01

    A simple method combining solvent extraction and electrodeposition procedures is described for the determination of the isotopic composition and content of uranium and thorium in travertine samples. The actinide elements are extracted with diethyl ether from a calcium nitrate solution. The isolation of the elements and the alpha source preparation are performed in two steps after the sample digestion. The acid leaching of samples is performed using both partial and total dissolution methods. High recoveries of both uranium and thorium and good alpha-spectra are obtained with both partial and total dissolution methods.

  16. Evidence for the involvement of 5f orbitals in the bonding and reactivity of organometallic actinide compounds: thorium(IV) and uranium(IV) bis(hydrazonato) complexes.

    PubMed

    Cantat, Thibault; Graves, Christopher R; Jantunen, Kimberly C; Burns, Carol J; Scott, Brian L; Schelter, Eric J; Morris, David E; Hay, P Jeffrey; Kiplinger, Jaqueline L

    2008-12-24

    Migratory insertion of diphenyldiazomethane into both metal-carbon bonds of the bis(alkyl) and bis(aryl) complexes (C(5)Me(5))(2)AnR(2) yields the first f-element bis(hydrazonato) complexes (C(5)Me(5))(2)An[eta(2)-(N,N')-R-N-N=CPh(2)](2) [An = Th, R = CH(3) (18), PhCH(2) (15), Ph (16); An = U, R = CH(3) (17), PhCH(2) (14)], which have been characterized by a combination of spectroscopy, electrochemistry, and X-ray crystallography. The two hydrazonato ligands adopt an eta(2)-coordination mode leading to 20-electron (for Th) and 22-electron (for U) complexes that have no transition-metal analogues. In fact, reaction of (C(5)H(5))(2)Zr(CH(3))(2) or (C(5)Me(5))(2)Hf(CH(3))(2) with diphenyldiazomethane is limited to the formation of the corresponding mono(hydrazonato) complex (C(5)R(5))(2)M[eta(2)-(N,N')-CH(3)-N-N=CPh(2)](CH(3)) (M = Zr, R = H or M = Hf, R = CH(3)). The difference in the reactivities of the group 4 metal complexes and the actinides was used as a unique platform for investigating in depth the role of 5f orbitals on the reactivity and bonding in actinide organometallic complexes. The electronic structure of the (C(5)H(5))(2)M[eta(2)-(N,N')-CH(3)-N-N=CH(2)](2) (M = Zr, Th, U) model complexes was studied using density functional theory (DFT) calculations and compared to experimental structural, electrochemical, and spectroscopic results. Whereas transition-metal bis(cyclopentadienyl) complexes are known to stabilize three ligands in the metallocene girdle to form saturated (C(5)H(5))(2)ML(3) species, in a bis(hydrazonato) system, a fourth ligand is coordinated to the metal center to give (C(5)H(5))(2)ML(4). DFT calculations have shown that 5f orbitals in the actinide complexes play a crucial role in stabilizing this fourth ligand by stabilizing both the sigma and pi electrons of the two eta(2)-coordinated hydrazonato ligands. In contrast, the stabilization of the hydrazonato ligands was found to be significantly less effective for the putative bis

  17. Smart thorium and uranium determination exploiting renewable solid-phase extraction applied to environmental samples in a wide concentration range.

    PubMed

    Avivar, Jessica; Ferrer, Laura; Casas, Montserrat; Cerdà, Víctor

    2011-07-01

    A smart fully automated system is proposed for determination of thorium and uranium in a wide concentration range, reaching environmental levels. The hyphenation of lab-on-valve (LOV) and multisyringe flow injection analysis (MSFIA), coupled to a long path length liquid waveguide capillary cell, allows the spectrophotometric determination of thorium and uranium in different types of environmental sample matrices achieving high selectivity and sensitivity levels. Online separation and preconcentration of thorium and uranium is carried out by means of Uranium and TEtraValents Actinides resin. The potential of the LOV-MSFIA makes possible the full automation of the system by the in-line regeneration of the column and its combination with a smart methodology is a step forward in automation. After elution, thorium(IV) and uranium(VI) are spectrophotometrically detected after reaction with arsenazo-III. We propose a rapid, inexpensive, and fully automated method to determine thorium(IV) and uranium(VI) in a wide concentration range (0-1,200 and 0-2,000 μg L(-1) Th and U, respectively). Limits of detection reached are 5.9 ηg L(-1) of uranium and 60 ηg L(-1) of thorium. Different water sample matrices (seawater, well water, freshwater, tap water, and mineral water), and a channel sediment reference material which contained thorium and uranium were satisfactorily analyzed with the proposed method.

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

    SciTech Connect

    Marcalo, Joaquim; Gibson, John K.

    2009-08-10

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

  19. Gas-Phase Energetics of Actinide Oxides: An Assessment of Neutral and Cationic Monoxides and Dioxides from Thorium to Curium

    NASA Astrophysics Data System (ADS)

    Marçalo, Joaquim; Gibson, John K.

    2009-09-01

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

  20. Gas-phase energetics of actinide oxides: an assessment of neutral and cationic monoxides and dioxides from thorium to curium.

    PubMed

    Marçalo, Joaquim; Gibson, John K

    2009-11-12

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

  1. Infrared emission spectra or uranium and thorium

    SciTech Connect

    Palmer, B.A.; Phillips, M.V.; Engleman, R. Jr.

    1983-01-01

    The region between 1 and 5.5 ..mu..m has been observed with a high-resolution Fourier transform spectrometer. See-through hollow cathode lamps with calcium fluoride windows were operated at high current. Special precautions were required to minimize interference by blackbody radiation from the hot cathode. Observed lines were measured to an absolute accuracy of about 0.001 cm/sup -1/ and about 5% relative intensity accuracy. The argon carrier gas lines were readily distinguished by their much wider Doppler-broadened linewidths. Many lines were assigned to neutral or singly-ionized thorium on the basis of predicted transition wavenumbers calculated from accurate level lists. However, many lines remain to be assigned. This new spectral data connects to, and extends similar, spectral information given in our uranium and thorium atlases which cover the ultraviolet and visible regions.

  2. Evolution of uranium and thorium minerals

    NASA Astrophysics Data System (ADS)

    Hazen, R. M.; Ewing, R. C.; Sverjensky, D. A.

    2009-12-01

    The origins and near-surface distributions of the approximately 250 known uranium and/or thorium minerals elucidate principles of mineral evolution. This history can be divided into four phases. The first, from ~4.5 to 3.5 Ga, involved successive concentrations of uranium and thorium from their initial uniform trace distribution into magmatic-related fluids from which the first U4+ and Th4+ minerals, uraninite (UO2), thorianite (ThO2) and coffinite (USiO4), precipitated in the crust. The second period, from ~3.5 to 2.2 Ga, saw the formation of large low-grade concentrations of detrital uraninite (containing several weight percent Th) in the Witwatersrand-type quartz-pebble conglomerates deposited in a highly anoxic fluvial environment. Abiotic alteration of uraninite and coffinite, including radiolysis and auto-oxidation caused by radioactive decay and the formation of helium from alpha particles, may have resulted in the formation of a limited suite of uranyl oxide-hydroxides. Earth’s third phase of uranium mineral evolution, during which most known U minerals first precipitated from reactions of soluble uranyl (U6+O2)2+ complexes, followed the Great Oxidation Event (GOE) at ~2.2 Ga and thus was mediated indirectly by biologic activity. Most uraninite deposited during this phase was low in Th and precipitated from saline and oxidizing hydrothermal solutions (100 to 300°C) transporting (UO2)2+-chloride complexes. Examples include the unconformity- and vein-type U deposits (Australia and Canada) and the unique Oklo natural nuclear reactors in Gabon. The onset of hydrothermal transport of (UO2)2+ complexes in the upper crust may reflect the availability of CaSO4-bearing evaporites after the GOE. During this phase, most uranyl minerals would have been able to form in the O2-bearing near-surface environment for the first time through weathering processes. The fourth phase of uranium mineralization began approximately 400 million years ago, as the rise of land plants

  3. ADSORPTION METHOD FOR SEPARATING THORIUM VALUES FROM URANIUM VALUES

    DOEpatents

    Boyd, G.E.; Russell, E.R.; Schubert, J.

    1959-08-01

    An improved ion exchange method is described for recovery of uranium and thorium values as separate functions from an aqueous acidic solution containing less than 10/sup -3/ M thorium ions and between 0.1 and 1 M uranyl ions. The solution is passed through a bed of cation exchange resin in the acid form to adsorb all the thorium ions and a portion of the uranyl ions. The uranium is eluted by means of aqueous 0.1 to 0.4 M sulfuric acid. The thorium may then be stripped from the resin by elution with aqueous 0.5 M oxalic acid.

  4. RECOVERY OF URANIUM AND THORIUM FROM AQUEOUS SOLUTIONS

    DOEpatents

    Calkins, G.D.

    1958-06-10

    >A process is described for the recovery of uranium and thorium from monazite sand, which is frequently processed by treating it with a hot sodium hydroxide solution whereby a precipitate forms consisting mainly of oxides or hydroxides of the rare earths, thorium and uranium. The precipitate is dissolved in mineral acid, and the acid solution is then neutralized to a pH value of between 5.2 and 6.2 whereby both the uranium and thorium precipitate as the hydroxides, while substantially all the rare earth metal values present remain in the solution. The uranium and thoriunn can then be separated by dissolving the precipitate in a solution containing a mixture of alkali carbonate and alkali bicarbonate: and contacting the carbonate solution with a strong-base anion exchange resin whereby the uranium values are adsorbed on the resin while the thorium remains in solution.

  5. 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.

  6. 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.

  7. Uranium and thorium sorption on minerals studied by x-ray absorption spectroscopy

    SciTech Connect

    Hudson, E.A.; Terminello, L.J.; Viani, B.E.

    1995-12-01

    Several actinide-mineral sorption systems were studied by uranium and thorium L{sub 3}-edge x-ray absorption spectroscopy. A series of layer silicate minerals, including micas, were selected for their systematic variations in surface structure, e.g. degree of permanent negative charge on the basal planes. An expansible layer silicate, vermiculite, was treated to provide several different interlayer spacings, allowing variations in the accessibility of interior cation exchange sites. The finely powdered minerals were exposed to aqueous solutions of uranyl chloride or thorium chloride. Analysis of the EXAFS and XANES spectra indicates the influence of the mineral substrate upon the local structure of the bound actinide species. Trends in the data are interpreted based upon the known variations in mineral structure.

  8. 49 CFR 173.434 - Activity-mass relationships for uranium and natural thorium.

    Code of Federal Regulations, 2012 CFR

    2012-10-01

    ... natural thorium. 173.434 Section 173.434 Transportation Other Regulations Relating to Transportation....434 Activity-mass relationships for uranium and natural thorium. The table of activity-mass relationships for uranium and natural thorium are as follows: Thorium and uranium enrichment 1(Wt% 235 U...

  9. 49 CFR 173.434 - Activity-mass relationships for uranium and natural thorium.

    Code of Federal Regulations, 2011 CFR

    2011-10-01

    ... natural thorium. 173.434 Section 173.434 Transportation Other Regulations Relating to Transportation....434 Activity-mass relationships for uranium and natural thorium. The table of activity-mass relationships for uranium and natural thorium are as follows: Thorium and uranium enrichment 1(Wt% 235 U...

  10. 49 CFR 173.434 - Activity-mass relationships for uranium and natural thorium.

    Code of Federal Regulations, 2014 CFR

    2014-10-01

    ... natural thorium. 173.434 Section 173.434 Transportation Other Regulations Relating to Transportation....434 Activity-mass relationships for uranium and natural thorium. The table of activity-mass relationships for uranium and natural thorium are as follows: Thorium and uranium enrichment 1(Wt% 235 U...

  11. 49 CFR 173.434 - Activity-mass relationships for uranium and natural thorium.

    Code of Federal Regulations, 2013 CFR

    2013-10-01

    ... natural thorium. 173.434 Section 173.434 Transportation Other Regulations Relating to Transportation....434 Activity-mass relationships for uranium and natural thorium. The table of activity-mass relationships for uranium and natural thorium are as follows: Thorium and uranium enrichment 1(Wt% 235 U...

  12. 49 CFR 173.434 - Activity-mass relationships for uranium and natural thorium.

    Code of Federal Regulations, 2010 CFR

    2010-10-01

    ... natural thorium. 173.434 Section 173.434 Transportation Other Regulations Relating to Transportation....434 Activity-mass relationships for uranium and natural thorium. The table of activity-mass relationships for uranium and natural thorium are as follows: Thorium and uranium enrichment 1(Wt% 235 U...

  13. RECOVERY OF THORIUM AND URANIUM VALUES FROM AQUEOUS SOLUTIONS

    DOEpatents

    Calkins, G.D.

    1958-02-18

    This patent deals with the separation and recovery of uranium from monazite sand. After initial treatment of the sand with sodium hydroxide, a precipitate is obtuined which contains the uranium, thorium, rare earths and some phosphorus. This precipitate is then dissolved in nitric acid. The bulk of the rare earths are removed from thls soiution by adding aa excess of alkali carbonate, causing precipitation of the rare earths together with part of the thorium present. The solution still contains a considerable amount of thorium, some rare earths, and practically all of the uranium originally present. Thorium and rare earth values are readily precipitated from such solution, and the uranium values thus isolated, by the addition of an excess hydrogen peroxide. The pH value of the solution is preferably adjusted to at least 9 prior to the addition of the peroxide.

  14. Tables for determining lead, uranium, and thorium isotope ages

    NASA Technical Reports Server (NTRS)

    Schonfeld, E.

    1974-01-01

    Tables for determining lead, uranium, and thorium isotope ages are presented in the form of computer printouts. Decay constants, analytical expressions for the functions evaluated, and the precision of the calculations are briefly discussed.

  15. Uranium- and thorium-doped graphene for efficient oxygen and hydrogen peroxide reduction.

    PubMed

    Sofer, Zdeněk; Jankovský, Ondřej; Šimek, Petr; Klímová, Kateřina; Macková, Anna; Pumera, Martin

    2014-07-22

    Oxygen reduction and hydrogen peroxide reduction are technologically important reactions in the fields of energy generation and sensing. Metal-doped graphenes, where metal serves as the catalytic center and graphene as the high area conductor, have been used as electrocatalysts for such applications. In this paper, we investigated the use of uranium-graphene and thorium-graphene hybrids prepared by a simple and scalable method. The hybrids were synthesized by the thermal exfoliation of either uranium- or thorium-doped graphene oxide in various atmospheres. The synthesized graphene hybrids were characterized by high-resolution XPS, SEM, SEM-EDS, combustible elemental analysis, and Raman spectroscopy. The influence of dopant and exfoliation atmosphere on electrocatalytic activity was determined by electrochemical measurements. Both hybrids exhibited excellent electrocatalytic properties toward oxygen and hydrogen peroxide reduction, suggesting that actinide-based graphene hybrids have enormous potential for use in energy conversion and sensing devices.

  16. Laser-induced breakdown spectroscopy measurements of uranium and thorium powders and uranium ore

    NASA Astrophysics Data System (ADS)

    Judge, Elizabeth J.; Barefield, James E., II; Berg, John M.; Clegg, Samuel M.; Havrilla, George J.; Montoya, Velma M.; Le, Loan A.; Lopez, Leon N.

    2013-05-01

    Laser-induced breakdown spectroscopy (LIBS) was used to analyze depleted uranium and thorium oxide powders and uranium ore as a potential rapid in situ analysis technique in nuclear production facilities, environmental sampling, and in-field forensic applications. Material such as pressed pellets and metals, has been extensively studied using LIBS due to the high density of the material and more stable laser-induced plasma formation. Powders, on the other hand, are difficult to analyze using LIBS since ejection and removal of the powder occur in the laser interaction region. The capability of analyzing powders is important in allowing for rapid analysis of suspicious materials, environmental samples, or trace contamination on surfaces since it most closely represents field samples (soil, small particles, debris etc.). The rapid, in situ analysis of samples, including nuclear materials, also reduces costs in sample collection, transportation, sample preparation, and analysis time. Here we demonstrate the detection of actinides in oxide powders and within a uranium ore sample as both pressed pellets and powders on carbon adhesive discs for spectral comparison. The acquired LIBS spectra for both forms of the samples differ in overall intensity but yield a similar distribution of atomic emission spectral lines.

  17. 76 FR 30696 - Reimbursement for Costs of Remedial Action at Active Uranium and Thorium Processing Sites

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-05-26

    ... Reimbursement for Costs of Remedial Action at Active Uranium and Thorium Processing Sites AGENCY: Department of... eligible active uranium and thorium processing site licensees for reimbursement under Title X of the Energy... requires DOE to reimburse eligible uranium and thorium licensees for certain costs of...

  18. 75 FR 71677 - Reimbursement for Costs of Remedial Action at Active Uranium and Thorium Processing Sites

    Federal Register 2010, 2011, 2012, 2013, 2014

    2010-11-24

    ... Reimbursement for Costs of Remedial Action at Active Uranium and Thorium Processing Sites AGENCY: Department of... uranium and thorium processing site licensees for reimbursement under Title X of the Energy Policy Act of... requires DOE to reimburse eligible uranium and thorium licensees for certain costs of...

  19. 76 FR 24871 - Reimbursement for Costs of Remedial Action at Active Uranium and Thorium Processing Sites

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-05-03

    ... Reimbursement for Costs of Remedial Action at Active Uranium and Thorium Processing Sites AGENCY: Department of... from eligible active uranium and thorium processing site licensees for reimbursement under Title X of...). Title X requires DOE to reimburse eligible uranium and thorium licensees for certain costs...

  20. Estimating terrestrial uranium and thorium by antineutrino flux measurements.

    PubMed

    Dye, Stephen T; Guillian, Eugene H

    2008-01-08

    Uranium and thorium within the Earth produce a major portion of terrestrial heat along with a measurable flux of electron antineutrinos. These elements are key components in geophysical and geochemical models. Their quantity and distribution drive the dynamics, define the thermal history, and are a consequence of the differentiation of the Earth. Knowledge of uranium and thorium concentrations in geological reservoirs relies largely on geochemical model calculations. This article describes the methods and criteria to experimentally determine average concentrations of uranium and thorium in the continental crust and in the mantle by using site-specific measurements of the terrestrial antineutrino flux. Optimal, model-independent determinations involve significant exposures of antineutrino detectors remote from nuclear reactors at both a midcontinental and a midoceanic site. This would require major, new antineutrino detection projects. The results of such projects could yield a greatly improved understanding of the deep interior of the Earth.

  1. A Thorium/Uranium fuel cycle for an advanced accelerator transmutation of nuclear waste concept

    SciTech Connect

    Truebenbach, M.T.; Henderson, D.L.; Venneri, F.

    1993-12-31

    Utilizing the high thermal neutron flux of an accelerator driven transmuter to drive a Thorium-Uranium fuel production scheme, it is possible to produce enough energy in the transmuter not only to power the accelerator, but to have enough excess power available for commercial use. A parametric study has been initiated to determine the ``optimum`` equilibrium operation point in terms of the minimization of the equilibrium actinide inventory and the fuel {alpha} for various residence times in the High Flux Region (HFR) and in the Low Flux Region (LFR). For the cases considered, the ``optimum`` equilibrium operation point was achieved for a HFR residence time of 45 days and a LFR residence time of 60 days. For this case, the total actinide inventory in the system is about 20 tonnes and the fuel {alpha} approximately 1.46.

  2. Uranium- and thorium-bearing pegmatites of the United States

    SciTech Connect

    Adams, J.W.; Arengi, J.T.; Parrish, I.S.

    1980-04-01

    This report is part of the National Uranium Resource Evaluation (NURE) Program designed to identify criteria favorable for the occurrence of the world's significant uranium deposits. This project deals specifically with uranium- and thorium-bearing pegmatites in the United States and, in particular, their distribution and origin. From an extensive literature survey and field examination of 44 pegmatite localities in the United States and Canada, the authors have compiled an index to about 300 uranium- and thorium-bearing pegmatites in the United States, maps giving location of these deposits, and an annotated bibliography to some of the most pertinent literature on the geology of pegmatites. Pegmatites form from late-state magma differentiates rich in volatile constituents with an attendant aqueous vapor phase. It is the presence of an aqueous phase which results in the development of the variable grain size which characterizes pegmatites. All pegmatites occur in areas of tectonic mobility involving crustal material usually along plate margins. Those pegmatites containing radioactive mineral species show, essentially, a similar distribution to those without radioactive minerals. Criteria such as tectonic setting, magma composition, host rock, and elemental indicators among others, all serve to help delineate areas more favorable for uranium- and thorium-bearing pegmatites. The most useful guide remains the radioactivity exhibited by uranium- and thorium-bearing pegmatites. Although pegmatites are frequently noted as favorable hosts for radioactive minerals, the general paucity and sporadic distribution of these minerals and inherent mining and milling difficulties negate the resource potential of pegmatites for uranium and thorium.

  3. Configurational analysis of uranium-doped thorium dioxide

    NASA Astrophysics Data System (ADS)

    Shields, A. E.; Ruiz-Hernandez, S. E.; de Leeuw, N. H.

    2015-04-01

    While thorium dioxide is already used industrially in high temperature applications, more insight is needed about the behaviour of the material as part of a mixed-oxide (MOX) nuclear fuel, incorporating uranium. We have developed a new interatomic potential model, commensurate with a prominent existing UO2 potential, to conduct configurational analyses of uranium-doped ThO2 supercells. Using the GULP and Site Occupancy Disorder (SOD) computational codes, we have analysed the distribution of low concentrations of uranium in the bulk material, but have not observed the formation of uranium clusters or a single dominant configuration.

  4. Separation of thorium and uranium in nitric acid solution using silica based anion exchange resin.

    PubMed

    Chen, Yanliang; Wei, Yuezhou; He, Linfeng; Tang, Fangdong

    2016-09-30

    To separate thorium and uranium in nitric acid solution using anion exchange process, a strong base silica-based anion exchange resin (SiPyR-N4) was synthesized. Batch experiments were conducted and the separation factor of thorium and uranium in 9M nitric acid was about 10. Ion exchange chromatography was applied to separate thorium and uranium in different ratios. Uranium could be eluted by 9M nitric acid and thorium was eluted by 0.1M nitric acid. It was proved that thorium and uranium can be separated and recovered successfully by this method.

  5. Discovery of actinium, thorium, protactinium, and uranium isotopes

    NASA Astrophysics Data System (ADS)

    Fry, C.; Thoennessen, M.

    2013-05-01

    Thirty-one actinium, thirty-one thorium, twenty-eight protactinium, and twenty-three uranium isotopes have so far been observed; the discovery of these isotopes is described. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  6. Helium on Venus - Implications for uranium and thorium

    NASA Technical Reports Server (NTRS)

    Prather, M. J.; Mcelroy, M. B.

    1983-01-01

    Helium is removed at an average rate of 10 to the 6th atoms per square centimeter per second from Venus's atmosphere by the solar wind following ionization above the plasmapause. The surface source of helium-4 on Venus is similar to that on earth, suggesting comparable abundances of crustal uranium and thorium.

  7. 49 CFR 173.426 - Excepted packages for articles containing natural uranium or thorium.

    Code of Federal Regulations, 2012 CFR

    2012-10-01

    ... uranium or thorium. 173.426 Section 173.426 Transportation Other Regulations Relating to Transportation....426 Excepted packages for articles containing natural uranium or thorium. A manufactured article in... or natural thorium, and its packaging, are excepted from the requirements in this subchapter...

  8. 49 CFR 173.426 - Excepted packages for articles containing natural uranium or thorium.

    Code of Federal Regulations, 2013 CFR

    2013-10-01

    ... uranium or thorium. 173.426 Section 173.426 Transportation Other Regulations Relating to Transportation....426 Excepted packages for articles containing natural uranium or thorium. A manufactured article in... or natural thorium, and its packaging, are excepted from the requirements in this subchapter...

  9. 49 CFR 173.426 - Excepted packages for articles containing natural uranium or thorium.

    Code of Federal Regulations, 2011 CFR

    2011-10-01

    ... uranium or thorium. 173.426 Section 173.426 Transportation Other Regulations Relating to Transportation....426 Excepted packages for articles containing natural uranium or thorium. A manufactured article in... or natural thorium, and its packaging, are excepted from the requirements in this subchapter...

  10. 49 CFR 173.426 - Excepted packages for articles containing natural uranium or thorium.

    Code of Federal Regulations, 2014 CFR

    2014-10-01

    ... uranium or thorium. 173.426 Section 173.426 Transportation Other Regulations Relating to Transportation....426 Excepted packages for articles containing natural uranium or thorium. A manufactured article in... or natural thorium, and its packaging, are excepted from the requirements in this subchapter...

  11. 49 CFR 173.426 - Excepted packages for articles containing natural uranium or thorium.

    Code of Federal Regulations, 2010 CFR

    2010-10-01

    ... uranium or thorium. 173.426 Section 173.426 Transportation Other Regulations Relating to Transportation....426 Excepted packages for articles containing natural uranium or thorium. A manufactured article in... or natural thorium, and its packaging, are excepted from the requirements in this subchapter...

  12. Functional Sorbents for Selective Capture of Plutonium, Americium, Uranium, and Thorium in Blood

    SciTech Connect

    Yantasee, Wassana; Sangvanich, Thanapon; Creim, Jeffrey A.; Pattamakomsan, Kanda; Wiacek, Robert J.; Fryxell, Glen E.; Addleman, Raymond S.; Timchalk, Charles

    2010-09-01

    Nano-engineered solid sorbents for chelation of actinides (239Pu, 241Am, uranium, thorium) from human blood were developed and evaluated in vitro. These sorbents, known as the self-assembled monolayer on mesoporous supports (SAMMSTM), are hybrid materials created from attachment of organic moieties onto extremely high surface area mesoporous silica. The organic moieties known to be effective at capturing actinides including three isomers of hydroxypyridinone, diphosphonic acid, acetamide phosphonic acid, glycinyl urea, and diethylenetriamine pentaacetate analog were evaluated. SAMMS are being reported elsewhere as potential candidates for orally administered drug for radionuclide decorporation. Herein, actinide decorporation of SAMMS in blood were evaluated to assess their viability for sorbent hemoperfusion in renal insufficient patients, whose kidney clear radionuclides at very slow rate. Sorption affinity (Kd), sorption rate, selectivity, and stability of SAMMS were measured in batch contact experiments. An isomer of hydroxypyridinone (3,4-HOPO) on SAMMS demonstrated the highest affinity for decorporation of all four actinides and outperformed the DTPA analog on SAMMS and on commercial resins by a factor of 103-fold in term of affinity. A fifty percent reduction of actinides in blood was achieved within minutes with no evidence of protein fouling and material leaching in blood after 24 hr of contact time. Less than 0.4 wt.% of Si was dissolved from 3,4-HOPO-SAMMS across the pH of 0 to 8. The engineered form of SAMMS (bead format) was further evaluated in a 100-fold scaled-down hemoperfusion device and showed no blood clotting after 2 hr. A 0.2 g of SAMMS could reduce 50 wt.% of 100 ppb uranium in 50 mL of plasma in just 18 min and that of 500 dpm mL-1 in just 24 min. 3,4-HOPO-SAMMS has a long shelf-life in air and at room temperature for at least 8 years, indicating their feasibility for stockpiling in preparedness for emergency.

  13. PROCESS FOR DECONTAMINATING THORIUM AND URANIUM WITH RESPECT TO RUTHENIUM

    DOEpatents

    Meservey, A.A.; Rainey, R.H.

    1959-10-20

    The control of ruthenium extraction in solvent-extraction processing of neutron-irradiated thorium is presented. Ruthenium is rendered organic-insoluble by the provision of sulfite or bisulfite ions in the aqueous feed solution. As a result the ruthenium remains in the aqueous phase along with other fission product and protactinium values, thorium and uranium values being extracted into the organic phase. This process is particularly applicable to the use of a nitrate-ion-deficient aqueous feed solution and to the use of tributyl phosphate as the organic extractant.

  14. Accelerator breeder with uranium, thorium target

    SciTech Connect

    Takahashi, H.; Powell, J.; Kouts, H.

    1983-01-01

    An accelerator breeder, that uses a low-enriched fuel as the target material, can produce substantial amounts of fissile material and electric power. A study of H/sub 2/O- and D/sub 2/O-cooled, UO/sub 2/, U, (depleted U), or thorium indicates that U-metal fuel produces a good fissile production rate and electrical power of about 60% higher than UO/sub 2/ fuel. Thorium fuel has the same order of magnitude as UO/sub 2/ fuel for fissile-fuel production, but the generating electric power is substantially lower than in a UO/sub 2/ reactor. Enriched UO/sub 2/ fuel increases the generating electric power but not the fissile-material production rate. The Na-cooled breeder target has many advantages over the H/sub 2/O-cooled breeder target.

  15. Coprecipitation of thorium and uranium peroxides from acid solutions

    SciTech Connect

    McTaggart, D.R.; Mailen, J.C.

    1981-01-01

    The factors affecting successful coprecipitation of thorium and uranium peroxides from acid media were studied. Variables considered in this work were H/sup +/ concentration, H/sub 2/O/sub 2/ concentration, duration of contact, and rate of feed solution addition. In all experiments, stock solutions of Th(NO/sub 3/)/sub 4/ and UO/sub 2/(NO/sub 3/)/sub 2/ were fed at a controlled rate into H/sub 2/O/sub 2/ solutions with constant stirring. Samples were taken as a function of time to follow the H/sup +/ concentration of the solution, uranium precipitation, thorium precipitation, precipitant weight/volume of solution, and crystalline structure and growth. The optimum conditions for maximum coprecipitation are low H/sup +/ concentration, high H/sub 2/O/sub 2/ concentration, and extended contact time between the solutions.

  16. SELECTIVE SEPARATION OF URANIUM FROM THORIUM, PROTACTINIUM AND FISSION PRODUCTS BY PEROXIDE DISSOLUTION METHOD

    DOEpatents

    Seaborg, G.T.; Gofman, J.W.; Stoughton, R.W.

    1959-08-18

    A method is described for separating U/sup 233/ from thorium and fission products. The separation is effected by forming a thorium-nitric acid solution of about 3 pH, adding hydrogen peroxide to precipitate uranium and thorium peroxide, treating the peroxides with sodium hydroxide to selectively precipitate the uranium peroxide, and reacting the separated solution with nitric acid to re- precipitate the uranium peroxide.

  17. Landscape control of uranium and thorium in boreal streams - spatiotemporal variability and the role of wetlands

    NASA Astrophysics Data System (ADS)

    Lidman, F.; Mörth, C. M.; Laudon, H.

    2012-11-01

    The concentrations of uranium and thorium in ten partly nested streams in the boreal forest region were monitored over a two-year period. The investigated catchments ranged from small headwaters (0.1 km2) up to a fourth-order stream (67 km2). Considerable spatiotemporal variations were observed, with little or no correlation between streams. The fluxes of both uranium and thorium varied substantially between the subcatchments, ranging from 1.7 to 30 g km-2 a-1 for uranium and from 3.2 to 24 g km-2 a-1 for thorium. Airborne gamma spectrometry was used to measure the concentrations of uranium and thorium in surface soils throughout the catchment, suggesting that the concentrations of uranium and thorium in mineral soils are similar throughout the catchment. The fluxes of uranium and thorium were compared to a wide range of parameters characterising the investigated catchments and the chemistry of the stream water, e.g. soil concentrations of these elements, pH, TOC (total organic carbon), Al, Si and hydrogen carbonate, but it was concluded that the spatial variabilities in the fluxes of both uranium and thorium mainly were controlled by wetlands. The results indicate that there is a predictable and systematic accumulation of both uranium and thorium in boreal wetlands that is large enough to control the transport of these elements. On the landscape scale approximately 65-80% of uranium and 55-65% of thorium entering a wetland were estimated to be retained in the peat. Overall, accumulation in mires and other types of wetlands was estimated to decrease the fluxes of uranium and thorium from the boreal forest landscape by 30-40%, indicating that wetlands play an important role for the biogeochemical cycling of uranium and thorium in the boreal forest landscape. The atmospheric deposition of uranium and thorium was also quantified, and its contribution to boreal streams was found to be low compared to weathering.

  18. Landscape control of uranium and thorium in boreal streams - spatiotemporal variability and the role of wetlands

    NASA Astrophysics Data System (ADS)

    Lidman, F.; Mörth, C. M.; Laudon, H.

    2012-03-01

    The concentrations of uranium and thorium in ten partly nested streams in the boreal forest region were monitored over a two-year period. Considerable spatiotemporal variations were observed, with little or no correlation between streams. The export of both uranium and thorium varied substantially between the subcatchments, ranging from 1.7 to 30 g km-2 a-1 for uranium and from 3.2 to 24 g km-2 a-1 for thorium. Airborne gamma spectrometry was used to measure the concentrations of uranium and thorium in surface soils throughout the catchment, but could not explain the variability in the export. Instead, the extent of lakes and mires within each subcatchment was found to be a stronger predictor for the transport of uranium and thorium. The results indicate that there is a predictable and systematic accumulation of both uranium and thorium in boreal mires. Approximately 65-80 % of uranium and 55-65 % of thorium entering a mire is estimated to be retained in the peat. Overall, accumulation in mires and other types of wetlands is estimated to decrease the fluxes of uranium and thorium from the boreal forest landscape by 30-40 %. The atmospheric deposition of uranium and thorium was also quantified and its contribution to boreal streams was found to be low compared to weathering.

  19. 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.

  20. SOLVENT EXTRACTION PROCESS FOR THE SEPARATION OF URANIUM AND THORIUM FROM PROTACTINIUM AND FISSION PRODUCTS

    DOEpatents

    Rainey, R.H.; Moore, J.G.

    1962-08-14

    A liquid-liquid extraction process was developed for recovering thorium and uranium values from a neutron irradiated thorium composition. They are separated from a solvent extraction system comprising a first end extraction stage for introducing an aqueous feed containing thorium and uranium into the system consisting of a plurality of intermediate extractiorr stages and a second end extractron stage for introducing an aqueous immiscible selective organic solvent for thorium and uranium in countercurrent contact therein with the aqueous feed. A nitrate iondeficient aqueous feed solution containing thorium and uranium was introduced into the first end extraction stage in countercurrent contact with the organic solvent entering the system from the second end extraction stage while intro ducing an aqueous solution of salting nitric acid into any one of the intermediate extraction stages of the system. The resultant thorium and uranium-laden organic solvent was removed at a point preceding the first end extraction stage of the system. (AEC)

  1. Thorium and uranium diphosphonates: Syntheses, structures, and spectroscopic properties

    SciTech Connect

    Adelani, Pius O.; Albrecht-Schmitt, Thomas E.

    2012-08-15

    Four new thorium and uranium diphosphonate compounds, [H{sub 3}O]{l_brace}Th{sub 2}[C{sub 6}H{sub 4}(PO{sub 3}){sub 2}]{sub 2}F{r_brace} (Thbbp-1), An{sub 2}{l_brace}(O{sub 3}PC{sub 6}H{sub 4}PO{sub 3}H){sub 2}[C{sub 6}H{sub 4}(PO{sub 3}H){sub 2}]{r_brace} [An=Th(IV), U(IV)] (Thbbp-2)/(U4bbp), and [(C{sub 2}H{sub 5})(CH{sub 3}){sub 3}N][(UO{sub 2}){sub 3}(O{sub 3}PC{sub 6}H{sub 4}PO{sub 3}H){sub 2}F(H{sub 2}O)] (U6bbp) have been synthesized hydrothermally using 1,4-benzenebisphosphonic acid as ligand. The crystal structures of these compounds were determined by single crystal X-ray diffraction. Thbbp-1 and Thbbp-2 contain seven-coordinate Th(IV) within ThO{sub 6}F and ThO{sub 7} units with capped trigonal prismatic and capped octahedral geometries, respectively. U4bbp is isotypic with Thbbp-2. The structure of U6bbp contains U(VI) is the common seven-coordinate pentagonal bipyramid. - Graphical abstract: Coordination polyhedra and luminescence properties in thorium and uranium compounds. Highlights: Black-Right-Pointing-Pointer Three-dimensional thorium and uranium complexes. Black-Right-Pointing-Pointer Conversion of U(VI) to U(IV) under hydrothermal condition. Black-Right-Pointing-Pointer Unusual seven-coordinate thorium complexes exhibiting capped octahedral and capped trigonal prismatic geometries.

  2. Uranium and thorium distribution in soils and weathered bedrock in south Texas

    USGS Publications Warehouse

    Dickinson, Kendell A.

    1977-01-01

    The distribution of uranium and thorium in soils and weathered bedrock in areas of calich soil development on various kinds of sedimentary bedrock in south Texas indicates that uranium and thorium are leached from the surface layers and deposited deeper in the soil or weathered bedrock. The data provide field evidence that uranium is mobilized during dry-climate weathering, and suggest that caution be used in the interpretation of airborne, radioactive surveys that measure uranium at the surface.

  3. METHOD OF PREPARING URANIUM, THORIUM, OR PLUTONIUM OXIDES IN LIQUID BISMUTH

    DOEpatents

    Davidson, J.K.; Robb, W.L.; Salmon, O.N.

    1960-11-22

    A method is given for forming compositions, as well as the compositions themselves, employing uranium hydride in a liquid bismuth composition to increase the solubility of uranium, plutonium and thorium oxides in the liquid bismuth. The finely divided oxide of uranium, plutonium. or thorium is mixed with the liquid bismuth and uranium hydride, the hydride being present in an amount equal to about 3 at. %, heated to about 5OO deg C, agitated and thereafter cooled and excess resultant hydrogen removed therefrom.

  4. Quantification of thorium and uranium sorption to contaminated sediments

    SciTech Connect

    Kaplan, D.I.

    2000-08-01

    Desorption tests using a sequential extraction method were used to characterize and quantify thorium and uranium sorption to contaminated wetland sediments collected from the Savannah River Site located in South Carolina. In situ distribution coefficients, or Kd values (Kd equal to Csolid/Cliquid), were determined. A problem associated with determining desorption Kd values is that it is difficult to identify Csolid, because by definition it must comprise only the fraction that is reversibly (and linearly) sorbed. A series of selective and sequential extractions was used to determine desorption Kd values. Thorium Kd values ranged from 115 to 2255 mL/g. Uranium Kd values ranged from 170 to 6493 mL/g. Compared to sorption Kd values, these desorption Kd values were appreciably greater because they captured the ``aging'' process of the radionuclides with the sediment, making the radionuclide more refractory. Compared to nonsite-specific data, these in situ Kd values improved accuracy, were more defensible, reduced uncertainty, and removed unnecessary conservatism for subsequent transport and risk calculations. Additional tests were conducted to provide geochemical information relevant for selecting appropriate remediation technologies for the contaminated site. Thorium and U were associated with labile fractions and were not concentrated with the smaller sediment particles. These findings suggest that phytoremediation or heap leaching, and not soil washing, are viable remediation approaches for this site.

  5. Comparison of thorium(IV) and uranium(VI) carboxyphosphonates.

    PubMed

    Adelani, Pius O; Albrecht-Schmitt, Thomas E

    2010-06-21

    The hydrothermal reactions of thorium nitrate and uranyl acetate with carboxyphenylphosphonic acid and HF result in the formation of ThF(2)(PO(3)C(6)H(4)CO(2)H) and UO(2)(PO(3)HC(6)H(4)CO(2)H)(2).2H(2)O, respectively. ThF(2)(PO(3)C(6)H(4)CO(2)H) adopts a pillared structure constructed from thorium oxyfluoride layers built from [ThO(4)F(4)] units that are bridged by carboxyphenylphosphonate to yield a three-dimensional network. UO(2)(PO(3)HC(6)H(4)CO(2)H)(2).2H(2)O forms one-dimensional chains of UO(6) tetragonal bipyramids that are bridged by the phosphonate moiety of the ligand. The carboxylate portion of the structure links the chains together into layers via a hydrogen-bonding network. The higher effective charge and more isotropic coordination of the Th(IV) centers versus the uranium centers contained within uranyl cations allow for coordination by the protonated carboxylate portions of the ligands to the thorium cations, which does not occur with uranium in carboxyphosphonates. UO(2)(PO(3)HC(6)H(4)CO(2)H)(2).2H(2)O displays vibronically coupled fluorescence and the potential for energy transfer from the ligand to the charge-transfer bands of the uranyl cations. The main fluorescence by the ligand is quenched in ThF(2)(PO(3)C(6)H(4)CO(2)H).

  6. 78 FR 21352 - Update on Reimbursement for Costs of Remedial Action at Active Uranium and Thorium Processing Sites

    Federal Register 2010, 2011, 2012, 2013, 2014

    2013-04-10

    ... on Reimbursement for Costs of Remedial Action at Active Uranium and Thorium Processing Sites AGENCY... reimbursement for cleanup work performed by licensees at eligible uranium and thorium processing sites in... licensees of eligible uranium and thorium processing sites. If licensees submit claims in FY 2013,...

  7. Primary oxidation variation and distribution of uranium and thorium in a lava flow.

    PubMed

    Watkins, N D; Holmes, C W; Haggerty, S E

    1967-02-03

    An Icelandic basalt lava flow has a systematic oxidation variation, formed during the initial cooling, with a resultant maximum oxidation just below the center of the lava. The ratio of thorium to uranium shows a clear dependence on this primary oxidation variation. Between-lava comparisons of thorium and uranium may be critically dependent on the position of the samples in each lava.

  8. Uranium and thorium content in long-tailed ducks (Clangula hyemalis L.).

    PubMed

    Szefer, P; Falandysz, J

    1983-08-01

    Concentrations of uranium and thorium have been determined in liver, breast muscle, leg muscle, stomach and heart of long-tailed ducks wintering in Gdańsk Bay during 1980-81. The highest concentration of uranium and thorium was found in stomach, and the lowest in breast muscle.

  9. Uranium and thorium sequestration by a Pseudomonas sp.: mechanism and chemical characterization.

    PubMed

    Kazy, Sufia K; D'Souza, S F; Sar, Pinaki

    2009-04-15

    The mechanism and chemical nature of uranium and thorium sequestration by a Pseudomonas strain was investigated by transmission electron microscopy, energy dispersive X-ray (EDX) analysis, FTIR spectroscopy and X-ray diffractometry. Atomic force microscopy (AFM) used in the tapping mode elucidated the morphological changes in bacterial cells following uranium and thorium binding. Transmission electron microscopy revealed intracellular sequestration of uranium and thorium throughout the cell cytoplasm with electron dense microprecipitations of accumulated metals. Energy dispersive X-ray analysis confirmed the cellular deposition of uranium and thorium. EDX and elemental analysis of sorption solution indicated the binding of uranium and thorium by the bacterial biomass via displacement of cellular potassium and calcium. The strong involvement of cellular phosphate, carboxyl and amide groups in radionuclide binding was ascertained by FTIR spectroscopy. X-ray powder diffraction (XRD) analyses confirmed cellular sequestration of crystalline uranium and thorium phosphates. Overall results indicate that a combined ion-exchange-complexation-microprecipitation mechanism could be involved in uranium and thorium sequestration by this bacterium. Atomic force microscopy and topography analysis revealed an undamaged cell surface with an increase in cell length, width and height following radionuclide accumulation. The arithmetic average roughness (R(a)) and root mean square (RMS) roughness (R(q)) values indicated an increase in surface roughness following uranium and thorium sequestration.

  10. Uranium-thorium-lead isotope relations in lunar materials.

    PubMed

    Silver, L T

    1970-01-30

    The lead isotopic compositions and uranium, thorium, and lead concentrations have been measured on six samples of material from the Sea of Tranquillity. The leads are moderately to very radiogenic; the initial lead concentrations are very low; the uranium and thorium levels are 0.26 to 0.88 and 0.87 to 3.35 parts per million, respectively. The Th/U ratios cluster about a 3.6 value. Apparent ages calculated for four rocks are 4.1 to 4.2 x 10(9) years. Dust and breccia yield apparent ages of 4.60 to 4.63 x 10(9) years. The uranium-lead ages are concordant, or nearly so, in all cases. The lunar surface is an ancient region with an extended record of events in the early history of the solar system. discrepancy between the rock ages and dust ages poses a fundamental qusestion about rock genesis on the moon.

  11. Interim report on studies of uranium, thorium, and lead migration at Key Lake, Saskatchewan, Canada

    SciTech Connect

    Curtis, D.B.; Gancarz, A.J.

    1980-07-01

    The redistribution of uranium, thorium, and lead is being examined in samples representing several million cubic meters of sandstone and metamorphased sediments in the Athabasca Basin which is located in the northwest corner of the Canadian province of Saskatchewan. The region of study includes zones of uranium mineralization at Key Lake. Mineralization occurs at the unconformity between the Athabasca sandstone and the underlying metasediments and in fault zones within the metasediments. Lead isotopes record a radiometric age of 1300 +- 150 m.y. in samples from above and below the unconformity. This age probably reflects the time of deposition of the sandstones and an associated redistribution of uranium and/or lead in the underlying rocks. Many of the samples have been fractionated with respect to radiogenic lead and the actinide parent elements since that time. Sandstones and altered rocks from the region above the unconformity have been a transport path and are a repository for lead. In contrast, mineralized rocks are deficient in radiogenic lead and must be an important source of lead in the local geologic environment. However, the isotopic composition of lead missing from the ores is different from that found in the overlying sandstones. The two types of rocks do not appear to represent complements with respect to a source and a repository for lead.

  12. Supercritical Fluid Extraction and Separation of Uranium from Other Actinides

    SciTech Connect

    Donna L. Quach; Bruce J. Mincher; Chien M. Wai

    2014-06-01

    This paper investigates the feasibility of separating uranium from other actinides by using supercritical fluid carbon dioxide (sc-CO2) as a solvent modified with tri-n-butylphosphate (TBP) for the development of an extraction and counter current stripping technique, which would be a more efficient and environmentally benign technology for used nuclear fuel reprocessing compared to traditional solvent extraction. Several actinides (U(VI), Np(VI), Pu(IV), and Am(III)) were extracted in sc-CO2 modified with TBP over a range of nitric acid concentrations and then the actinides were exposed to reducing and complexing agents to suppress their extractability. According to this study, the separation of uranium from plutonium in sc-CO2 modified with TBP was successful at nitric acid concentrations of less than 3 M in the presence of acetohydroxamic acid or oxalic acid, and the separation of uranium from neptunium was successful at nitric acid concentrations of less than 1 M in the presence of acetohydroxamic acid, oxalic acid, or sodium nitrite.

  13. Evaluation of in vitro dissolution rates of thorium in uranium mill tailings.

    PubMed

    Reif, R H

    1994-11-01

    Dissolution rates of thorium from the uranium mill tailings piles at two Department of Energy Uranium Mill Tailings Remedial Action Project (UMTRAP) sites have been evaluated. The thorium dissolution rates were evaluated in vitro using simulated lung fluid. The former uranium mills at the UMTRAP sites employed different chemical processes (acid leach and alkaline pressure leach) to extract the uranium from the ore, and the thorium dissolution rates at these sites were found to be markedly different. A site specific annual limit on intake (ALI) value for 230Th was calculated for the UMTRAP site that was associated with a multiple component dissolution curve.

  14. 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.

  15. Functional sorbents for selective capture of plutonium, americium, uranium, and thorium in blood.

    PubMed

    Yantasee, Wassana; Sangvanich, Thanapon; Creim, Jeffery A; Pattamakomsan, Kanda; Wiacek, Robert J; Fryxell, Glen E; Addleman, R Shane; Timchalk, Charles

    2010-09-01

    Self-assembled monolayer on mesoporous supports (SAMMS) are hybrid materials created from attachment of organic moieties onto very high surface area mesoporous silica. SAMMS with surface chemistries including three isomers of hydroxypyridinone, diphosphonic acid, acetamide phosphonic acid, glycinyl urea, and diethylenetriamine pentaacetate (DTPA) analog were evaluated for chelation of actinides ((239)Pu, (241)Am, uranium, thorium) from blood. Direct blood decorporation using sorbents does not have the toxicity or renal challenges associated with traditional chelation therapy and may have potential applications for critical exposure cases, reduction of nonspecific dose during actinide radiotherapy, and for sorbent hemoperfusion in renal insufficient patients, whose kidneys clear radionuclides at a very slow rate. Sorption affinity (K(d)), sorption rate, selectivity, and stability of SAMMS were measured in batch contact experiments. An isomer of hydroxypyridinone (3,4-HOPO) on SAMMS demonstrated the highest affinity for all four actinides from blood and plasma and greatly outperformed the DTPA analog on SAMMS and commercial resins. In batch contact, a fifty percent reduction of actinides in blood was achieved within minutes, and there was no evidence of protein fouling or material leaching in blood after 24 h. The engineered form of SAMMS (bead format) was further evaluated in a 100-fold scaled-down hemoperfusion device and showed no blood clotting after 2 h. A 0.2 g quantity of SAMMS could reduce 50 wt.% of 100 ppb uranium in 50 mL of plasma in 18 min and that of 500 dpm mL(-1) in 24 min. 3,4-HOPO-SAMMS has a long shelf-life in air and at room temperature for at least 8 y, indicating its feasibility for stockpiling in preparedness for an emergency. The excellent efficacy and stability of SAMMS materials in complex biological matrices suggest that SAMMS can also be used as orally administered drugs and for wound decontamination. By changing the organic groups of

  16. X-ray powder data for uranium and thorium minerals

    USGS Publications Warehouse

    Frondel, Clifford; Riska, Daphne; Frondel, Judith Weiss

    1956-01-01

    The U.S. Geological Survey has in preparation a comprehensive volume on the mineralogy of uranium and thorium. This work has been done as part of a continuing systematic survey of data on uranium and thorium minerals on behalf of the Division of Raw Materials, U.S. Atomic Energy Commission. Pending publication of this volume and in response to a widespread demand among workers in uranium and thorium mineralogy, the X-ray powder diffraction data for the known minerals that contain uranium or thorium as an essential constituent are presented here. The coverage is complete except for a few minerals for which there are no reliable data owing to lack of authentic specimens. With the exception of that for ianthinite, the new data either originated in the Geological Survey or in the Mineralogical Laboratory of Harvard University. Data from the literature or other sources were cross-checked against the files of standard patterns of these laboratories; the sources are indicated in the references. Data not accompanied by a reference were obtained from films in the Harvard Standard File and cross-checked as to the identity of the film with the Geological Survey's file. Minor differences can be expected in the d-spacings reported for the same specimens by different investigators because of the manner of preparation of the mount, the conditions of X-ray irradiation, and the method of photography and measurement of the film or chart. The Harvard and Geological Survey data all were obtained from films taken in 114-mm diameter cameras, using either ethyl cellulose and toluene or collodion spindle mounts and Straumanis-type film mounting. Unless otherwise indicated all patterns were taken with copper radiation (Kα 1.5418 A.) and nickel filter and data are given in Angstrom units. The d-spacings are not corrected for film shrinkage. The correction ordinarily is small and in general is less than either the variation in spacing arising from differences in experimental technique of

  17. Biomonitoring of environmental pollution by thorium and uranium in selected regions of the Republic of Kazakhstan.

    PubMed

    Zoriy, P; Ostapczuk, P; Dederichs, H; Höbig, J; Lennartz, R; Zoriy, M

    2010-05-01

    Two former uranium mines and a uranium reprocessing factory in the city of Aktau, Kazakhstan, may represent a risk of contaminating the surrounding areas by uranium and its daughter elements. One of the possible fingerprinting tools for studying the environmental contamination is using plant samples, collected in the surroundings of this city in 2007 and 2008. The distribution pattern of environmental pollution by uranium and thorium was evaluated by determining the thorium and uranium concentrations in plant samples (Artemisia austriaca) from the city of Aktau and comparing these results with those obtained for the same species of plants from an unpolluted area (town of Kurchatov). The determination of the uranium and thorium concentrations in different parts of A. austriaca plants collected from the analyzed areas demonstrated that the main contamination of the flora in areas surrounding the city of Aktau was due to dust transported by the wind from the uranium mines. The results obtained demonstrate that all the areas surrounding Aktau have a higher pollution level due to thorium and uranium than the control area (Kurchatov). A few "hot points" with high concentrations of uranium and thorium were found near the uranium reprocessing factory and the uranium mines.

  18. Reconnaissance for uranium and thorium in Alaska, 1954

    USGS Publications Warehouse

    Matzko, John J.; Bates, Robert G.

    1957-01-01

    During 1954 reconnaissance investigations to locate minable deposits of uranium and thorium in Alaska were unsuccessful. Areas examined, from which prospectors had submitted radioactive samples, include Cap Yakataga, Kodiak Island, and Shirley Lake. Unconcentrated gravels from the beach at Cape Yakataga average about 0.001 percent equivalent uranium. Uranothorianite has been identified by X-ray diffraction data and is the principal source of radioactivity in the Cape Yakataga beach sands studied; but the zircon, monazite, and uranothorite are also radioactive. The black, opaque uranothorianite generally occurs as minute euhedral cubs, the majority of which will pass through a 100-mesh screen. The bedrock source of the radioactive samples from Kodiak Island was not found; the maximum radioactivity of samples from the Shirley Lake area was equivalent to about 0.02 percent uranium. Radiometric traverses of the 460-foot level of the Garnet shaft of the Nixon Fork mine in the Nixon Fork mining district indicated a maximum of 0.15 mr/hr. In the Hot Springs district, drill hole concentrates of gravels examined contained a maximum of 0.03 percent equivalent uranium. A radioactivity anomaly noted during the Survey's airborne reconnaissance of portions of the Territory during 1954 is located in the Fairhaven district. A ground check disclosed that the radioactivity was due to accessory minerals in the granitic rock.

  19. 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

  20. Systematic studies of early actinide complexes: thorium(IV) fluoroketimides.

    PubMed

    Schelter, Eric J; Yang, Ping; Scott, Brian L; Re, Ryan E Da; Jantunen, Kimberly C; Martin, Richard L; Hay, P Jeffrey; Morris, David E; Kiplinger, Jaqueline L

    2007-04-25

    Reaction of (C5Me5)2Th(CH3)2 with 2 equiv of NC-ArF gives the corresponding fluorinated thorium(IV) bis(ketimide) complexes (C5Me5)2Th[-N=C(CH3)(ArF)]2 (where ArF = 3-F-C6H4 (4), 4-F-C6H4 (5), 2-F-C6H4 (6), 3,5-F2-C6H3 (7), 3,4,5-F3-C6H2 (8), 2,6-F2-C6H3 (9), 2,4,6-F3-C6H2 (10), and C6F5 (11)). The complexes have been characterized by a combination of single-crystal X-ray diffraction, cyclic voltammetry and NMR, and UV-visible absorption and low-temperature luminescence spectroscopies. Density functional theory (DFT) and time-dependent DFT (TD-DFT) results are reported for complexes 5, 11, and (C5Me5)2Th[-N=C(Ph)2]2 (1) for comparison with experimental data and to guide in the interpretation of the spectroscopic results. The most significant structural perturbation imparted by the fluorine substitution in these complexes is a rotation of the fluorophenyl group (ArF) out of the plane defined by the N=C(CMe)(Cipso) fragment in complexes 9-11 when the ArF group possesses two ortho fluorine atoms. Excellent agreement is obtained between the optimized ground state DFT calculated structures and crystal structures for 11, which displays the distortion, as well as 5, which does not. In complexes 9-11, the out-of-plane rotation results in large interplanar angles (phi) between the planes formed by ketimide atoms N=C(CMe)(Cipso) and the ketimide aryl groups in the range phi = 49.1-88.8 degrees , while in complexes 5, 7, and 8, phi = 5.7-34.9 degrees . The large distortions in 9-11 are a consequence of an unfavorable steric interaction between one of the two ortho fluorine atoms and the methyl group [-N=C(CH3)] on the ketimide ligand. Excellent agreement is also observed between the experimental electronic spectroscopic data and the TD-DFT predictions that the two lowest lying singlet states are principally of nonbonding nitrogen p orbital to antibonding C=N pi* orbital (pN-->pi*C=N or npi*) character, giving rise to moderately intense transitions in the mid-visible spectral

  1. Actinide(IV) Deposits on Bone: Potential Role of the Osteopontin-Thorium Complex.

    PubMed

    Creff, Gaëlle; Safi, Samir; Roques, Jérôme; Michel, Hervé; Jeanson, Aurélie; Solari, Pier-Lorenzo; Basset, Christian; Simoni, Eric; Vidaud, Claude; Den Auwer, Christophe

    2016-01-04

    In case of a nuclear event, contamination (broad or limited) of the population or of specific workers might occur. In such a senario, the fate of actinide contaminants may be of first concern, in particular with regard to human target organs like the skeleton. To improve our understanding of the toxicological processes that might take place, a mechanistic approach is necessary. For instance, ∼50% of Pu(IV) is known from biokinetic data to accumulate in bone, but the underlining mechanisms are almost unknown. In this context, and to obtain a better description of the toxicological mechanisms associated with actinides(IV), we have undertaken the investigation, on a molecular scale, of the interaction of thorium(IV) with osteopontin (OPN) a hyperphosphorylated protein involved in bone turnover. Thorium is taken here as a simple model for actinide(IV) chemistry. In addition, we have selected a phosphorylated hexapeptide (His-pSer-Asp-Glu-pSer-Asp-Glu-Val) that is representative of the peptidic sequence involved in the bone interaction. For both the protein and the biomimetic peptide, we have determined the local environment of Th(IV) within the bioactinidic complex, combining isothermal titration calorimetry, attenuated total reflectance Fourier transform infrared spectroscopy, theoretical calculations with density functional theory, and extended X-ray absorption fine structure spectroscopy at the Th LIII edge. The results demonstrate a predominance of interaction of metal with the phosphate groups and confirmed the previous physiological studies that have highlighted a high affinity of Th(IV) for the bone matrix. Data are further compared with those of the uranyl case, representing the actinyl(V) and actinyl(VI) species. Last, our approach shows the importance of developing simplified systems [Th(IV)-peptide] that can serve as models for more biologically relevant systems.

  2. The distribution of uranium and thorium in samples taken from different polluted marine environment.

    PubMed

    Akyil, S; Yusof, A M

    2007-06-01

    Concentrations of uranium and thorium in seawater, sediment and some marine species taken from along the coastal areas of Malaysia were determined spectrophotometrically. The uranium and thorium concentrations in seawater were found to vary ranging from 1.80 to 4.1 and 0.14 to 0.88 microg/L, respectively. The concentration of uranium in sediment samples was reported to range from 3.00 to 6.60 microg/g while those of thorium were slightly lower ranging from 0.01 to 0.68 microg/g. The uptake of uranium and thorium in marine species was found to be rather low. Similar variations in total alpha activities in samples were also observed with the total alpha activities relatively lower than the beta activities in most samples.

  3. Uranium-series dating of actinide decay series mobility at Pena Blanca

    SciTech Connect

    Dixon, P.R.; Goldstein, S.J.; Murrell, M.T.

    1997-12-31

    Studies of U-series disequilibria near uranium ore deposits can provide valuable information on the mobility of actinides and their daughters over the range of timescales needed to assess the stability of proposed waste repositories. We have applied highly sensitive TIMS methods to obtain 238U-234U-230Th dates for three whole rock samples within a {approximately}30 in long fracture emanating into surrounding tuff from the deposit at Pena Blanca, Mexico. The 238U-234U-230Th data lie on a whole-rock isochron that requires closed-system behavior for the last 380 ka. Preliminary 231Pa-235U data for the U-rich vein also indicates closed system behavior for at least the last 100 ka. In contrast, 226Ra/230Th activity ratios range from 0.76-0.99 which indicates more recent Ra mobility within the fracture most likely due to surface water infiltration. Our results require uranium, thorium and protactinium stability despite recent radium mobility and provide important constraints on repository stability over {approximately}100 ka timescales.

  4. Stability of dilute solutions of uranium, lead, and thorium ions

    USGS Publications Warehouse

    Milkey, R.G.

    1954-01-01

    Standard solutions and samples containing a few micrograms of metallic ions per milliliter are frequently used in determination of trace elements. It is important to know whether the concentrations of such solutions remain constant from day to day. The stability of dilute solutions of three metallic ions-uranium, lead, and thorium-has been investigated. Solutions containing concentrations of metallic ions, ranging from 1000 to 0.1 ?? per milliliter, were allowed to stand for approximately 2.5 months, and then the metallic ion content of those solutions that had lost strength was determined. Both adsorption and hydrolysis variously influenced the solute loss, but the minimum pH at which loss of concentration of lead and uranium occurred seemed to coincide with the pH at which the hydrolyzed metal ions began to precipitate. No increase in the stability of the solutions was obtained by substituting polyethylene containers for borosilicate glass. The solutions that lost strength could not be restored promptly to the original concentration by manual means, such as shaking them vigorously for several minutes.

  5. Global Uranium And Thorium Resources: Are They Adequate To Satisfy Demand Over The Next Half Century?

    NASA Astrophysics Data System (ADS)

    Lambert, I. B.

    2012-04-01

    This presentation will consider the adequacy of global uranium and thorium resources to meet realistic nuclear power demand scenarios over the next half century. It is presented on behalf of, and based on evaluations by, the Uranium Group - a joint initiative of the OECD Nuclear Energy Agency and the International Atomic Energy Agency, of which the author is a Vice Chair. The Uranium Group produces a biennial report on Uranium Resources, Production and Demand based on information from some 40 countries involved in the nuclear fuel cycle, which also briefly reviews thorium resources. Uranium: In 2008, world production of uranium amounted to almost 44,000 tonnes (tU). This supplied approximately three-quarters of world reactor requirements (approx. 59,000 tU), the remainder being met by previously mined uranium (so-called secondary sources). Information on availability of secondary sources - which include uranium from excess inventories, dismantling nuclear warheads, tails and spent fuel reprocessing - is incomplete, but such sources are expected to decrease in market importance after 2013. In 2008, the total world Reasonably Assured plus Inferred Resources of uranium (recoverable at less than 130/kgU) amounted to 5.4 million tonnes. In addition, it is clear that there are vast amounts of uranium recoverable at higher costs in known deposits, plus many as yet undiscovered deposits. The Uranium Group has concluded that the uranium resource base is more than adequate to meet projected high-case requirements for nuclear power for at least half a century. This conclusion does not assume increasing replacement of uranium by fuels from reprocessing current reactor wastes, or by thorium, nor greater reactor efficiencies, which are likely to ameliorate future uranium demand. However, progressively increasing quantities of uranium will need to be mined, against a backdrop of the relatively small number of producing facilities around the world, geopolitical uncertainties and

  6. Characterization of thorium and uranium contaminated soil from a nuclear fuel facility

    SciTech Connect

    Brown, N.R.; Buck, E.C.; Dietz, N.L.; Bates, J.K.; Carlson, B.

    1994-02-01

    This paper describes the utility of soil characterization using electron microscopy to support decontamination efforts of contaminated soil. Soil contaminated with thorium and uranium from the grounds of a nuclear fuel manufacturing facility was subjected to remediation efforts. A light acid leach was able to remove only 30% of the thorium suggesting that the thorium was present in two or more forms. Analytical electron microscopy determined that all of the thorium was present as ThO{sub 2}, but in a bimodal size distribution and occasionally closely associated with other minerals. Electron microscopy was useful in understanding the remediation data and demonstrates the need for characterization of contaminated soils.

  7. Potential of Melastoma malabathricum as bio-accumulator for uranium and thorium from soil

    NASA Astrophysics Data System (ADS)

    Saat, Ahmad; Kamsani, Ain Shaqina; Kamri, Wan Nur Aina Nadzira; Talib, Nur Hasyimah Mat; Wood, Ab Khalik; Hamzah, Zaini

    2015-04-01

    Uranium and Thorium are naturally occuring radionuclides. However, due to anthropogenic activities in some locations their concentrations in the soils could be elevated. This study explores the potential of Melastoma malabathricum (locally known as `pokok senduduk') as bio-accumulator of uranium and thorium from soils of three different study areas, namely former tin mining, industrial and residential/commercial areas in Peninsular Malaysia. The study found elevated concentrations of uranium and thorium in former tin mining soils as compared to natural abundance. However in industral and residential/commercial areas the concentrations are within the range of natural abundance. In terms of transfer factor (TF), in ex-mining areas TF > 1 for uranium in the leaf, stem and roots, indicating accumulation of uranium from soil. However for thorium TF < 1, indicating the occurence of transfer from soil to root, stem and leaf, but no accumulation. For other areas only transfer of uranium and thorium were observed. The results indicated the potential of Melastoma malabathricum to be used as bio-accumulatior of uranium, especially in areas of elevated concentration.

  8. Potential of Melastoma malabathricum as bio-accumulator for uranium and thorium from soil

    SciTech Connect

    Saat, Ahmad; Kamsani, Ain Shaqina; Kamri, Wan Nur Aina Nadzira; Talib, Nur Hasyimah Mat; Wood, Ab Khalik; Hamzah, Zaini

    2015-04-29

    Uranium and Thorium are naturally occuring radionuclides. However, due to anthropogenic activities in some locations their concentrations in the soils could be elevated. This study explores the potential of Melastoma malabathricum (locally known as ‘pokok senduduk’) as bio-accumulator of uranium and thorium from soils of three different study areas, namely former tin mining, industrial and residential/commercial areas in Peninsular Malaysia. The study found elevated concentrations of uranium and thorium in former tin mining soils as compared to natural abundance. However in industral and residential/commercial areas the concentrations are within the range of natural abundance. In terms of transfer factor (TF), in ex-mining areas TF > 1 for uranium in the leaf, stem and roots, indicating accumulation of uranium from soil. However for thorium TF < 1, indicating the occurence of transfer from soil to root, stem and leaf, but no accumulation. For other areas only transfer of uranium and thorium were observed. The results indicated the potential of Melastoma malabathricum to be used as bio-accumulatior of uranium, especially in areas of elevated concentration.

  9. Application of extraction chromatography to the separation of thorium and uranium dissolved in a solution of high salt concentration.

    PubMed

    Fujiwara, Asako; Kameo, Yutaka; Hoshi, Akiko; Haraga, Tomoko; Nakashima, Mikio

    2007-01-26

    Extraction chromatography with commercially available UTEVA resin (for uranium and tetravalent actinide) was applied for the separation of Th and U from control solutions prepared from a multi-element control solution and from sample solutions of solidified simulated waste. Thorium and U in control solutions with 1-5mol/dm(3) HNO(3) were extracted with UTEVA resin and recovered with a solution containing 0.1mol/dm(3) HNO(3) and 0.05mol/dm(3) oxalic acid to be separated from the other metallic elements. Extraction behavior of U in the sample solutions was similar to that in the control solutions, but extraction of Th was dependent on the concentration of HNO(3). Thorium was extracted from 5mol/dm(3) HNO(3) sample solutions but not from 1mol/dm(3) HNO(3) sample solutions. We conjecture that thorium fluoride formation interferes with extraction of Th. Addition of Al(NO(3))(3) and Fe(NO(3))(3), which have higher stability constant with fluoride ion than Th, does improve extractability of Th from 1mol/dm(3) HNO(3) sample solution.

  10. Sequential isotopic determination of plutonium, thorium, americium, strontium and uranium in environmental and bioassay samples.

    PubMed

    Wang, Jeng-Jong; Chen, Ing-Jane; Chiu, Jih-Hung

    2004-01-01

    A procedure has been developed to provide sequential analysis of 238Pu, 230Th, 241Am, 238U, and 90Sr in environmental and bioassay samples. Tracers and/or carriers (242Pu, 243Am, 232U, and stable strontium) are added into the sample as chemical yield monitors, and then, plutonium, thorium, strontium, americium, and uranium are sequentially separated and purified by Dowex ion-exchange resin, EiChroM Sr-resin, EiChroM TRU-resin, and Chelate-100 resin, respectively. The radioactivities of 90Sr and the actinides are measured using the liquid scintillation counter and alpha-particle spectrometer, respectively. Acidified water, glass-fiber air filter, soil, synthetic urine and synthetic feces samples of US National Institute of Standard and Technology Radiochemical Intercomparison Program(NRIP) were analyzed to verify this method. All the analytical results of 238Pu, 230Th, 90Sr, 241Am and 238U meet the traceability limit per ANSI N42.22, and when appropriate, evaluation of radiobioassay measurement bias and precision per ANSI N13.30.

  11. Comparative analysis of thorium and uranium fuel for transuranic recycle in a sodium cooled Fast Reactor

    SciTech Connect

    C. Fiorina; N. E. Stauff; F. Franceschini; M. T. Wenner; A. Stanculescu; T. K. Kim; A. Cammi; M. E. Ricotti; R. N. Hill; T. A. Taiwo; M. Salvatores

    2013-12-01

    The present paper compares the reactor physics and transmutation performance of sodium-cooled Fast Reactors (FRs) for TRansUranic (TRU) burning with thorium (Th) or uranium (U) as fertile materials. The 1000 MWt Toshiba-Westinghouse Advanced Recycling Reactor (ARR) conceptual core has been used as benchmark for the comparison. Both burner and breakeven configurations sustained or started with a TRU supply, and assuming full actinide homogeneous recycle strategy, have been developed. State-of-the-art core physics tools have been employed to establish fuel inventory and reactor physics performances for equilibrium and transition cycles. Results show that Th fosters large improvements in the reactivity coefficients associated with coolant expansion and voiding, which enhances safety margins and, for a burner design, can be traded for maximizing the TRU burning rate. A trade-off of Th compared to U is the significantly larger fuel inventory required to achieve a breakeven design, which entails additional blankets at the detriment of core compactness as well as fuel manufacturing and separation requirements. The gamma field generated by the progeny of U-232 in the U bred from Th challenges fuel handling and manufacturing, but in case of full recycle, the high contents of Am and Cm in the transmutation fuel impose remote fuel operations regardless of the presence of U-232.

  12. Elemental bio-imaging of thorium, uranium, and plutonium in tissues from occupationally exposed former nuclear workers.

    PubMed

    Hare, Dominic; Tolmachev, Sergei; James, Anthony; Bishop, David; Austin, Christine; Fryer, Fred; Doble, Philip

    2010-04-15

    Internal exposure from naturally occurring radionuclides (including the inhaled long-lived actinides (232)Th and (238)U) is a component of the ubiquitous background radiation dose (National Council on Radiation Protection and Measurements. Ionizing radiation exposure of the population of the United States; NCRP Report No. 160; NCRP: Bethesda, MD, 2009). It is of interest to compare the concentration distribution of these natural alpha-emitters in the lungs and respiratory lymph nodes with those resulting from occupational exposure, including exposure to anthropogenic plutonium and depleted and enriched uranium. This study examines the application of laser ablation-inductively coupled plasma-mass spectrometry (LA-ICPMS) to quantifying and visualizing the mass distribution of uranium and thorium isotopes from both occupational and natural background exposure in human respiratory tissues and, for the first time, extends this application to the direct imaging of plutonium isotopes. Sections of lymphatic and lung tissues taken from deceased former nuclear workers with a known history of occupational exposure to specific actinide elements (uranium, plutonium, or americium) were analyzed by LA-ICPMS. Using a previously developed LA-ICPMS protocol for elemental bio-imaging of trace elements in human tissue and a new software tool, we generated images of thorium ((232)Th), uranium ((235)U and (238)U), and plutonium ((239)Pu and (240)Pu) mass distributions in sections of tissue. We used a laboratory-produced matrix-matched standard to quantify the (232)Th, (235)U, and (238)U concentrations. The plutonium isotopes (239)Pu and (240)Pu were detected by LA-ICPMS in 65 mum diameter localized regions of both a paratracheal lymph node and a sample of lung tissue from a person who was occupationally exposed to refractory plutonium (plutonium dioxide). The average (overall) (239)Pu concentration in the lymph node was 39.2 ng/g, measured by high purity germanium (HPGe) gamma

  13. 10 CFR 40.28 - General license for custody and long-term care of uranium or thorium byproduct materials disposal...

    Code of Federal Regulations, 2010 CFR

    2010-01-01

    ... or thorium byproduct materials disposal sites. 40.28 Section 40.28 Energy NUCLEAR REGULATORY... long-term care of uranium or thorium byproduct materials disposal sites. (a) A general license is... in this part for uranium or thorium mill tailings sites closed under title II of the Uranium...

  14. 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.

  15. A density functional theory study of uranium-doped thoria and uranium adatoms on the major surfaces of thorium dioxide

    NASA Astrophysics Data System (ADS)

    Shields, Ashley E.; Santos-Carballal, David; de Leeuw, Nora H.

    2016-05-01

    Thorium dioxide is of significant research interest for its use as a nuclear fuel, particularly as part of mixed oxide fuels. We present the results of a density functional theory (DFT) study of uranium-substituted thorium dioxide, where we found that increasing levels of uranium substitution increases the covalent nature of the bonding in the bulk ThO2 crystal. Three low Miller index surfaces have been simulated and we propose the Wulff morphology for a ThO2 particle and STM images for the (100), (110), and (111) surfaces studied in this work. We have also calculated the adsorption of a uranium atom and the U adatom is found to absorb strongly on all three surfaces, with particular preference for the less stable (100) and (110) surfaces, thus providing a route to the incorporation of uranium into a growing thoria particle.

  16. Environmental consequences of uranium atmospheric releases from fuel cycle facility: II. The atmospheric deposition of uranium and thorium on plants.

    PubMed

    Pourcelot, L; Masson, O; Renaud, P; Cagnat, X; Boulet, B; Cariou, N; De Vismes-Ott, A

    2015-03-01

    Uranium and thorium isotopes were measured in cypress leaves, wheat grains and lettuce taken in the surroundings of the uranium conversion facility of Malvési (South of France). The comparison of activity levels and activity ratios (namely (238)U/(232)Th and (230)Th/(232)Th) in plants with those in aerosols taken at this site and plants taken far from it shows that aerosols emitted by the nuclear site (uranium releases in the atmosphere by stacks and (230)Th-rich particles emitted from artificial ponds collecting radioactive waste mud) accounts for the high activities recorded in the plant samples close to the site. The atmospheric deposition process onto the plants appears to be the dominant process in plant contamination. Dry deposition velocities of airborne uranium and thorium were measured as 4.6 × 10(-3) and 5.0 × 10(-3) m s(-1), respectively.

  17. Relativistic density functional study on uranium(IV) and thorium(IV) oxide clusters of zonohedral geometry.

    PubMed

    Shamov, Grigory A

    2012-06-18

    Free and ligated oxide clusters of thorium(IV) and uranium(IV) were studied with density functional theory using all-electron scalar relativistic method, as well as energy-consistent relativistic f-in-core pseudopotentials. The main driving force for the cluster formation is the sintering of the dioxoactinide moieties, which is more favorable for thorium(IV) than for uranium(IV) because, for the latter, a penalty for bending of the uranyl(IV) is to be paid. We assumed that the rhombic structural motif that exists already in the (AnO(2))(2) dimer could be a guide to explaining the preference for the existing An(6)O(8)-type clusters. On the basis of this, we have theoretically explored the possibility of the existence of similar (zonohedric) polyhedral actinide oxide clusters and found that the next possible cluster would be of An(12)O(20) stoicheometry. We have predicted by our DFT computations that the corresponding zonohedral clusters would be minima on the potential energy surface. The alternating An-O rhombic structural motif also offers a possible explanation of the existence and stoichiometry of the only nonfluorite cluster thus far, the An(12)O(20), which is nonzonohedral, nonconvex, but still a rhombic polyhedron. Our relativistic all electron DFT computations of both free cationic and ligated clusters predict that preparation of the larger clusters is not forbidden thermodynamically. We have also found that for the uranium(IV), oxide dimer and hexamer clusters are antiferromagnetic, broken spin singlet in their ground state, while ligated [U(6)O(8)] clusters prefer an all high-spin electronic configuration.

  18. Effects of solution pH and complexing reagents on uranium and thorium desorption under saturated equilibrium conditions

    SciTech Connect

    Wang, Yug-Yea; Yu, C.

    1992-08-01

    Three contaminated bulk surface soils were used for investigating the effect of solution pH and complexing reagents on uranium and thorium desorption. At a low solution pH, the major chemical species of uranium and thorium, uranyl UO{sub 2}{sup +2}, thorium dihydroxide Th(OH){sub 2}{sup +2}, and thorium hydroxide Th(OH){sup +3}, tend to form complexes with acetates in the solution phase, which increases the fractions of uranium and thorium desorbed into this phase. At a high solution pH, important uranium and thorium species such as uranyl tricarbonate complex UO{sub 2}(CO){sub 3}{sub 3}{sup {minus}4} and thorium tetrahydroxide complex Th(OH){sub 4} tend to resist complexation with acetates. The presence of complexing reagents in solution can release radionuclides such as uranium and/or thorium from the soil to the solution by forming soluble complexes. Sodium bicarbonate (NaHCO{sub 3}) and diethylenetriaminepentaacetic acid (DTPA) are strong complex formers that released 38% to 62% of total uranium activity and 78% to 86% of total thorium activity, respectively, from the soil samples investigated. Solutions of 0.1 molar sodium nitrate (NaNO{sub 3}) and 0.1 molar sodium sulfate (Na{sub 2}SO{sub 4}) were not effective complex formers with uranium and thorium under the experimental conditions. Fractions of uranium and thorium desorbed by 0.15g/200ml humic acid ranged from 4.62% to 6.17% and 1.59% to 7.09%, respectively. This work demonstrates the importance of a knowledge of solution chemistry in investigating the desorption of radionuclides.

  19. Effects of solution pH and complexing reagents on uranium and thorium desorption under saturated equilibrium conditions

    SciTech Connect

    Wang, Yug-Yea; Yu, C.

    1992-01-01

    Three contaminated bulk surface soils were used for investigating the effect of solution pH and complexing reagents on uranium and thorium desorption. At a low solution pH, the major chemical species of uranium and thorium, uranyl UO{sub 2}{sup +2}, thorium dihydroxide Th(OH){sub 2}{sup +2}, and thorium hydroxide Th(OH){sup +3}, tend to form complexes with acetates in the solution phase, which increases the fractions of uranium and thorium desorbed into this phase. At a high solution pH, important uranium and thorium species such as uranyl tricarbonate complex UO{sub 2}(CO){sub 3}{sub 3}{sup {minus}4} and thorium tetrahydroxide complex Th(OH){sub 4} tend to resist complexation with acetates. The presence of complexing reagents in solution can release radionuclides such as uranium and/or thorium from the soil to the solution by forming soluble complexes. Sodium bicarbonate (NaHCO{sub 3}) and diethylenetriaminepentaacetic acid (DTPA) are strong complex formers that released 38% to 62% of total uranium activity and 78% to 86% of total thorium activity, respectively, from the soil samples investigated. Solutions of 0.1 molar sodium nitrate (NaNO{sub 3}) and 0.1 molar sodium sulfate (Na{sub 2}SO{sub 4}) were not effective complex formers with uranium and thorium under the experimental conditions. Fractions of uranium and thorium desorbed by 0.15g/200ml humic acid ranged from 4.62% to 6.17% and 1.59% to 7.09%, respectively. This work demonstrates the importance of a knowledge of solution chemistry in investigating the desorption of radionuclides.

  20. Comparison of the radiological impacts of thorium and uranium nuclear fuel cycles

    SciTech Connect

    Meyer, H.R.; Witherspoon, J.P.; McBride, J.P.; Frederick, E.J.

    1982-03-01

    This report compares the radiological impacts of a fuel cycle in which only uranium is recycled, as presented in the Final Generic Environmental Statement on the Use of Recycle Plutonium in Mixed Oxide Fuel in Light Water Cooled Reactors (GESMO), with those of the light-water breeder reactor (LWBR) thorium/uranium fuel cycle in the Final Environmental Statement, Light Water Breeder Reactor Program. The significant offsite radiological impacts from routine operation of the fuel cycles result from the mining and milling of thorium and uranium ores, reprocessing spent fuel, and reactor operations. The major difference between the impacts from the two fuel cycles is the larger dose commitments associated with current uranium mining and milling operations as compared to thorium mining and milling. Estimated dose commitments from the reprocessing of either fuel type are small and show only moderate variations for specific doses. No significant differences in environmental radiological impact are anticipated for reactors using either of the fuel cycles. Radiological impacts associated with routine releases from the operation of either the thorium or uranium fuel cycles can be held to acceptably low levels by existing regulations.

  1. The distribution of uranium and thorium in granitic rocks of the basin and range province, Western United States

    USGS Publications Warehouse

    McNeal, J.M.; Lee, D.E.; Millard, H.T.

    1981-01-01

    Some secondary uranium deposits are thought to have formed from uranium derived by the weathering of silicic igneous rocks such as granites, rhyolites, and tuffs. A regional geochemical survey was made to determine the distribution of uranium and thorium in granitic rocks of the Basin and Range province in order to evaluate the potential for secondary uranium occurrences in the area. The resulting geochemical maps of uranium, thorium, and the Th:U ratio may be useful in locating target areas for uranium exploration. The granites were sampled according to a five-level, nested, analysis-of-variance design, permitting estimates to be made of the variance due to differences between:(1) two-degree cells; (2) one-degree cells; (3) plutons; (4) samples; and (5) analyses. The cells are areas described in units of degrees of latitude and longitude. The results show that individual plutons tend to differ in uranium and thorium concentrations, but that each pluton tends to be relatively homogeneous. Only small amounts of variance occur at the two degree and the between-analyses levels. The three geochemical maps that were prepared are based on one-degree cell means. The reproducibility of the maps is U > Th ??? Th:U. These geochemical maps may be used in three methods of locating target areas for uranium exploration. The first method uses the concept that plutons containing the greatest amounts of uranium may supply the greatest amounts of uranium for the formation of secondary uranium occurrences. The second method is to examine areas with high thorium contents, because thorium and uranium are initially highly correlated but much uranium could be lost by weathering. The third method is to locate areas in which the plutons have particularly high Th:U ratios. Because uranium, but not thorium, is leached by chemical weathering, high Th:U ratios suggest a possible loss of uranium and possibly a greater potential for secondary uranium occurrences to be found in the area. ?? 1981.

  2. Analysis of thorium-salted fuels to improve uranium utilization in the once-through fuel cycle

    SciTech Connect

    Eschbach, E.A.; Merrill, E.T.; Prichard, A.W.

    1981-09-01

    Calculations and analyses indicate that no improvement can be achieved in uranium utilization for the once-through LWR fuel cycle over use of slightly enriched uranium by employing thorium distributed with uranium. The study included thorium additions: (1) slight amounts, (2) larger amounts, in either intimately mixed or in duplex pellets, (3) in spectrally shifted or not spectrally shifted reactors, and (4) in three- or five-year reactivity limited exposures. While thorium-uranium combinations improves the initial conversion ratio, the reactivity lifetime was not extended enough to override the additional uranium required. The effective fission cross-section of the bred /sup 233/U relative to /sup 239/Pu's in typical LWR neutron spectra is not large enough for /sup 233/U to make as great a contribution to end-of-life reactivity as /sup 239/Pu in a slightly enriched uranium fuel element. /sup 233/U's reactivity contribution relative to /sup 239/Pu's is lower in fuel configurations such as slightly enriched uranium LWR fuel loads. On the other hand, /sup 233/U's reactivity contribution appears more positive for reactors that involve lower average concentrations of thermal neutron absorbers. If /sup 238/U-thorium fuels reprocessed, the recovered /sup 233/U would increase uranium utilization, but may not reduce fuel cycle costs. The thorium-salted fuels exhibit substantially flatter reactivity characteristics with exposure time. Spectral shift helped the utilization of uranium and thorium.

  3. 10 CFR 40.28 - General license for custody and long-term care of uranium or thorium byproduct materials disposal...

    Code of Federal Regulations, 2011 CFR

    2011-01-01

    ... in this part for uranium or thorium mill tailings sites closed under title II of the Uranium Mill... this general license is to ensure that uranium and thorium mill tailings disposal sites will be cared... may issue a specific license, as specified in the Uranium Mill Tailings Radiation Control Act of...

  4. 10 CFR 40.28 - General license for custody and long-term care of uranium or thorium byproduct materials disposal...

    Code of Federal Regulations, 2013 CFR

    2013-01-01

    ... in this part for uranium or thorium mill tailings sites closed under title II of the Uranium Mill... this general license is to ensure that uranium and thorium mill tailings disposal sites will be cared... may issue a specific license, as specified in the Uranium Mill Tailings Radiation Control Act of...

  5. On the equilibrium isotopic composition of the thorium-uranium-plutonium fuel cycle

    NASA Astrophysics Data System (ADS)

    Marshalkin, V. Ye.; Povyshev, V. M.

    2016-12-01

    The equilibrium isotopic compositions and the times to equilibrium in the process of thorium-uranium-plutonium oxide fuel recycling in VVER-type reactors using heavy water mixed with light water are estimated. It is demonstrated thEhfat such reactors have a capacity to operate with self-reproduction of active isotopes in the equilibrium mode.

  6. Recovery of uranium-233 from a thorium breeding blanket by pyrochemical techniques

    SciTech Connect

    Coops, M.S.; Knighton, J.B.

    1982-12-08

    We have carefully evaluated several processes that might be suitable for uranium recovery from thorium metal, and have chosen two that hold great promise. Both are simple non-aqueous methods that can readily be performed by remote means, and both require only a few simple process steps.

  7. Uranium and thorium sequential separation from norm samples by using a SIA system.

    PubMed

    Mola, M; Nieto, A; Peñalver, A; Borrull, F; Aguilar, C

    2014-01-01

    This study presents a sequential radiochemical separation method for uranium and thorium isotopes using a novel Sequential Injection Analysis (SIA) system with an extraction chromatographic resin (UTEVA). After the separation, uranium and thorium isotopes have been quantified by using alpha-particle spectrometry. The developed method has been tested by analyzing an intercomparison sample (phosphogypsum sample) from International Atomic Energy Agency (IAEA) with better recoveries for uranium and thorium than the obtained by using a classical method (93% for uranium using the new methodology and 82% with the classical method, and in the case of thorium the recoveries were 70% for the semi-automated method and 60% for the classical strategy). Afterwards, the method was successfully applied to different Naturally Occurring Radioactive Material (NORM) samples, in particular sludge samples taken from a drinking water treatment plant (DWTP) and also sediment samples taken from an area of influence of the dicalcium phosphate (DCP) factory located close to the Ebro river reservoir in Flix (Catalonia). The obtained results have also been compared with the obtained by the classical method and from that comparison it has been demonstrated that the presented strategy is a good alternative to existing methods offering some advantages as minimization of sample handling, reduction of solvents volume and also an important reduction of the time per analysis.

  8. Mechanisms of magma generation beneath hawaii and mid-ocean ridges: uranium/thorium and samarium/neodymium isotopic evidence.

    PubMed

    Sims, K W; Depaolo, D J; Murrell, M T; Baldridge, W S; Goldstein, S J; Clague, D A

    1995-01-27

    Measurements of uranium/thorium and samarium/neodymium isotopes and concentrations in a suite of Hawaiian basalts show that uranium/thorium fractionation varies systematically with samarium/neodymium fractionation and major-element composition; these correlations can be understood in terms of simple batch melting models with a garnet-bearing peridotite magma source and melt fractions of 0.25 to 6.5 percent. Midocean ridge basalts shows a systematic but much different relation between uranium/thorium fractionation and samarium/neodymium fractionation, which, although broadly consistent with melting of a garnet-bearing peridotite source, requires a more complex melting model.

  9. 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.

  10. Southern complex: geology, geochemistry, mineralogy, and mineral chemistry of selected uranium- and thorium-rich granites

    SciTech Connect

    Hoffman, M.A.

    1987-01-01

    Four major rock groups are defined in the Southern Complex: the Bell Creek Granite (BCG), the Clotted Granitoids (CGR), the Albite Granite (AGR), and the Migmatite Complex. Metatexites of the Migmatite Complex are the oldest rocks and include paleosome of a metasedimentary and metavolcanic protolith represented by Banded Iron Formation, Banded Amphibolite, and Banded Gneisses, and interlayered or crosscutting leucogranites. The CGR span the range from metatexite to diatexite and represent in-situ partial melting of metapelitic layers in the protolith during intrusion of the BCG. The BCG cuts the migmatites, is locally cut by the CGR, and was derived by partial melting of a dominantly metasedimentary protolith at some depth below the presently exposed migmatites during a regional tectonothermal event. The Albite Granite is a 2km diameter, muscovite-fluorite-columbite-bearing intrusive stock that cuts all other major units. The thorium history of the BCG is a function of the history of monazite. The thorium history of the CGR is also dominated by monazite but the thorium content of this unit cannot be entirely accounted for by original restite monazite. The uranium history of the BCG and CGR was dominated by magmatic differentiation and post magmatic, metamorphic and supergene redistributions and is largely independent of the thorium history. The thorium and uranium history of the AGR was dominated by magmatic/deuteric processes unlike the BCG and CGR.

  11. Conceptual Core Analysis of Long Life PWR Utilizing Thorium-Uranium Fuel Cycle

    NASA Astrophysics Data System (ADS)

    Rouf; Su'ud, Zaki

    2016-08-01

    Conceptual core analysis of long life PWR utilizing thorium-uranium based fuel has conducted. The purpose of this study is to evaluate neutronic behavior of reactor core using combined thorium and enriched uranium fuel. Based on this fuel composition, reactor core have higher conversion ratio rather than conventional fuel which could give longer operation length. This simulation performed using SRAC Code System based on library SRACLIB-JDL32. The calculation carried out for (Th-U)O2 and (Th-U)C fuel with uranium composition 30 - 40% and gadolinium (Gd2O3) as burnable poison 0,0125%. The fuel composition adjusted to obtain burn up length 10 - 15 years under thermal power 600 - 1000 MWt. The key properties such as uranium enrichment, fuel volume fraction, percentage of uranium are evaluated. Core calculation on this study adopted R-Z geometry divided by 3 region, each region have different uranium enrichment. The result show multiplication factor every burn up step for 15 years operation length, power distribution behavior, power peaking factor, and conversion ratio. The optimum core design achieved when thermal power 600 MWt, percentage of uranium 35%, U-235 enrichment 11 - 13%, with 14 years operation length, axial and radial power peaking factor about 1.5 and 1.2 respectively.

  12. 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.

  13. Uranium and thorium complexes of the phosphaethynolate ion

    DOE PAGES

    Camp, Clément; Settineri, Nicholas; Lefèvre, Julia; ...

    2015-06-20

    New tris-amidinate actinide (Th, U) complexes containing a rare O-bound terminal phosphaethynolate (OCP⁻) ligand were synthesized and fully characterized. The cyanate (OCN⁻) and thiocyanate (SCN⁻) analogs were prepared for comparison and feature a preferential N-coordination to the actinide metals. The Th(amid)3(OCP) complex reacts with Ni(COD)2 to yield the heterobimetallic adduct (amid)3Th(μ-η1(O):η2(C,P)-OCP)Ni(COD) featuring an unprecedented reduced (OCP⁻) bent fragment bridging the two metals.

  14. Uranium and thorium complexes of the phosphaethynolate ion

    SciTech Connect

    Camp, Clément; Settineri, Nicholas; Lefèvre, Julia; Jupp, Andrew R.; Goicoechea, José M.; Maron, Laurent; Arnold, John

    2015-06-20

    New tris-amidinate actinide (Th, U) complexes containing a rare O-bound terminal phosphaethynolate (OCP⁻) ligand were synthesized and fully characterized. The cyanate (OCN⁻) and thiocyanate (SCN⁻) analogs were prepared for comparison and feature a preferential N-coordination to the actinide metals. The Th(amid)3(OCP) complex reacts with Ni(COD)2 to yield the heterobimetallic adduct (amid)3Th(μ-η1(O):η2(C,P)-OCP)Ni(COD) featuring an unprecedented reduced (OCP⁻) bent fragment bridging the two metals.

  15. EPA Method EMSL-33: Isotopic Determination of Plutonium, Uranium, and Thorium in Water, Soil, Air, and Biological Tissue

    EPA Pesticide Factsheets

    SAM lists this method to provide for the analysis of isotopic plutonium, uranium and thorium, together or individually, in drinking water, aqueous/liquid, soil/sediment, surface wipe and/or air filter samples by alpha spectrometry.

  16. Uranium and thorium in granitic rocks of northeastern Washington and northern Idaho, with comments on uranium resource potential

    USGS Publications Warehouse

    Nash, J. Thomas

    1979-01-01

    Northeastern Washington and northern Idaho is a uranium province in which many Cretaceous and Tertiary granitic plutons contain abnormal amounts of uranium. Mean uranium content of 108 samples of granitic rock is 8.8 parts per million (ppm), more than twice normal for rocks of this composition. The mean thorium content, 20.3 ppm, and mean Th/U, 3.19, are normal. The most uraniferous and fertile rocks are the peraluminous two-mica granitic suite, although not all two-mica plutons are enriched in uranium. The muscovite-bearing suite has mean uranium content of 22.3 ppm, mean thorium content of 22.8 ppm, and mean Th/U of 2.82. Porphyritic quartz monzonite of the Midnite mine, which I interpret to be a two-mica granitic rock, is especially radioactive with mean U of 14.7 ppm, mean Th of 32.1 ppm, and mean Th/U of 2.72. Mean uranium and thorium contents of the two-mica granitic plutons are significantly different from those of the calcalkaline hornblende granitic suite, which are mean U, 5.0 ppm; mean Th, 17.6; and mean Th/U, 3.78. Biotite granitic rocks containing no hornblende or muscovite appear to be an intermediate suite in terms of U and Th, or possibly are variants of both hornblende and muscovite type; mean U is 3.88 ppm, mean Th is 14.4 ppm, and mean Th/U is 3.03 as calculated from the more abundant data of Castor and others (1978). occurrence of uranium and thorium in the muscovite and hornblende suites is systematically different. Many muscovite-bearing rocks are much more enriched in uranium (>15 ppm) than they are in thorium, and have a relatively low Th:U correlation coefficient of +0.409. Many of the uraniferous muscovite-bearing rocks contain less than 20 ppm Th, probably a consequence of forming by anatexis of thorium deficient sedimentary rocks. Uranium and thorium variation is much more regular in the hornblende suite, which has a Th:U correlation coefficient of +0.780. Uranium in the muscovite suite is held primarily in magnetite and biotite, and

  17. Determination of uranium and thorium in complex samples using chromatographic separation, ICP-MS and spectrophotometric detection.

    PubMed

    Rozmarić, Martina; Ivsić, Astrid Gojmerac; Grahek, Zeljko

    2009-11-15

    The paper describes a research of possible application of UTEVA and TRU resins and anion exchanger AMBERLITE CG-400 in nitrate form for the isolation of uranium and thorium from natural samples. The results of determination of distribution coefficient have shown that uranium and thorium bind on TRU and UTEVA resins from the solutions of nitric and hydrochloric acids, and binding strength increases proportionally to increase the concentration of acids. Uranium and thorium bind rather strongly to TRU resin from the nitric acid in concentration ranging from 0.5 to 5 mol L(-1), while large quantities of other ions present in the sample do not influence on the binding strength. Due to the difference in binding strength in HCl and HNO(3) respectively, uranium and thorium can be easily separated from each other on the columns filled with TRU resin. Furthermore, thorium binds to anion exchanger in nitrate form from alcohol solutions of nitric acid very strongly, while uranium does not, so they can be easily separated. Based on these results, we have created the procedures of preconcentration and separation of uranium and thorium from the soil, drinking water and seawater samples by using TRU and UTEVA resins and strong base anion exchangers in nitrate form. In one of the procedures, uranium and thorium bind directly from the samples of drinking water and seawater on the column filled with TRU resin from 0.5 mol L(-1) HNO(3) in a water sample. After binding, thorium is separated from uranium with 0.5 mol L(-1) HCl, and uranium is eluted with deionised water. By applying the described procedure, it is possible to achieve the concentration factor of over 1000 for the column filled with 1g of resin and splashed with 2L of the sample. Spectrophotometric determination with Arsenazo III, with this concentration factor results in detection limits below 1 microg L(-1) for uranium and thorium. In the second procedure, uranium and thorium are isolated from the soil samples with TRU

  18. 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)

  19. Laser-induced breakdown spectroscopy for determination of uranium in thorium-uranium mixed oxide fuel materials.

    PubMed

    Sarkar, Arnab; Alamelu, Devanathan; Aggarwal, Suresh K

    2009-05-15

    Laser-induced breakdown spectroscopy (LIBS) has been developed for determining the percentage of uranium in thorium-uranium mixed oxide fuel samples required as a part of the chemical quality assurance of fuel materials. The experimental parameters were optimized using mixed oxide pellets prepared from 1:1 (w/w) mixture of thorium-uranium mixed oxide standards and using boric acid as a binder. Calibration curves were established using U(II) 263.553 nm, U(II) 367.007 nm, U(II) 447.233 nm and U(II) 454.363 nm emission lines. The uranium amount determined in two synthetic mixed oxide samples using calibration curves agreed well with that of the expected values. Except for U(II) 263.553 nm, all the other emission lines exhibited a saturation effect due to self-absorption when U amount exceeded 20 wt.% in the Th-U mixture. The present method will be useful for fast and routine determination of uranium in mixed oxide samples of Th and U, without the need for dissolution, which is difficult and time consuming due to the refractory nature of ThO(2). The methodology developed is encouraging since a very good analytical agreement was obtained considering the limited resolution of the spectrometer employed in the work.

  20. Summary of the radiological assessment of the fuel cycle for a thorium-uranium carbide-fueled fast breeder reactor

    SciTech Connect

    Tennery, V.J.; Bomar, E.S.; Bond, W.D.; Meyer, H.R.; Morse, L.E.; Till, J.E.; Yalcintas, M.G.

    1980-01-01

    A large fraction of the potential fuel for nuclear power reactors employing fissionable materials exists as ores of thorium. In addition, certain characteristics of a fuel system based on breeding of the fissionable isotope {sup 233}U from thorium offer the possibility of a greater resistance to the diversion of fissionable material for the fabrication of nuclear weapons. This report consolidates into a single source the principal content of two previous reports which assess the radiological environmental impact of mining and milling of thorium ore and of the reprocessing and refabrication of spent FBR thorium-uranium carbide fuel.

  1. Micro-column solid phase extraction to determine uranium and thorium in environmental samples.

    PubMed

    Tsai, Tsuey-Lin; Lin, Chun-Chih; Chu, Tieh-Chi

    2008-08-01

    Extraction chromatographic separation techniques based on U/TEVA and TEVA resins were utilized to separate uranium and thorium isotopes in complex matrices from environmental samples. This approach has the advantages of ease of quantitative analysis, small sample size, an absence of mixed waste solvents, complete separation of U/Th isotopes, acceptable chemical yields and good energy resolution in the alpha spectrum. The procedure for analyzing alpha-emitting isotopes of uranium and thorium in geothermal water from Peito, Taiwan, is illustrated in detail. It involves sample pre-concentration, filtration and separation by highly selective extraction chromatographic resins, followed by electroplating and alpha-spectroscopy. The analytical results show a chemical recovery exceeding 55% for U and 65% for Th, respectively, under optimized conditions. The efficient and cost-effective use of recyclable columns makes the analytical methods simple, accurate, rapid, reliable and robust.

  2. New Twists and Turns for Actinide Chemistry: Organometallic Infinite Coordination Polymers of Thorium Diazide.

    PubMed

    Monreal, Marisa J; Seaman, Lani A; Goff, George S; Michalczyk, Ryszard; Morris, David E; Scott, Brian L; Kiplinger, Jaqueline L

    2016-03-07

    Two organometallic 1D infinite coordination polymers and two organometallic monometallic complexes of thorium diazide have been synthesized and characterized. Steric control of these self-assembled arrays, which are dense in thorium and nitrogen, has also been demonstrated: infinite chains can be circumvented by using steric bulk either at the metallocene or with a donor ligand in the wedge.

  3. Thorium: Uranium fuel cycle in safe reactors, the time is now

    SciTech Connect

    Gat, Uri

    1995-12-31

    The thorium-uranium fuel cycle has several advantages that make it attractive. Some of these beneficial properties are of particular interest now as they help alleviate current concerns. The Th-U cycle has neutronic advantages when utilized in thermal or epithermal reactors. Some of these reactors enjoy extraordinary safety qualities. The combination of these traits suggest that now is an appropriate time to deploy and begin exploiting the Th-U fuel cycle.

  4. Uranium, thorium and rare earth elements in macrofungi: what are the genuine concentrations?

    PubMed

    Borovička, Jan; Kubrová, Jaroslava; Rohovec, Jan; Randa, Zdeněk; Dunn, Colin E

    2011-10-01

    Concentrations of uranium, thorium and rare earth elements (REE) in 36 species of ectomycorrhizal (26 samples) and saprobic (25 samples) macrofungi from unpolluted sites with differing bedrock geochemistry were analyzed by inductively coupled plasma mass spectrometry (ICP-MS). Analytical results are supported by use of certified reference materials (BCR-670, BCR-667, NIST-1575a) and the reliability of the determination of uranium was verified by epithermal neutron activation analysis (ENAA). It appears that data recently published on these elements are erroneous, in part because of use of an inappropriate analytical method; and in part because of apparent contamination by soil particles resulting in elevated levels of thorium and REE. Macrofungi from unpolluted areas, in general, did not accumulate high levels of the investigated metals. Concentrations of uranium and thorium were generally below 30 and 125 μg kg(-1) (dry weight), respectively. Concentrations of REE in macrofungi did not exceed 360 μg kg(-1) (dry weight) and their distribution more or less followed the trend observed in post-Archean shales and loess.

  5. Electrodeposition of uranium and thorium onto small platinum electrodes

    NASA Astrophysics Data System (ADS)

    Reichenberger, Michael A.; Ito, Takashi; Ugorowski, Philip B.; Montag, Benjamin W.; Stevenson, Sarah R.; Nichols, Daniel M.; McGregor, Douglas S.

    2016-03-01

    Preparation of thin U- and Th-coated 0.3 mm diameter Pt working electrodes by the cyclic potential sweep method is described. Uranyl- and thorium hydroxide layers were electrodeposited from ethanol solutions containing 0.02 M natural uranyl and 0.02 M natural thorium nitrate, each with 3.6 M ammonium nitrate. The cell for electrodeposition was specially developed in order to accommodate the small working electrodes for this research by including a working electrode probe, 3-D translation stage, and microscope. The source material deposition was analyzed using digital microscopy and scanning electron microscopy, and confirmed using x-ray fluorescence measurements. The appropriate potential range for electrodeposition was determined to be -0.62 V to -0.64 V for a 0.3 mm diameter Pt working electrode placed 1 cm from the counter electrode. Smooth, uniform deposition was observed near the central region of the working electrode, while surface cracking and crystalline formations were found near the edge of the working electrode. The final procedure for sample substrate preparation, electrolytic solution preparation and electrodeposition are described.

  6. Dissolution of metal oxides and separation of uranium from lanthanides and actinides in supercritical carbon dioxide

    SciTech Connect

    Quach, D.L.; Wai, C.M.; Mincher, B.J.

    2013-07-01

    This paper investigates the feasibility of extracting and separating uranium from lanthanides and other actinides by using supercritical fluid carbon dioxide (sc-CO{sub 2}) as a solvent modified with tri-n-butylphosphate (TBP) for the development of a counter current stripping technique, which would be a more efficient and environmentally benign technology for spent nuclear fuel reprocessing compared to traditional solvent extraction. Several actinides (U, Pu, and Np) and europium were extracted in sc-CO{sub 2} modified with TBP over a range of nitric acid concentrations and then the actinides were exposed to reducing and complexing agents to suppress their extractability. According to this study, uranium/europium and uranium/plutonium extraction and separation in sc-CO{sub 2} modified with TBP is successful at nitric acid concentrations of less than 6 M and at nitric acid concentrations of less than 3 M with acetohydroxamic acid or oxalic acid, respectively. A scheme for recycling uranium from spent nuclear fuel by using sc-CO{sub 2} and counter current stripping columns is presented. (authors)

  7. DISSOLUTION OF METAL OXIDES AND SEPARATION OF URANIUM FROM LANTHANIDES AND ACTINIDES IN SUPERCRITICAL CARBON DIOXIDE

    SciTech Connect

    Donna L. Quach; Bruce J. Mincher; Chien M. Wai

    2013-10-01

    This paper investigates the feasibility of extracting and separating uranium from lanthanides and other actinides by using supercritical fluid carbon dioxide (sc-CO2) as a solvent modified with tri-n-butylphosphate (TBP) for the development of a counter current stripping technique, which would be a more efficient and environmentally benign technology for spent nuclear fuel reprocessing compared to traditional solvent extraction. Several actinides (U, Pu, and Np) and europium were extracted in sc-CO2 modified with TBP over a range of nitric acid concentrations and then the actinides were exposed to reducing and complexing agents to suppress their extractability. According to this study, uranium/europium and uranium/plutonium extraction and separation in sc-CO2 modified with TBP is successful at nitric acid concentrations of less than 6 M and at nitric acid concentrations of less than 3 M with acetohydroxamic acid or oxalic acid, respectively. A scheme for recycling uranium from spent nuclear fuel by using sc-CO2 and counter current stripping columns is presented.

  8. Calculated optical properties of thorium, protactinium, and uranium metals

    SciTech Connect

    Gasche, T.; Brooks, M.S.; Johansson, B.

    1996-07-01

    We report self-consistent energy band calculations using the linear muffin-tin orbital method and the local-spin-density approximation to exchange and correlation in density-functional theory for the light actinide metals Th, Pa, and U. The optical properties have been calculated and compared with measurements, where possible. The dependence of the optical response functions upon crystal structure was found to be surprisingly large and the dependence upon spin-orbit coupling, less so. Where it was possible to make comparison, agreement with experiment was obtained for the maxima of the optical spectra, the exception being a feature in the optical conductivity at 10 eV measured in both Th and U but not obtained in the calculations. {copyright} {ital 1996 The American Physical Society.}

  9. A neutron activation analysis procedure for the determination of uranium, thorium and potassium in geologic samples

    USGS Publications Warehouse

    Aruscavage, P. J.; Millard, H.T.

    1972-01-01

    A neutron activation analysis procedure was developed for the determination of uranium, thorium and potassium in basic and ultrabasic rocks. The three elements are determined in the same 0.5-g sample following a 30-min irradiation in a thermal neutron flux of 2??1012 n??cm-2??sec-1. Following radiochemical separation, the nuclides239U (T=23.5 m),233Th (T=22.2 m) and42K (T=12.36 h) are measured by ??-counting. A computer program is used to resolve the decay curves which are complex owing to contamination and the growth of daughter activities. The method was used to determine uranium, throium and potassium in the U. S. Geological Survey standard rocks DTS-1, PCC-1 and BCR-1. For 0.5-g samples the limits of detection for uranium, throium and potassium are 0.7, 1.0 and 10 ppb, respectively. ?? 1972 Akade??miai Kiado??.

  10. Uranium-thorium isotope geochemistry of saline ground waters from central Missouri

    SciTech Connect

    Banner, J.L.; Chen, J.H.; Wasserburg, G.J.

    1989-03-01

    The isotopic and elemental distributions of uranium and thorium were examined in a suite of saline ground waters from central Missouri using mass spectrometric techniques. The waters were sampled from natural springs and artesian wells in Mississippian and Ordovician aquifers and have a wide range in salinity (5 to 26 /per thousand/), deltaD (/minus/108 to /minus/45 /per thousand/), and delta/sup 18/O (/minus/14.7 to /minus/6.5 /per thousand/) values. The suite of samples has a large range in /sup 238/U (50 to 200 x 10/sup /minus/12/g/g) and /sup 232/Th (0.3 to 9.1 x 10/sup /minus/12/g/g) concentrations and extremely high /sup 234/U//sup 238/U activity ratios ranging from 2.15 to 16.0. These isotopic compositions represent pronounced uranium-series disequilibrium compared with the value of modern seawater (1.15) or the equilibrium value (1.00). For such /sup 234/U-enriched waters, /sup 234/U//sup 238/U isotope ratios can be determined with a precision of /+-/ 10 /per thousand/ (2sigma) on 10 mL of sample and less than /+-/5 /per thousand/ on 100 mL. In contrast to the large /sup 234/U enrichments, /sup 230/Th//sup 238/U activity ratios in the ground waters are significantly lower than the equilibrium value. The more saline samples have markedly higher /sup 234/U//sup 238/U activity ratios and lower deltaD and delta/sup 18/O values. Unfiltered and filtered (< 0.1 ..mu..m) aliquots of a saline sample have the same isotopic composition and concentration of uranium, indicating uranium essentially occurs entirely as a dissolved species. The filtered/unfiltered concentration ratio for thorium in this sample is 0.29, demonstrating the predominant association of thorium with particulates.

  11. PWR core design, neutronics evaluation and fuel cycle analysis for thorium-uranium breeding recycle

    SciTech Connect

    Bi, G.; Liu, C.; Si, S.

    2012-07-01

    This paper was focused on core design, neutronics evaluation and fuel cycle analysis for Thorium-Uranium Breeding Recycle in current PWRs, without any major change to the fuel lattice and the core internals, but substituting the UOX pellet with Thorium-based pellet. The fuel cycle analysis indicates that Thorium-Uranium Breeding Recycle is technically feasible in current PWRs. A 4-loop, 193-assembly PWR core utilizing 17 x 17 fuel assemblies (FAs) was taken as the model core. Two mixed cores were investigated respectively loaded with mixed reactor grade Plutonium-Thorium (PuThOX) FAs and mixed reactor grade {sup 233}U-Thorium (U{sub 3}ThOX) FAs on the basis of reference full Uranium oxide (UOX) equilibrium-cycle core. The UOX/PuThOX mixed core consists of 121 UOX FAs and 72 PuThOX FAs. The reactor grade {sup 233}U extracted from burnt PuThOX fuel was used to fabrication of U{sub 3}ThOX for starting Thorium-. Uranium breeding recycle. In UOX/U{sub 3}ThOX mixed core, the well designed U{sub 3}ThOX FAs with 1.94 w/o fissile uranium (mainly {sup 233}U) were located on the periphery of core as a blanket region. U{sub 3}ThOX FAs remained in-core for 6 cycles with the discharged burnup achieving 28 GWD/tHM. Compared with initially loading, the fissile material inventory in U{sub 3}ThOX fuel has increased by 7% via 1-year cooling after discharge. 157 UOX fuel assemblies were located in the inner of UOX/U{sub 3}ThOX mixed core refueling with 64 FAs at each cycle. The designed UOX/PuThOX and UOX/U{sub 3}ThOX mixed core satisfied related nuclear design criteria. The full core performance analyses have shown that mixed core with PuThOX loading has similar impacts as MOX on several neutronic characteristic parameters, such as reduced differential boron worth, higher critical boron concentration, more negative moderator temperature coefficient, reduced control rod worth, reduced shutdown margin, etc.; while mixed core with U{sub 3}ThOX loading on the periphery of core has no

  12. Ion source development for ultratrace detection of uranium and thorium

    NASA Astrophysics Data System (ADS)

    Liu, Y.; Batchelder, J. C.; Galindo-Uribarri, A.; Chu, R.; Fan, S.; Romero-Romero, E.; Stracener, D. W.

    2015-10-01

    Efficient ion sources are needed for detecting ultratrace U and Th impurities in a copper matrix by mass spectrometry techniques such as accelerator mass spectrometry (AMS). Two positive ion sources, a hot-cavity surface ionization source and a resonant ionization laser ion source, are evaluated in terms of ionization efficiencies for generating ion beams of U and Th. The performances of the ion sources are characterized using uranyl nitrate and thorium nitrate sample materials with sample sizes between 20 and 40 μg of U or Th. For the surface ion source, the dominant ion beams observed are UO+ or ThO+ and ionization efficiencies of 2-4% have been obtained with W and Re cavities. With the laser ion source, three-step resonant photoionization of U atoms has been studied and only atomic U ions are observed. An ionization efficiency of about 9% has been demonstrated. The performances of both ion sources are expected to be further improved.

  13. Ion Source Development for Ultratrace Detection of Uranium and Thorium

    SciTech Connect

    Liu, Yuan; Batchelder, Jon Charles; Galindo-Uribarri, Alfredo {nmn}; Stracener, Daniel W

    2015-01-01

    A hot-cavity surface ionization source and a hot-cavity laser ion source are evaluated in terms of ionization efficiencies for generating ion beams of U and Th. The work is motivated by the need for more efficient ion sources for detecting ultratrace U and Th impurities in a copper matrix by mass spectrometry techniques such as accelerator mass spectrometry (AMS). The performances of the ion sources are characterized using uranyl nitrate and thorium nitrate sample materials and sample sizes of 20 - 40 g of U or Th. For the surface source, the dominant ion beams observed are UO+ or ThO+ and ionization efficiencies of 2-4% have been obtained with W and Re cavities. Three-step resonant photoionization of U atoms is studied and an ionization efficiency of 8.7% has been obtained with the laser ion source. The positive ion sources promise more than an order of magnitude more efficient than conventional Cs-sputter negative ion sources used for AMS. In addition, the laser ion source is highly selective and effective in suppressing interfering and ions. Work is in progress to improve the efficiencies of both positive ion sources.

  14. Contents of cesium, iodine, strontium, thorium, and uranium in selected human organs of adult asian population.

    PubMed

    Iyengar, G V; Kawamura, H; Dang, H S; Parr, R M; Wang, J W; Cho, S Y; Natera, E S

    2004-08-01

    Contents of cesium, iodine, strontium, thorium, and uranium in some selected human organs were estimated for adult Asian population using data obtained in four Asian countries: China, India, Philippines, and Republic of Korea, as part of a Coordinated Research Program of the International Atomic Energy Agency on "Ingestion and Organ contents of elements of importance in radiation protection." These countries together represent more than 40% of the world population. Highly sensitive analytical techniques were employed to measure cesium in skeletal muscle, iodine in thyroid, strontium in skeleton, thorium and uranium in skeleton, liver, kidneys, and lungs where, in comparison to other organs, these elements are present in higher concentrations. The organ contents for adult Asian population, when compared with the corresponding data proposed for Reference Man by International Commission on Radiological Protection (ICRP), showed about 40 times lower kidneys content and about 10 times lower skeleton content of uranium. The content of thorium in skeleton for Asian population was also half of the ICRP Reference Man value. Interestingly, organ contents for the other elements such as iodine in thyroid, cesium in skeletal muscle, and strontium in skeleton were comparable for Asian and the Caucasian population (represented by ICRP Reference Man). Organ contents for these elements were also calculated by applying the new ICRP models of these elements to their daily intakes. The comparison of the calculated and measured organ contents showed that despite uncertainties in the organ content values arising due to the inter-country variations in daily dietary intakes, the contents were within a factor of two to three. This observation is significant since human data both on organ contents and ingestion were obtained at environmental level of intakes. The study suggests that currently available ICRP models for these elements are quite realistic.

  15. Thorium-uranium fractionation by garnet - Evidence for a deep source and rapid rise of oceanic basalts

    NASA Technical Reports Server (NTRS)

    Latourrette, T. Z.; Kennedy, A. K.; Wasserburg, G. J.

    1993-01-01

    Mid-ocean ridge basalts (MORBs) and ocean island basalts (OIBs) are derived by partial melting of the upper mantle and are marked by systematic excesses of thorium-230 activity relative to the activity of its parent, uranium-238. Experimental measurements of the distribution of thorium and uranium between the melt and solid residue show that, of the major phases in the upper mantle, only garnet will retain uranium over thorium. This sense of fractionation, which is opposite to that caused by clinopyroxene-melt partitioning, is consistent with the thorium-230 excesses observed in young oceanic basalts. Thus, both MORBs and OIBs must begin partial melting in the garnet stability field or below about 70 kilometers. A calculation shows that the thorium-230-uranium-238 disequilibrium in MORBs can be attributed to dynamic partial melting beginning at 80 kilometers with a melt porosity of 0.2 percent or more. This result requires that melting beneath ridges occurs in a wide region and that the magma rises to the surface at a velocity of at least 0.9 meter per year.

  16. Supercritical fluid extraction and separation of uranium from other actinides.

    PubMed

    Quach, Donna L; Mincher, Bruce J; Wai, Chien M

    2014-06-15

    The feasibility of separating U from nitric acid solutions of mixed actinides using tri-n-butylphosphate (TBP)-modified supercritical fluid carbon dioxide (sc-CO2) was investigated. The actinides U, Np, Pu, and Am were extracted into sc-CO2 modified with TBP from a range of nitric acid concentrations, in the absence of, or in the presence of, a number of traditional reducing and/or complexing agents to demonstrate the separation of these metals from U under sc-CO2 conditions. The separation of U from Pu using sc-CO2 was successful at nitric acid concentrations of less than 3M in the presence of acetohydroxamic acid (AHA) or oxalic acid (OA) to mitigate Pu extraction, and the separation of U from Np was successful at nitric acid concentrations of less than 1M in the presence of AHA, OA, or sodium nitrite to mitigate Np extraction. Americium was not well extracted under any condition studied.

  17. Uranium and thorium leached from uranium mill tailing of Guangdong Province, China and its implication for radiological risk.

    PubMed

    Wang, J; Liu, J; Zhu, L; Qi, J Y; Chen, Y H; Xiao, T F; Fu, S M; Wang, C L; Li, J W

    2012-11-01

    The paper focused on the leaching behaviour of uranium (U) and thorium (Th) from uranium mill tailing collected from the Uranium Mill Plant in Northern Guangdong Province, China. Distilled water (pH 6) and sulphuric acid solution (pH 4 and 3) were used as solvent for the leaching over 22 weeks. It was found that the cumulative leach fraction from the mill tailing was 0.1, 0.1 and 0.7 % for U release, and overall 0.01 % for Th release, using distilled water, sulphuric acid solution of pH 4 and pH 3 as leaching agents, respectively. The results indicate that (1) the release of U and Th in uranium mill tailing is a slow and long-term process; (2) surface dissolution is the main mechanism for the release of U and Th when sulphuric acid solution of pH 3 is employed as the leaching agent; (3) both U and Th are released by diffusion when using sulphuric acid solution of pH 4 as the leaching agent and (4) U is released by surface dissolution, while Th is released by diffusion when using distilled water as the leaching agent. The implication for radiological risk in the real environment was also discussed.

  18. Theoretical analysis of uranium-doped thorium dioxide: Introduction of a thoria force field with explicit polarization

    SciTech Connect

    Shields, A. E.; Ruiz Hernandez, S. E.; Leeuw, N. H. de

    2015-08-15

    Thorium dioxide is used industrially in high temperature applications, but more insight is needed into the behavior of the material as part of a mixed-oxide (MOX) nuclear fuel, incorporating uranium. We have developed a new interatomic potential model including polarizability via a shell model, and commensurate with a prominent existing UO{sub 2} potential, to conduct configurational analyses and to investigate the thermophysical properties of uranium-doped ThO{sub 2}. Using the GULP and Site Occupancy Disorder (SOD) computational codes, we have analyzed the distribution of low concentrations of uranium in the bulk material, where we have not observed the formation of uranium clusters or the dominance of a single preferred configuration. We have calculated thermophysical properties of pure thorium dioxide and Th{sub (1−x)}U{sub x}O{sub 2} which generated values in very good agreement with experimental data.

  19. Theoretical analysis of uranium-doped thorium dioxide: Introduction of a thoria force field with explicit polarization

    NASA Astrophysics Data System (ADS)

    Shields, A. E.; Ruiz Hernandez, S. E.; de Leeuw, N. H.

    2015-08-01

    Thorium dioxide is used industrially in high temperature applications, but more insight is needed into the behavior of the material as part of a mixed-oxide (MOX) nuclear fuel, incorporating uranium. We have developed a new interatomic potential model including polarizability via a shell model, and commensurate with a prominent existing UO2 potential, to conduct configurational analyses and to investigate the thermophysical properties of uranium-doped ThO2. Using the GULP and Site Occupancy Disorder (SOD) computational codes, we have analyzed the distribution of low concentrations of uranium in the bulk material, where we have not observed the formation of uranium clusters or the dominance of a single preferred configuration. We have calculated thermophysical properties of pure thorium dioxide and Th(1-x)UxO2 which generated values in very good agreement with experimental data.

  20. IMPACT OF URANIUM AND THORIUM ON HIGH TIO2 CONCENTRATION NUCLEAR WASTE GLASSES

    SciTech Connect

    Fox, K.; Edwards, T.

    2012-01-11

    This study focused on the potential impacts of the addition of Crystalline Silicotitanate (CST) and Monosodium Titanate (MST) from the Small Column Ion Exchange (SCIX) process on the Defense Waste Processing Facility (DWPF) glass waste form and the applicability of the DWPF process control models. MST from the Salt Waste Processing Facility (SWPF) is also considered in the study. The KT08-series of glasses was designed to evaluate any impacts of the inclusion of uranium and thorium in glasses containing the SCIX components. All but one of the study glasses were found to be amorphous by X-ray diffraction (XRD). One of the slowly cooled glasses contained a small amount of trevorite, which is typically found in DWPF-type glasses and had no practical impact on the durability of the glass. The measured Product Consistency Test (PCT) responses for the study glasses and the viscosities of the glasses were well predicted by the current DWPF models. No unexpected issues were encountered when uranium and thorium were added to the glasses with SCIX components.

  1. Abundances of uranium, thorium, and potassium for some Australian crystalline rocks

    USGS Publications Warehouse

    Bunker, Carl Maurice; Bush, C.A.; Munroe, Robert J.; Sass, J.H.

    1975-01-01

    This report contains a tabulation of the basic radioelement and radiogenic heat data obtained during an Australian National University (ANU) - United States Geological Survey (USGS) heat-flow project, directed jointly by J. C. Jaeger (ANU) and J. H. Sass (USGS). Most samples were collected during the periods June through September, 1971 and 1972. The measurements were made subsequently by two of us (C. M. Bunker and C. A. Bush) using the gamma-ray spec trometric techniques described by Bunker and Bush (1966, 1967). Interpreting the spectra for quantitative analyses of the radioelements was accomplished with an iterative leastsquares computer program modified from one by Schonfeld (1966). Uranium content determined by gamma-ray spectrometry is based on a measurement of the daughter products of 226Ra. Equilibrium in the uranium-decay series was assumed for these analyses . Throughout the report, when U content is stated, radium-equivalent uranium is implied. The coefficient of variation for the accuracy of the radioelement data, when compared to ana lyses by isotope dilution and flame photometry is about 3 percent for radium-equivalent uranium and thorium and about 1 percent for potassium. These percentages are in addition to minimum standard deviations of about 0.05 ppm for U and Th, and about 0.03 percent for K.

  2. The feasibility study of small long-life gas cooled fast reactor with mixed natural Uranium/Thorium as fuel cycle input

    SciTech Connect

    Ariani, Menik; Su'ud, Zaki; Waris, Abdul; Khairurrijal,; Monado, Fiber; Sekimoto, Hiroshi

    2012-06-06

    A conceptual design study of Gas Cooled Fast Reactors with Modified CANDLE burn-up scheme has been performed. In this study, design GCFR with Helium coolant which can be continuously operated by supplying mixed Natural Uranium/Thorium without fuel enrichment plant or fuel reprocessing plant. The active reactor cores are divided into two region, Thorium fuel region and Uranium fuel region. Each fuel core regions are subdivided into ten parts (region-1 until region-10) with the same volume in the axial direction. The fresh Natural Uranium and Thorium is initially put in region-1, after one cycle of 10 years of burn-up it is shifted to region-2 and the each region-1 is filled by fresh natural Uranium/Thorium fuel. This concept is basically applied to all regions in both cores area, i.e. shifted the core of i{sup th} region into i+1 region after the end of 10 years burn-up cycle. For the next cycles, we will add only Natural Uranium and Thorium on each region-1. The calculation results show the reactivity reached by mixed Natural Uranium/Thorium with volume ratio is 4.7:1. This reactor can results power thermal 550 MWth. After reactor start-up the operation, furthermore reactor only needs Natural Uranium/Thorium supply for continue operation along 100 years.

  3. Selected values of chemical thermodynamic properties: compounds of uranium, protactinium, thorium, actinium, and the alkali metals. Final report

    SciTech Connect

    Wagman, D.D.; Evans, W.H.; Parker, V.B.; Schumm, R.H.; Nuttall, R.L.

    1981-05-01

    This publication contains tables of recommended values for the standard enthalpies (heats) of formation, Gibbs (free) energies of formation, entropies, enthalpy contents and heat capacities at 298.15 K, and enthalpies of formation at O K for compounds of uranium, protactinium, thorium, actinium, lithium, sodium, potassium, rubidium, cesium, and francium.

  4. Characteristics of a Mixed Thorium-Uranium Dioxide High-Burnup Fuel

    SciTech Connect

    J. S. Herring; P. E. MacDonald

    1999-06-01

    Future nuclear fuels must satisfy three sets of requirements: longer times between refueling; concerns for weapons proliferation; and development of a spent fuel form more suitable for direct geologic disposal. This project has investigated a fuel consisting of mixed thorium and uranium dioxide to satisfy these requirements. Results using the SCALE 4.3 code system indicated that the mixed Th-U fuel could be burned to 72 MWD/kg or 100 MWD/kg using 25% of 35% UO2 respectively. The uranium remained below 20% total fissile fraction throughout the cycle, making it unusable for weapons. Total plutonium production per MWD was a factor of 4.5 less in the Th-U fuel than in the conventional fuel; Pu-239 production per MWD was a factor of 6.5 less; and the plutonium produced was high in Pu-238, leading to a decay heat 5 times greater than that from plutonium derived from conventional fuel and 40 times greater than weapons grade plutonium. High decay heat would require active cooling of any crude weapon, lest the components surrounding the plutonium be melted. Spontaneous neutron production for plutonium from Th-U fuel was 2.3 times greater than that from conventional fuel and 15 times greater than that from weapons grade plutonium. High spontaneous neutron production drastically limits the probable yield of a crude weapon. Because ThO2 is the highest oxide of thorium, while UO2 can be oxidized further to U3O8, ThO2-UO2 fuel may be a superior wasteform if the spent fuel is ever to be exposed to oxygenated water. Even if the cost of fabricating the mixed Th-U fuel is $100/kg greater, the cost of the Th-U fuel is 13% to 15% less than that of the fuels using uranium only.

  5. Characteristics of a Mixed Thorium - Uranium Dioxide High-Burnup Fuel

    SciTech Connect

    Herring, James Stephen; Mac Donald, Philip Elsworth

    1999-06-01

    Future nuclear fuel must satisfy three sets of requirements: longer times between refueling; concerns for weapons proliferation; and development of a spent fuel form more suitable for direct geologic disposal. This project has investigated a fuel consisting of mixed thorium and uranium dioxide to satisfy these requirements. Results using the SCALE 4.3 code system indicated that the mixed Th-U fuel could be burned to 72 MWD/kg or 100 MWD/kg using 25% and 35% UO2 respectively. The uranium remained below 20 % total fissile fraction throughout the cycle, making it unusable for weapons. Total plutonium production per MWD was a factor of 4.5 less in the Th-U fuel than in the conventional fuel; Pu-239 production per MWD was a factor of 6.5 less; and the plutonium produced was high in Pu-238, leading to a decay heat 5 times greater than that from plutonium derived from conventional fuel and 40 times greater than weapons grade plutonium. High decay heat would require active cooling of any crude weapon, lest the components surrounding the plutonium be melted. Spontaneous neutron production for plutonium from Th-U fuel was 2.3 times greater than that from conventional fuel and 15 times greater than that from weapons grade plutonium. High spontaneous neutron production drastically limits the probable yield of a crude weapon. Because ThO2 is the highest oxide of thorium, while UO2 can be oxidized further to U3O8, ThO2- UO2 fuel may be a superior wasteform if the spent fuel is ever to be exposed to oxygenated water. Even if the cost of fabricating the mixed Th-U fuel is $100/kg greater, the cost of the Th-U fuel is 13% to 25% less than that of the fuels using uranium only.

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

    SciTech Connect

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

    1980-10-01

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

  7. A sequential method for the determination of 210Pb, 226Ra, and uranium and thorium radioisotopes by LSC and alpha-spectrometry.

    PubMed

    Lozano, J C; Tomé, F Vera; Rodríguez, P Blanco; Prieto, C

    2010-01-01

    A procedure for the determination of (210)Pb, and alpha-emitting radioisotopes of uranium, thorium, and radium from the same aliquot of a sample has been proposed. The key step consisted in the recovery of Pb(II) and Ra by precipitation of insoluble Pb(NO(3))(2), the uranium and thorium radioisotopes remaining in solution. Afterwards, the fractions were handled by specific, well consolidated procedures. Lead-210 was determined by the LSC technique while the uranium, thorium, and radium radioisotopes were measured with silicon alpha-spectrometers. The procedure was applied to a reference sample and several environmental samples obtaining satisfactory results.

  8. 10 CFR 40.28 - General license for custody and long-term care of uranium or thorium byproduct materials disposal...

    Code of Federal Regulations, 2014 CFR

    2014-01-01

    ... may issue a specific license, as specified in the Uranium Mill Tailings Radiation Control Act of 1978... 10 Energy 1 2014-01-01 2014-01-01 false General license for custody and long-term care of uranium... long-term care of uranium or thorium byproduct materials disposal sites. (a) A general license...

  9. 10 CFR 40.28 - General license for custody and long-term care of uranium or thorium byproduct materials disposal...

    Code of Federal Regulations, 2012 CFR

    2012-01-01

    ... may issue a specific license, as specified in the Uranium Mill Tailings Radiation Control Act of 1978... 10 Energy 1 2012-01-01 2012-01-01 false General license for custody and long-term care of uranium... long-term care of uranium or thorium byproduct materials disposal sites. (a) A general license...

  10. Electronic structure, excited states, and photoelectron spectra of uranium, thorium, and zirconium bis(Ketimido) complexes (C5R5)2M[-NCPh2]2 (M = Th, U, Zr; R = H, CH3).

    PubMed

    Clark, Aurora E; Martin, Richard L; Hay, P Jeffrey; Green, Jennifer C; Jantunen, Kimberly C; Kiplinger, Jaqueline L

    2005-06-23

    Organometallic actinide bis(ketimide) complexes (C5Me5)2An[-N=C(Ph)(R)]2 (where R = Ph, Me, and CH2Ph) of thorium(IV) and uranium(IV) have recently been synthesized that exhibit chemical, structural, and spectroscopic (UV-Visible, resonance-enhanced Raman) evidence for unusual actinide-ligand bonding. [Da Re et al., J. Am. Chem. Soc., 2005, 127, 682; Jantunen et al., Organometallics, 2004, 23, 4682; Morris et al., Organometallics, 2004, 23, 5142.] Similar evidence has been observed for the group 4 analogue (C5H5)2Zr[-N=CPh2]2. [Da Re et al., J. Am. Chem. Soc., 2005, 127, 682.] These compounds have important implications for the development of new heavy-element systems that possess novel electronic and magnetic properties. Here, we have investigated M-ketimido bonding (M = Th, U, Zr), as well as the spectroscopic properties of the highly colored bis-ketimido complexes, using density functional theory (DFT). Photoelectron spectroscopy (PES) has been used to experimentally elucidate the ground-state electronic structure of the thorium and uranium systems. Careful examination of the ground-state electronic structure, as well as a detailed modeling of the photoelectron spectra, reveals similar bonding interactions between the thorium and uranium compounds. Using time-dependent DFT (TDDFT), we have assigned the bands in the previously reported UV-Visible spectra for (C5Me5)2Th[-N=CPh2]2, (C5Me5)2U[-N=CPh2]2, and (C5H5)2Zr[-N=CPh2]2. The low-energy transitions are attributed to ligand-localized N p --> C=N pi excitations. These excited states may be either localized on a single ketimido unit or may be of the ligand-ligand charge-transfer type. Higher-energy transitions are cyclopentadienyl pi --> CN pi or cyclopentadienyl pi --> phenyl pi in character. The lowest-energy excitation in the (C5Me5)2U[-N=Ph2]2 compound is attributed to f-f and metal-ligand charge-transfer transitions that are not available in the thorium and zirconium analogues. Geometry optimization and

  11. Rapid fusion method for the determination of refractory thorium and uranium isotopes in soil samples

    SciTech Connect

    Maxwell, Sherrod L.; Hutchison, Jay B.; McAlister, Daniel R.

    2015-02-14

    Recently, approximately 80% of participating laboratories failed to accurately determine uranium isotopes in soil samples in the U.S Department of Energy Mixed Analyte Performance Evaluation Program (MAPEP) Session 30, due to incomplete dissolution of refractory particles in the samples. Failing laboratories employed acid dissolution methods, including hydrofluoric acid, to recover uranium from the soil matrix. The failures illustrate the importance of rugged soil dissolution methods for the accurate measurement of analytes in the sample matrix. A new rapid fusion method has been developed by the Savannah River National Laboratory (SRNL) to prepare 1-2 g soil sample aliquots very quickly, with total dissolution of refractory particles. Soil samples are fused with sodium hydroxide at 600 ºC in zirconium crucibles to enable complete dissolution of the sample. Uranium and thorium are separated on stacked TEVA and TRU extraction chromatographic resin cartridges, prior to isotopic measurements by alpha spectrometry on cerium fluoride microprecipitation sources. Plutonium can also be separated and measured using this method. Batches of 12 samples can be prepared for measurement in <5 hours.

  12. Rapid fusion method for the determination of refractory thorium and uranium isotopes in soil samples

    DOE PAGES

    Maxwell, Sherrod L.; Hutchison, Jay B.; McAlister, Daniel R.

    2015-02-14

    Recently, approximately 80% of participating laboratories failed to accurately determine uranium isotopes in soil samples in the U.S Department of Energy Mixed Analyte Performance Evaluation Program (MAPEP) Session 30, due to incomplete dissolution of refractory particles in the samples. Failing laboratories employed acid dissolution methods, including hydrofluoric acid, to recover uranium from the soil matrix. The failures illustrate the importance of rugged soil dissolution methods for the accurate measurement of analytes in the sample matrix. A new rapid fusion method has been developed by the Savannah River National Laboratory (SRNL) to prepare 1-2 g soil sample aliquots very quickly, withmore » total dissolution of refractory particles. Soil samples are fused with sodium hydroxide at 600 ºC in zirconium crucibles to enable complete dissolution of the sample. Uranium and thorium are separated on stacked TEVA and TRU extraction chromatographic resin cartridges, prior to isotopic measurements by alpha spectrometry on cerium fluoride microprecipitation sources. Plutonium can also be separated and measured using this method. Batches of 12 samples can be prepared for measurement in <5 hours.« less

  13. Uranium, plutonium, and thorium isotopes in the atmosphere and the lithosphere

    SciTech Connect

    Essien, I.O.

    1983-01-01

    Concentration of /sup 238/U in rain and snow collected at Fayetteville (36/sup 0/N, 94/sup 0/W), Arkansas, showed a marked increase during the summer months of 1980, while Mount St. Helens remained active. This observed increase of /sup 238/U can be explained as due to the fallout of natural uranium from the eruption of Mount St. Helens. Large increases in the concentration of thorium isotopes detected in rain and snow samples during the last months of 1982 and early months of 1983 probably originated from the eruption of El Chichon volcano, which occurred on 28 March 1982. About 450 Ci of /sup 232/Th is estimated to have been injected into the atmosphere by this eruption. Isotopic anomalies were observed in atmospheric samples such as rain and snow. These anomalies can be attributed to various natural as well as man-made sources: nuclear weapon tests, nuclear accidents involving the burn-up of nuclear powered satellites, and volcanic eruptions. The variation of /sup 234/U//sup 238/U ratios in radioactive minerals when leached with nitric acid were also noticed and this variation, while /sup 235/U//sup 238/U remained fairly constant, can be explained in terms of the ..cap alpha..-recoil effect and changes in oxidation state of uranium. Difference found in /sup 239/Pu//sup 238/U ratios in terrestrial samples and uranium minerals can be explained as due to fallout contamination.

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

    PubMed

    Fattal, Elias; Tsapis, Nicolas; Phan, Guillaume

    2015-08-01

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

  15. Uranium and thorium in the middle Precambrian Estes Conglomerate, Nemo District, Lawrence County, South Dakota: a preliminary report

    USGS Publications Warehouse

    Hills, F. Allan

    1977-01-01

    The Estes Conglomerate, which is exposed in the Nemo District on the northeastern flank of the Black Hills, South Dakota, is inferred to be of early middle Precambrian age (early Precambrian X or Paleoaphebian) and to be resting on late early Precambrian (late Precambrian W) granitic continental crust. The Estes contains beds of quartzite and quartz-pebble conglomerate (oligomictic conglomerate) with matrices of micaceous quartzite that locally contain 5 to 25 percent dispersed pyrite. Highly oxidized outcrop samples of the oligomictic conglomerate have anomalously high contents of both uranium (10 to 40 ppm) and thorium (20 to 800 ppm). High thorium values in the oligomictic conglomerate favor a placer mechanism for the concentration of radioactive minerals and appear to eliminate the possibility of epigenetic processes, such as reduction of uranium by pyrite. The presence of abundant old prospect pits and of several abandoned mines suggests that these conglomerates may also contain some gold. Early prospectors may have been attracted by the gossan produced by oxidation of pyrite. Uranium in the Estes Conglomerate may be of similar origin to the economically very important uranium deposits in the Matinenda Formation of the Elliot Lake District, Ontario. Because uranium is rapidly dissolved in acidic, oxygenated ground water, such as is present where pyrite is weathering, most of the uranium originally present in the analyzed samples has probably been leached out. Conglomerate located below the zone of weathering and oxidation has good potential for economic uranium deposits.

  16. Assessment of co-contaminant effects on uranium and thorium speciation in freshwater using geochemical modelling.

    PubMed

    Lofts, Stephen; Fevrier, Laureline; Horemans, Nele; Gilbin, Rodolphe; Bruggeman, Christophe; Vandenhove, Hildegarde

    2015-11-01

    Speciation modelling of uranium (as uranyl) and thorium, in four freshwaters impacted by mining activities, was used to evaluate (i) the influence of the co-contaminants present on the predicted speciation, and (ii) the influence of using nine different model/database combinations on the predictions. Generally, co-contaminants were found to have no significant effects on speciation, with the exception of Fe(III) in one system, where formation of hydrous ferric oxide and adsorption of uranyl to its surface impacted the predicted speciation. Model and database choice on the other hand clearly influenced speciation prediction. Complexes with dissolved organic matter, which could be simulated by three of the nine model/database combinations, were predicted to be important in a slightly acidic, soft water. Model prediction of uranyl and thorium speciation needs to take account of database comprehensiveness and cohesiveness, including the capability of the model and database to simulate interactions with dissolved organic matter. Measurement of speciation in natural waters is needed to provide data that may be used to assess and improve model capabilities and to better constrain the type of predictive modelling work presented here.

  17. Studies of the mobility of uranium and thorium in Nevada Test Site tuff

    SciTech Connect

    Wollenberg, H.A.; Flexser, S.; Smith, A.R.

    1991-06-01

    Hydro-geochemical processes must be understood if the movement of radionuclides away from a breached radioactive waste canister is to be modeled and predicted. In this respect, occurrences of uranium and thorium in hydrothermal systems are under investigation in tuff and in rhyolitic tuff that was heated to simulate the effects of introduction of radioactive waste. In these studies, high-resolution gamma spectrometry and fission-track radiography are coupled with observations of alteration mineralogy and thermal history to deduce the evidence of, or potential for movement of, U and Th in response to the thermal environment. Observations to date suggest that U was mobile in the vicinity of the heater but that localized reducing environments provided by Fe-Ti-Mn-oxide minerals concentrated U and thus attenuated its migration.

  18. Technogenic Fallout of Uranium and Thorium in the Vicinity of Novosibirsk (Russia, West Siberia)

    NASA Astrophysics Data System (ADS)

    Artamonova, Svetlana Yu.

    Evaluation of the contribution of definite pollution sources among many others is rather complicated scientific challenge, but its solution may become decisive for the realization of measures aimed at ecological remediation of the territories. Element composition of aerosol particles accumulated during winter in the snow cover of Novosibirsk was determined by means of X-ray fluorescence measurements with synchrotron radiation at the "Siberian Synchrotron and Terahertz Radiation Center" based on VEPP-3 of the Budker Institute of Nuclear Physics SB RAS. Means of ICP-MS and scanning electron microscopy were used additionally. These studies allowed revealing the contribution of separate industrial enterprises into the general technogenic pollution of the megapolis with uranium and thorium.

  19. Reaction of active uranium and thorium with aromatic carbonyls and pinacols in hydrocarbon solvents

    SciTech Connect

    Kahn, B.E.; Rieke, R.D.

    1988-02-01

    Highly reactive uranium and thorium metal powders have been prepared by reduction of the anhydrous metal(IV) chlorides in hydrocarbon solvents. The reduction employs the crystalline hydrocarbon-soluble reducing agent ((TMEDA)Li)/sub 2/(Nap) (TMEDA = N,N,N',N'-tetramethylethylenediamine, Nap = naphthalene). The resulting active metal powders have been shown to be extremely reactive with oxygen-containing compounds and have been used in the reductive coupling of aromatic ketones giving tetra-arylethylenes. Reactions with pinacols have given some mechanistic insight into the ketone coupling reaction. These finely divided metal powders activate very weakly acidic C-H bonds forming metal hydrides, which can be transferred to organic substrates.

  20. Sorption and coprecipitation of trace concentrations of thorium with various minerals under conditions simulating an acid uranium mill effluent environment

    USGS Publications Warehouse

    Landa, Edward R.; Le, Anh H.; Luck, Rudy L.; Yeich, Philip J.

    1995-01-01

    Sorption of thorium by pre-existing crystals of anglesite (PbSO4), apatite (Ca5(PO4)3(HO)), barite (BaSO4), bentonite (Na0.7Al3.3Mg0.7Si8O20(OH)4), celestite (SrSO4), fluorite (CaF2), galena (PbS), gypsum (CaSO4·2H2O), hematite (Fe2O3), jarosite (KFe3(SO4)2(OH)6), kaolinite (Al2O3·2SiO2·2H2O), quartz (SiO2) and sodium feldspar (NaAlSi3O8) was studied under conditions that simulate an acidic uranium mill effluent environment. Up to 100% removal of trace quantitiees of thorim (approx. 1.00 ppm in 0.01 N H2SO4) from solution occurred within 3 h with fluorite and within 48 h in the case of bentonite. Quartz, jarosite, hematite, sodium feldspar, gypsum and galena removed less than 15% of the thorium from solution. In the coprecipitation studies, barite, anglesite, gypsum and celestite were formed in the presence of thorium (approx. 1.00 ppm). Approximately all of the thorium present in solution coprecipitated with barite and celestite; 95% coprecipitated with anglesite and less than 5% with gypsum under similar conditions. When jarosite was precipitated in the presence of thorium, a significant amount of thorium (78%) was incorporated in the precipitate.

  1. 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.

  2. Feasibility study on AFR-100 fuel conversion from uranium-based fuel to thorium-based fuel

    SciTech Connect

    Heidet, F.; Kim, T.; Grandy, C.

    2012-07-30

    Although thorium has long been considered as an alternative to uranium-based fuels, most of the reactors built to-date have been fueled with uranium-based fuel with the exception of a few reactors. The decision to use uranium-based fuels was initially made based on the technology maturity compared to thorium-based fuels. As a result of this experience, lot of knowledge and data have been accumulated for uranium-based fuels that made it the predominant nuclear fuel type for extant nuclear power. However, following the recent concerns about the extent and availability of uranium resources, thorium-based fuels have regained significant interest worldwide. Thorium is more abundant than uranium and can be readily exploited in many countries and thus is now seen as a possible alternative. As thorium-based fuel technologies mature, fuel conversion from uranium to thorium is expected to become a major interest in both thermal and fast reactors. In this study the feasibility of fuel conversion in a fast reactor is assessed and several possible approaches are proposed. The analyses are performed using the Advanced Fast Reactor (AFR-100) design, a fast reactor core concept recently developed by ANL. The AFR-100 is a small 100 MW{sub e} reactor developed under the US-DOE program relying on innovative fast reactor technologies and advanced structural and cladding materials. It was designed to be inherently safe and offers sufficient margins with respect to the fuel melting temperature and the fuel-cladding eutectic temperature when using U-10Zr binary metal fuel. Thorium-based metal fuel was preferred to other thorium fuel forms because of its higher heavy metal density and it does not need to be alloyed with zirconium to reduce its radiation swelling. The various approaches explored cover the use of pure thorium fuel as well as the use of thorium mixed with transuranics (TRU). Sensitivity studies were performed for the different scenarios envisioned in order to determine the

  3. Inductive cold crucible melting and characterization of uranium and thorium bearing murataite ceramics

    SciTech Connect

    Knyazev, O.A.; Stefanovsky, S.V.; Ptashkin, A.G.; Zen'kovskaya, M.A.

    2007-07-01

    Murataite-based ceramics containing 10 wt.% either UO{sub 2} or ThO{sub 2} were produced by inductive cold crucible melting (ICCM) at operating frequencies of 1.76 MHz and 5.28 MHz and examined using X-ray diffraction and scanning and transmission electron microscopy. High specific productivity was achieved. Average melting ratio was 8.3 kWh/kg. We identified three distinct murataite polytypes in the U-bearing ceramics: a five- (5C), eight- (8C), and three-fold (3C) fluorite unit cell composing respectively the core, intermediate and rim zones of the grains. In contrast, in the Th-bearing ceramic one of the polytypes with eight-fold (8C) fluorite unit cell was found to be prevailing over two others (5C and 3C). Computer simulation of the major reflection due to the murataite phase in the Th-bearing sample also exhibits superposition of peaks due to three distinct polytypes but one of them (8C) is predominant. The core zone of the murataite in the U-bearing specimens is characterized by UO{sub 2} concentrations as high as 12.1 wt%, which successively diminishes in concentration through the intermediate zone to the rim, the latter of which contains 5.2 wt% UO{sub 2}. Thorium distribution within the murataite crystals is more uniform. The other phases found in the ceramics are crichtonite, rutile and traces of perovskite, Fe/Mn titanate ilmenite/pyrophanite, zirconolite, and vitreous phase. The difference in phase composition and actinide partitioning in the ceramics is influenced by synthesis conditions. Thus, application of large-scale cold crucibles is a prospective route for the development of industrial-scale process and technology for ceramization of actinide-bearing HLW. The advantage of this method is production of zoned crystals with the highest concentrations of actinides and rare earth elements in the core, effectively isolating these elements from potential leach solutions. (authors)

  4. 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.

  5. 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.

  6. Aqueous biphasic extraction of uranium and thorium from contaminated soils. Final report

    SciTech Connect

    Chaiko, D.J.; Gartelmann, J.; Henriksen, J.L.; Krause, T.R.; Deepak; Vojta, Y.; Thuillet, E.; Mertz, C.J.

    1995-07-01

    The aqueous biphasic extraction (ABE) process for soil decontamination involves the selective partitioning of solutes and fine particulates between two immiscible aqueous phases. The biphase system is generated by the appropriate combination of a water-soluble polymer (e.g., polyethlene glycol) with an inorganic salt (e.g., sodium carbonate). Selective partitioning results in 99 to 99.5% of the soil being recovered in the cleaned-soil fraction, while only 0.5 to 1% is recovered in the contaminant concentrate. The ABE process is best suited to the recovery of ultrafine, refractory material from the silt and clay fractions of soils. During continuous countercurrent extraction tests with soil samples from the Fernald Environmental Management Project site (Fernald, OH), particulate thorium was extracted and concentrated between 6- and 16-fold, while the uranium concentration was reduced from about 500 mg/kg to about 77 mg/kg. Carbonate leaching alone was able to reduce the uranium concentration only to 146 mg/kg. Preliminary estimates for treatment costs are approximately $160 per ton of dry soil. A detailed flowsheet of the ABE process is provided.

  7. Radioactive waste forms stabilized by ChemChar gasification: characterization and leaching behavior of cerium, thorium, protactinium, uranium, and neptunium.

    PubMed

    Marrero, T W; Morris, J S; Manahan, S E

    2004-02-01

    The uses of a thermally reductive gasification process in conjunction with vitrification and cementation for the long-term disposal of low level radioactive materials have been investigated. gamma-ray spectroscopy was used for analysis of carrier-free protactinium-233 and neptunium-239 and a stoichiometric amount of cerium (observed cerium-141) subsequent to gasification and leaching, up to 48 days. High resolution ICP-MS was used to analyze the cerium, thorium, and uranium from 46 to 438 days of leaching. Leaching procedures followed the guidance of ASTM Procedure C 1220-92, Standard Test Method for Static Leaching of Monolithic Waste Forms for Disposal of Radioactive Waste. The combination of the thermally reductive pretreatment, vitrification and cementation produced a highly non-leachable form suitable for long-term disposal of cerium, thorium, protactinium, uranium, and neptunium.

  8. Environmental releases from fuel cycle facility: part 1: radionuclide resuspension vs. stack releases on ambient airborne uranium and thorium levels.

    PubMed

    Masson, Olivier; Pourcelot, Laurent; Boulet, Béatrice; Cagnat, Xavier; Videau, Gérard

    2015-03-01

    Airborne activity levels of uranium and thorium series were measured in the vicinity (1.1 km) of a uranium (UF4) processing plant, located in Malvési, south of France. Regarding its impact on the environment, this facility is characterized by its routine atmospheric releases of uranium and by the emission of radionuclide-labelled particles from a storage pond filled with waste water or that contain dried sludge characterized by traces of plutonium and thorium ((230)Th). This study was performed during a whole year (November 2009-November 2010) and based on weekly aerosol sampling. Thanks to ICP-MS results, it was possible to perform investigations of uranium and thorium decay product concentration in the air. The number of aerosol filters sampled (50) was sufficient to establish a relationship between airborne radionuclide variations and the wind conditions. As expected, the more the time spent in the plume, the higher the ambient levels. The respective contributions of atmospheric releases and resuspension from local soil and waste ponds on ambient dust load and uranium-bearing aerosols were estimated. Two shutdown periods dedicated to facility servicing made it possible to estimate the resuspension contribution and to specify its origin (local or regional) according to the wind direction and remote background concentration. Airborne uranium mainly comes from the emission stack and, to a minor extent (∼20%), from wind resuspension of soil particles from the surrounding fields and areas devoted to waste storage. Moreover, weighed activity levels were clearly higher during operational periods than for shutdown periods.

  9. Screening of plant species for phytoremediation of uranium, thorium, barium, nickel, strontium and lead contaminated soils from a uranium mill tailings repository in South China.

    PubMed

    Li, Guang-yue; Hu, Nan; Ding, De-xin; Zheng, Ji-fang; Liu, Yu-long; Wang, Yong-dong; Nie, Xiao-qin

    2011-06-01

    The concentrations of uranium, thorium, barium, nickel, strontium and lead in the samples of the tailings and plant species collected from a uranium mill tailings repository in South China were analyzed. Then, the removal capability of a plant for a target element was assessed. It was found that Phragmites australis had the greatest removal capabilities for uranium (820 μg), thorium (103 μg) and lead (1,870 μg). Miscanthus floridulus had the greatest removal capabilities for barium (3,730 μg) and nickel (667 μg), and Parthenocissus quinquefolia had the greatest removal capability for strontium (3,920 μg). In this study, a novel coefficient, termed as phytoremediation factor (PF), was proposed, for the first time, to assess the potential of a plant to be used in phytoremediation of a target element contaminated soil. Phragmites australis has the highest PFs for uranium (16.6), thorium (8.68), barium (10.0) and lead (10.5). Miscanthus floridulus has the highest PF for Ni (25.0). Broussonetia papyrifera and Parthenocissus quinquefolia have the relatively high PFs for strontium (28.1 and 25.4, respectively). On the basis of the definition for a hyperaccumulator, only Cyperus iria and Parthenocissus quinquefolia satisfied the criteria for hyperaccumulator of uranium (36.4 μg/g) and strontium (190 μg/g), and could be the candidates for phytoremediation of uranium and strontium contaminated soils. The results show that the PF has advantage over the hyperaccumulator in reflecting the removal capabilities of a plant for a target element, and is more adequate for assessing the potential of a plant to be used in phytoremediation than conventional method.

  10. 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.

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

    SciTech Connect

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

    2012-06-18

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

  12. Matrix infrared spectroscopic and density functional theoretical investigations on thorium and uranium atom reactions with dimethyl ether.

    PubMed

    Gong, Yu; Andrews, Lester

    2011-11-14

    Reactions of laser-ablated thorium and uranium atoms with dimethyl ether were investigated using matrix isolation infrared spectroscopy. Four types of reaction products for both uranium and thorium were identified using deuterium substituted samples as well as density functional frequency and energy calculations. Ground state uranium and thorium atoms react with dimethyl ether spontaneously to give the M(CH(3)OCH(3)) complexes (M = Th, U) on annealing, which are predicted to have C(2v) symmetry with triplet (Th) and quintet (U) ground states. Subsequent visible irradiation produces the divalent CH(3)OThCH(3) and CH(3)OUCH(3) insertion products with singlet and quintet states lowest in energy. Further UV irradiation induces isomerization of the CH(3)OMCH(3) molecules to the (CH(3))(2)MO isomers with M=O double bonds and pyramidal structures. In the presence of another dimethyl ether reagent, evidence for (CH(3)O)(2)M(CH(3))(2) molecules is also produced upon UV irradiation.

  13. A procedural manual for measurement of uranium and thorium isotopes utilizing the USGS-Stanford Finnegan Mat 262

    USGS Publications Warehouse

    Shamp, Donald D.

    2001-01-01

    Over the past several decades investigators have extensively examined the 238U-234U- 230Th systematics of a variety of geologic materials using alpha spectroscopy. Analytical uncertainty for 230Th by alpha spectroscopy has been limited to about 2% (2σ). The advantage of thermal ionization mass spectroscopy (TIMS), introduced by Edwards and co-workers in the late 1980’s is the increased detectability of these isotopes by a factor of ~200, and decreases in the uncertainty for 230Th to about 5‰ (2σ) error. This report is a procedural manual for using the USGS-Stanford Finnegan-Mat 262 TIMS to collect and isolate Uranium and Thorium isotopic ratio data. Chemical separation of Uranium and Thorium from the sample media is accomplished using acid dissolution and then processed using anion exchange resins. The Finnegan-Mat262 Thermal Ionization Mass Spectrometer (TIMS) utilizes a surface ionization technique in which nitrates of Uranium and Thorium are placed on a source filament. Upon heating, positive ion emission occurs. The ions are then accelerated and focused into a beam which passes through a curved magnetic field dispersing the ions by mass. Faraday cups and/or an ion counter capture the ions and allow for quantitative analysis of the various isotopes.

  14. Distribution of uranium and thorium in dolomitic gravel fill and shale saprolite.

    PubMed

    Phillips, D H; Watson, D B

    2015-03-21

    The objectives of this study were to examine (1) the distribution of U and Th in dolomitic gravel fill and shale saprolite, and (2) the removal of uranium from acidic groundwater by dolomitic gravel through precipitation with amorphous basaluminite at the U.S. DOE Oak Ridge Integrated Field Research Challenge (ORIFRC) field site west of the Oak Ridge Y-12 National Security Complex in East Tennessee. Media reactivity and sustainability are a technical concern with the deployment of any subsurface reactive media. Because the gravel was placed in the subsurface and exposed to contaminated groundwater for over 20 years, it provided a unique opportunity to study the solid and water phase geochemical conditions within the media after this length of exposure. This study illustrates that dolomite gravel can remove U from acidic contaminated groundwater with high levels of Al(3+), Ca(2+), NO(3-), and SO4(2-) over the long term. As the groundwater flows through high pH carbonate gravel, U containing amorphous basaluminite precipitates as the pH increases. This is due to an increase in groundwater pH from 3.2 to ∼6.5 as it comes in contact with the gravel. Therefore, carbonate gravel could be considered as a possible treatment medium for removal and sequestration of U and other pH sensitive metals from acidic contaminated groundwater. Thorium concentrations are also high in the carbonate gravel. Thorium generally shows an inverse relationship with U from the surface down into the deeper saprolite. Barite precipitated in the shallow saprolite directly below the dolomitic gravel from barium present in the acidic contaminated groundwater.

  15. Distribution of uranium and thorium in groundwater of arid climate region

    NASA Astrophysics Data System (ADS)

    Murad, Ahmed; Alshamsi, Dalal; Aldahan, Ala; Hou, Xiaolin

    2014-05-01

    Uranium, thorium and their decay products are the most common radionuclides in groundwater in addition to potassium-40. Once groundwater is used for drinking, domestic and irrigation purposes, the radionuclides will then pose environmental and health related hazard originating from radioactivity and toxicity. In the investigation presented here, assessment of 238U, 235U and 232Th concentrations in groundwater across of the United Arab Emirates (UAE) is evaluated in terms of quality and sources. The region is dominated by arid climate conditions and radioactivity assessment of groundwater is essential for safe use of groundwater. Furthermore, the results were linked to data from other arid regions and worldwide. Groundwater samples (total dissolved solids,TDS, 142.5 mg L-1 to 12770 mg L-1) from 67 different wells were collected across geomorphologically different areas and most of the wells are actively used for agriculture. The aquifers are recent sand dunes, Quaternary (3 million years to present) sediments, and older carbonate rocks (230-10 million years). The 235U, 238U and 232Th measurements were carried out using ICP-MS system equipped with an Xt-skimmer cone and a concentric nebulizer under hot plasma conditions. Concentrations of 235U, 238U and 232Th range at (0.125-508.4) ng L-1, (25.81-69237) ng L-1 and (0.236-2529) ng L-1, respectively. Apparently, most 235U, 238U, 232Th concentrations in the sampled groundwater are below the WHO proposed permissible level of 60000 ng/L for total uranium (1 Bq L-1 for 235U and 10 Bq L-1 for 238U) and 5000 ng L-1 (1Bq L-1) for 232Th. A few samples show high concentrations of uranium that are associated with high TDS values and occur within interbedded limestones and shales aquifer. Comparison with worldwide groundwater data suggests that 238U concentration is highest in the arid regions groundwater where the recharge to aquifers is relatively low. The situation for 232Th concentrations seems less affected by climatic

  16. Third minima in thorium and uranium isotopes in a self-consistent theory

    NASA Astrophysics Data System (ADS)

    McDonnell, J. D.; Nazarewicz, W.; Sheikh, J. A.

    2013-05-01

    Background: Well-developed third minima, corresponding to strongly elongated and reflection-asymmetric shapes associated with dimolecular configurations, have been predicted in some non-self-consistent models to impact fission pathways of thorium and uranium isotopes. These predictions have guided the interpretation of resonances seen experimentally. On the other hand, self-consistent calculations consistently predict very shallow potential-energy surfaces in the third minimum region.Purpose: We investigate the interpretation of third-minimum configurations in terms of dimolecular (cluster) states. We study the isentropic potential-energy surfaces of selected even-even thorium and uranium isotopes at several excitation energies. In order to understand the driving effects behind the presence of third minima, we study the interplay between pairing and shell effects.Methods: We use the finite-temperature superfluid nuclear density functional theory. We consider two Skyrme energy density functionals: a traditional functional SkM* and a recent functional UNEDF1 optimized for fission studies.Results: We predict very shallow or no third minima in the potential-energy surfaces of 232Th and 232U. In the lighter Th and U isotopes with N=136 and 138, the third minima are better developed. We show that the reflection-asymmetric configurations around the third minimum can be associated with dimolecular states involving the spherical doubly magic 132Sn and a lighter deformed Zr or Mo fragment. The potential-energy surfaces for 228,232Th and 232U at several excitation energies are presented. We also study isotopic chains to demonstrate the evolution of the depth of the third minimum with neutron number.Conclusions: We show that the neutron shell effect that governs the existence of the dimolecular states around the third minimum is consistent with the spherical-to-deformed shape transition in the Zr and Mo isotopes around N=58. We demonstrate that the depth of the third minimum

  17. National Uranium-Resource Evaluation: genesis of the Bokan Mountain, Alaska uranium-thorium deposits

    SciTech Connect

    Thompson, T.B.; Lyttle, T.; Pierson, J.R.

    1980-01-01

    The objective of this research project is to develop a model that can be used in evaluating peralkaline granitic-syenitic rocks for uranium potential. The deposits at Bokan Mountain (also known as Kendrick Bay) were studied to generate a specific model as to their mode of formation. To achieve the objective several types of data have been obtained: (1) Distinction by mapping and core logging of multiple intrusive phases within the Bokan Mountain Granite complex; (2) Detailed chemical and petrographic data on each igneous phase; (3) Extent of and mineralogical/chemical characteristics of the associated wallrock alteration; (4) Radiometric dates on magmatic and hydrothermal products; (5) Fluid inclusion analysis of quartz, calcite, and fluorite from mineralized rock; (6) Ore and sulfide mineralogy; (7) C, O, and S isotope analyses of minerals from mineralized rock; (8) Trace element dispersion with respect to mineralized zones; and (9) Structural data for interpretation of emplacement mechanisms as well as post-magmatic events important to ore localization. The U/Th mineralization is localized in shear zones as vein-like bodies or in irregular cylindrical bodies formed by concentrations of microfractures. The ore zones are localized within or on top of syenitic masses and have intense albitization and chloritization, with subordinate amounts of calcite, fluorite, quartz, sulfides, and tourmaline. Hematite occurs peripherally to the higher-grade ore zones. Uranothrorite and uraninite are the main ore minerals.

  18. Improving Natural Uranium Utilization By Using Thorium in Low Moderation PWRs - A Preliminary Neutronic Scoping Study

    SciTech Connect

    Gilles Youinou; Ignacio Somoza

    2010-10-01

    The Th-U fuel cycle is not quite self-sustainable when used in water-cooled reactors and with fuel burnups higher than a few thousand of MWd/t characteristic of CANDU reactors operating with a continuous refueling. For the other industrially mature water-cooled reactors (i.e. PWRs and BWRs) it is economically necessary that the fuel has enough reactivity to reach fuel burnups of the order of a few tens of thousand of MWd/t. In this particular case, an additional input of fissile material is necessary to complement the bred fissile U-233. This additional fissile material could be included in the form of Highly Enriched Uranium (HEU) at the fabrication of the Th-U fuel. The objective of this preliminary neutronic scoping study is to determine (1) how much HEU and, consequently, how much natural uranium is necessary in such Th-U fuel cycle with U recycling and (2) how much TRansUranics (TRU=Pu, Np, Am and Cm) are produced. These numbers are then compared with those of a standard UO2 PWR. The thorium reactors considered have a homogeneous hexagonal lattice made up of the same (Th-U)O2 pins. Furthermore, at this point, we are not considering the use of blankets inside or outside the core. The lattice pitch has been varied to estimate the effect of the water-to-fuel volume ratio, and light water as well as heavy water have been considered. For most cases, an average burnup at discharge of 45,000 MWd/t has been considered.

  19. 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.

  20. Fluxes of uranium and thorium series isotopes in the Santa Barbara Basin

    NASA Astrophysics Data System (ADS)

    Moore, Willard S.; Bruland, Kenneth W.; Michel, Jacqueline

    1981-05-01

    Samples from the MANOP Santa Barbara Basin sediment trap intercomparison were analyzed for the isotopes of uranium, thorium, radium, lead, and polonium. All of the traps showed approximately the same compositions and isotopic ratios, indicating that they trapped similar materials. The 234Th flux via falling particles was very close to the flux predicted from the production and scavenging rates of 234Th from the water column. The 210Pb content of the trapped particles and the surface sediments were the same, however, the measured flux of 210Pb was seven times greater than the predicted flux. Predicted and measured fluxes of 228Th and 210Po were similarly out of balance. To explain this apparent inconsistency, we suggest (as others have done) that the Santa Barbara Basin is an area where scavenging from the water column is intensified and where sediments deposited initially on the margins may be physically remobilized on a short time scale. These two effects increase the apparent area from which the basin derives the longer-lived isotopes but does not increase significantly the supply of the short-lived 234Th.

  1. Distributions of selenium, iodine, lead, thorium and uranium in Japanese river waters

    SciTech Connect

    Tagami, K.; Uchida, S.

    2007-07-01

    Long-lived radionuclides released from nuclear facilities, such as deep underground disposal facilities, could reach humans through several transfer paths in the environment. Uses of ground water and river water for agricultural field irrigation and for drinking water are important paths. In order to understand behavior of long-lived radionuclides in the terrestrial water environment, we carried out a natural analogue study, that is, measurement of selenium (Se), iodine (I), lead (Pb), thorium (Th) and uranium (U) concentrations in 45 Japanese rivers at 10 sampling points from the upper stream to the river mouth for each river. Geometric mean concentrations for Se, I, Pb, Th and U were 0.057, 1.4, 0.039, 0.0055, 0.0109 ng/mL, respectively. Distribution patterns from upper stream to river mouth were different by elements, for instance, the concentrations of I, Th and U increased when the sampling points were nearer the river mouth, while that of Se were almost constant. For Pb, the highest value was observed in the middle part of each river in many cases. (authors)

  2. Uranium and thorium adsorption from aqueous solution using a novel polyhydroxyethylmethacrylate-pumice composite.

    PubMed

    Akkaya, Recep

    2013-06-01

    Poly(hydroxyethylmethacrylate-pumice), [P(HEMA-Pum)], composite was synthesized by free radical polymerization in aqueous solution. The adsorptive features of P(HEMA-Pum) composite were investigated for UO2(2+) and Th(4+) using a range of pH, concentration, time (kinetics), temperature (thermodynamics), ionic strength and selectivity, and the related parameters were derived from the obtained results. These results indicated that all adsorbents had high affinity to the uranium and thorium ions. The parameters obtained from Langmuir, Freundlich and Dubinin-Radsushkevich models fit the data well. The values of enthalpy and entropy changes showed that the overall adsorption process was endothermic (ΔH > 0) and increasing entropy (ΔS > 0), and it was spontaneous (ΔG < 0) as expected. The adsorption kinetics following the pseudo-second order model indicated that the rate-controlling step was chemical adsorption that occurred by ion exchange process. Reusability of P(HEMA-Pum) was also investigated, and it was found that the composite could be used at least 5 times.

  3. Melting of the Earth's lithospheric mantle inferred from protactinium-thorium-uranium isotopic data

    PubMed

    Asmerom; Cheng; Thomas; Hirschmann; Edwards

    2000-07-20

    The processes responsible for the generation of partial melt in the Earth's lithospheric mantle and the movement of this melt to the Earth's surface remain enigmatic, owing to the perceived difficulties in generating large-degree partial melts at depth and in transporting small-degree melts through a static lithosphere. Here we present a method of placing constraints on melting in the lithospheric mantle using 231Pa-235U data obtained from continental basalts in the southwestern United States and Mexico. Combined with 230Th-238U data, the 231Pa-235U data allow us to constrain the source mineralogy and thus the depth of melting of these basalts. Our analysis indicates that it is possible to transport small melt fractions--of the order of 0.1%--through the lithosphere, as might result from the coalescence of melt by compaction owing to melting-induced deformation. The large observed 231Pa excesses require that the timescale of melt generation and transport within the lithosphere is small compared to the half-life of 231Pa (approximately 32.7 kyr). The 231Pa-230Th data also constrain the thorium and uranium distribution coefficients for clinopyroxene in the source regions of these basalts to be within 2% of one another, indicating that in this setting 230Th excesses are not expected during melting at depths shallower than 85 km.

  4. Evaluation of Ultra-Low Background Materials for Uranium and Thorium Using ICP-MS

    SciTech Connect

    Hoppe, Eric W.; Overman, Nicole R.; LaFerriere, Brian D.

    2013-08-08

    An increasing number of physics experiments require low background materials for their construction. The presence of Uranium and Thorium and their progeny in these materials present a variety of unwanted background sources for these experiments. The sensitivity of the experiments continues to drive the necessary levels of detection ever lower as well. This requirement for greater sensitivity has rendered direct radioassay impractical in many cases requiring large quantities of material, frequently many kilograms, and prolonged counting times, often months. Other assay techniques have been employed such as Neutron Activation Analysis but this requires access to expensive facilities and instrumentation and can be further complicated and delayed by the formation of unwanted radionuclides. Inductively Coupled Plasma Mass Spectrometry (ICP-MS) is a useful tool and recent advancements have increased the sensitivity particularly in the elemental high mass range of U and Th. Unlike direct radioassay, ICP-MS is a destructive technique since it requires the sample to be in liquid form which is aspirated into a high temperature plasma. But it benefits in that it usually requires a very small sample, typically about a gram. Here we will discuss how a variety of low background materials such as copper, polymers, and fused silica are made amenable to ICP-MS assay and how the arduous task of maintaining low backgrounds of U and Th is achieved.

  5. Evaluation of ultra-low background materials for uranium and thorium using ICP-MS

    SciTech Connect

    Hoppe, E. W.; Overman, N. R.; LaFerriere, B. D.

    2013-08-08

    An increasing number of physics experiments require low background materials for their construction. The presence of Uranium and Thorium and their progeny in these materials present a variety of unwanted background sources for these experiments. The sensitivity of the experiments continues to drive the necessary levels of detection ever lower as well. This requirement for greater sensitivity has rendered direct radioassay impractical in many cases requiring large quantities of material, frequently many kilograms, and prolonged counting times, often months. Other assay techniques have been employed such as Neutron Activation Analysis but this requires access to expensive facilities and instrumentation and can be further complicated and delayed by the formation of unwanted radionuclides. Inductively Coupled Plasma Mass Spectrometry (ICP-MS) is a useful tool and recent advancements have increased the sensitivity particularly in the elemental high mass range of U and Th. Unlike direct radioassay, ICP-MS is a destructive technique since it requires the sample to be in liquid form which is aspirated into a high temperature plasma. But it benefits in that it usually requires a very small sample, typically about a gram. This paper discusses how a variety of low background materials such as copper, polymers, and fused silica are made amenable to ICP-MS assay and how the arduous task of maintaining low backgrounds of U and Th is achieved.

  6. 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.

  7. Is daughter better than parent? A case study: Radon vs Uranium - Actinides for understanding Earthquake Physics -

    NASA Astrophysics Data System (ADS)

    Plastino, W.; Povinec, P.; Ermes Collaboration

    2011-12-01

    The ability to predict earthquakes is one of the greatest challenges for the Earth Sciences. Radon has been suggested as one possible precursor, and its groundwater anomalies associated with earthquakes and water-rock interactions were proposed in several seismogenic areas worldwide as due to crustal gas fluxes along active faults. However, the use of radon as possible earthquake's precursor is not clearly linked to crustal deformation. Here we show that uranium groundwater anomalies, which were observed in cataclastic rocks crossing the underground Gran Sasso National Laboratory (LNGS), can be used as possible precursor of earthquakes in domains where continental lithosphere is subducted. Measurements evidence clear, sharp anomalies from July, 2008 to the end of March, 2009, related to a preparation phase of the seismic swarm, which occurred near L'Aquila, Italy, from October, 2008 to April, 2009. On April 6th, 2009 an earthquake (Mw=6.3) occurred on 01:33 UT at the same area. About four years uranium groundwater monitoring at LNGS will be discussed as well as the role of actinides for understanding earthquake physics and new methodological and experimental procedures developed in the framework of the experiment ERMES (Environmental Radioactivity Monitoring for Earth Sciences): a perfect synergy between deep underground environment and groundwater for probing Earth's interior. Prof. Wolfango Plastino Scientific Coordinator and Spokesperson of the experiment ERMES (Environmental Radioactivity Monitoring for Earth Sciences) Italian National Institute of Nuclear Physics Gran Sasso National Laboratory

  8. Specific sequestering agents for the actinides. VI. Synthetic and structural chemistry of tetrakis(N-alkylalkanehydroxamato)thorium(IV) complexes

    SciTech Connect

    Smith, W.L.; Raymond, K.N.

    1981-06-17

    Hydroxamate complexes of the actinides have been investigated as structural archetypes in the design of actinide-specific sequestering agents. The complexes Th((CH/sub 3/)/sub 2/CHN(O)O(O)R)/sub 4/ have been prepared (R = C(CH/sub 3/)/sub 3/ (1) or CH/sub 2/C(CH/sub 3/)/sub 3/ (2) The uranium(IV) analogue of 1 was also prepared. The tert-butyl groups of 1 dominate the stereochemistry of the complex by assuming a tetrahedral disposition around the metal. The coordination polyhedron of 1, which has 4 (S/sub 4/) crystallographic symmetry, is nearly cubic. The localization of charge on the nitrogen oxygen of the hydroxamate group makes this ligand unsymmetrical, and this gives rise to a 0.14-A difference in R(Th-O/sub N/) (2.357(3) A) and R(Th-O/sub C/) (2.492 (3) A). The sterically less constrained neopentyl derivative 2 shows a more typical eight-coordinate geometry - the D/sub 2d/ trigonal-faced (mmmm) dodecahedron. The average R(Th-O/sub N/) (2.36 (1) A) is again shorter than R(Th-O/sub C/) (2.46 (2) A). There is apparently no sorting of sites by ligand charge, since the O/sub N/ and O/sub C/ atoms are equally distributed between the A and B sites of the dodecahedron. Crystals of 1 conform to space group I4/sub 1//a with a = 17.338 (4) A and c = 12.706 (4) A. For 4 formula units per cell the calculated density d/sub calcd/ is 1.50 g cm/sup -3/ and d/sub obsd/ is 1.50 (1) g cm/sup -3/. Crystals of 2 conform to space group P1 with a = 9.777 (2) A, b = 14.633 (2) A, c = 18.515 (1) A, ..cap alpha.. = 74.061/sub 0/ (8), ..beta.. = 88.41 (1)/sup 0/, and ..gamma.. = 74.71 (2)/sup 0/. For 2 formula units per cell d/sub calcd/ = 1.30 g cm/sup -3/ and d/sub obsd/ = 1.19 g cm/sup -3/. Full-matrix least-squares refinement of both structures using all averaged, independent data with F/sup 2/ > 3sigma(F)/sup 2/ gave for 1 with 1798 data and 117 variables R = 0.027 and R/sub w/ = 0.032 and for 2 with 6978 data and 467 variables R = 0.034, R/sub w/ = 0.042. 10 figures, 11 tables.

  9. Uranium and thorium behavior in groundwater of the natural spa area “Choygan mineral water” (East Tuva)

    NASA Astrophysics Data System (ADS)

    Kopylova, Y.; Guseva, N.; Shestakova, A.; Khvaschevskaya, A.; Arakchaa, K.

    2015-11-01

    The natural spa area “Choygan mineral waters”, a unique deposit of natural carbon dioxide mineral waters in Siberia, is located in the Eastern Sayan Mountains. There are 33 spring discharges in this area. Spring waters are mainly of HCO3-Na-Ca type. TDS varies from 300 mg/L to 2600 mg/L, the temperature ranges from 7 °C (in spring 33) to 39 °C (in spring 12), pH varies from 5.9 to 8.3, and the value of the oxidation-reduction potential is from -170 mV to 236 mV. All studied waters were divided into two groups according to their temperature and geochemical conditions: cold fresh water in oxidizing environment and warm slightly brackish water in reducing environment. The uranium concentration varies from 0.7 to 14 μg/l and the thorium concentration varies from 0.001 to 0.33 μg/l in the studied waters. The predominant uranium complexes are (UO2(CO3)3)4-, (UO2(CO3)2)2-, UO2CO3, (UO2(PO4)2)4- in the waters in oxidizing and reducing environments. It was found that acid-alkaline and oxidizing-reducing conditions were the determining factors for uranium behavior and speciation in the studied waters. The pH conditions are determining factors for thorium behavior and speciation in the studied waters. In slightly acidic water the predominant thorium species is negatively charge complex (ThCO3(OH)3)- (more than 95%).

  10. Polyacrylamide-hydroxyapatite composite: Preparation, characterization and adsorptive features for uranium and thorium

    SciTech Connect

    Baybas, Demet; Ulusoy, Ulvi

    2012-10-15

    The composite of synthetically produced hydroxyapatite (HAP) and polyacrylamide was prepared (PAAm-HAP) and characterized by BET, FT-IR, TGA, XRD, SEM and PZC analysis. The adsorptive features of HAP and PAAm-HAP were compared for UO{sub 2}{sup 2+} and Th{sup 4+}. The entrapment of HAP into PAAm-HAP did not change the structure of HAP. Both structures had high affinity to the studied ions. The adsorption capacity of PAAm-HAP was than that of HAP. The adsorption dependence on pH and ionic intensity provided supportive evidences for the effect of complex formation on adsorption process. The adsorption kinetics was well compatible to pseudo second order model. The values of enthalpy and entropy changes were positive. Th{sup 4+} adsorption from the leachate obtained from a regional fluorite rock confirmed the selectivity of PAAm-HAP for this ion. In consequence, PAAm-HAP should be considered amongst favorite adsorbents for especially deposition of nuclear waste containing U and Th, and radionuclide at secular equilibrium with these elements. - Graphical abstract: SEM images of hydroxyapatite (HAP) and polyacrylamide-hydroxyapatite (PAAm-HAP), and the adsorption isotherms for Uranium and Thorium. Highlights: Black-Right-Pointing-Pointer Composite of PAAm-HAP was synthesized from hydroxyapatite and polyacrylamide. Black-Right-Pointing-Pointer The materials were characterized by BET, FT-IR, XRD, SEM, TGA and PZC analysis. Black-Right-Pointing-Pointer HAP and PAAm-HAP had high sorption capacity and very rapid uptake for UO{sub 2}{sup 2+} and Th{sup 4+}. Black-Right-Pointing-Pointer Super porous PAAm was obtained from PAAm-HAP after its removal of HAP content. Black-Right-Pointing-Pointer The composite is potential for deposition of U, Th and its associate radionuclides.

  11. Uranium and thorium in weathering and pedogenetic profiles developed on granitic rocks from NW Spain.

    PubMed

    Taboada, Teresa; Martínez Cortizas, Antonio; García, Carlota; García-Rodeja, Eduardo

    2006-03-01

    Uranium and thorium were analyzed in seven weathering and pedogenetic soil profiles developed on granitic rocks from NW Spain. Concentrations were measured by X-ray fluorescence spectrometry (XRF) and the U- and Th-bearing minerals were studied by scanning electron microscopy (SEM) and energy dispersive X-ray spectrometry (EDS). Both elements were determined in rock, bulk soil and in different grain-size fractions (sand: 2000-50 microm, silt: 50-2 microm, and clay: <2 microm). U concentrations in the rock varied between 5.3 and 27.7 mg kg(-1) and Th concentrations from 5.5 to 50.7 mg kg(-1). The most alkalic rocks can be considered as U-rich granites. Bulk soil U and Th concentrations are similar to those of the rocks (4.8-29.2 and 7.4-56.7 mg kg(-1), respectively), but in the grain-size fractions both elements show the lowest concentrations in the sand and the highest in the clay. In the latter, concentrations are always higher than those of the rocks, particularly in the C horizons with enrichments up to 4 times for U and 5 times for Th. The concentration profiles and the ratios to the parent rock suggest that U and Th are leached from the surface soil and accumulate in the deeper horizons. Mass balance calculations, using Ti as a reference immobile element, also support U and Th leaching in the solum and supergene enrichment in bottom horizons. Leaching seems to be more intense on horizons with gravel content higher than 20%. The leaching of U and Th in the topmost horizons and the accumulation in the bottom soil horizons can be considered as a natural attenuation of the impact of these radiogenic elements in the environment. But their enrichment in the potentially airborne fraction poses some risk of redistribution in the ecosystems.

  12. Uranium, Thorium and some other trace elements in phosphorites from different provenances

    NASA Astrophysics Data System (ADS)

    Bech, J.; Reverter, F.; Tume, P.; Roca, N.; Suarez, E.; Sepúlveda, G.; Sokolovska, M.

    2012-04-01

    Data on the trace element composition of phosphorites is scarce. Some of them may be harmful at certain concentrations. Special concern is given to the radionuclides U and Th and some other heavy metals such as: Co, Cr, Cu, Ni and V. Phosphorites of different origins can vary significantly in the trace element concentrations. 37 samples of phosphorites from 16 deposits were analyzed for Uranium, Thorium and five potential toxic elements (Co, Cr, Cu, Ni and V) as well as 26 samples of data gathered from the literature. In total 63 samples of phosphorites from 20 deposits of 19 countries were studied: Algeria, Australia, Brazil, Burkina Faso, Chile, Colombia, Egypt, India, Israel, Mongolia, Morocco, New Zealand, Peru, Senegal, Syria, Togo, Tunisia, USA and Venezuela. Aqua regia extracts were used to estimate the "pseudototal" values, following standard procedures (ISO 11466, 2002) and measured by ICP-MS. The median concentrations (mgkg-1) obtained were: U 53 (range 0.20-177), Th 4.05 (range 1-49), Co 4 (range 0.5-159), Cr 100 (range 15-1000), Cu 20 (range 5-213), Ni 21 (range 3-850) and V 70.05 (range 20-591). As 120 mgkg-1 of U concentration of phosphorites is the value considered to be useful as a source of nuclear fuel, we now indicate the deposits with values higher than 120 mgkg-1: Khouribga KIISB (Morocco) 121, Khouribga KIISL (Morocco) 123, Champ mines (Idaho, USA) 131, Noralyn (Central Florida, USA) 138, Bone Valley (Florida, USA) 140, Boucraa BGB (Morocco) 141, Boucraa BGC (Morocco) 152, Negev (Israel) 172 and Chatam Rise (New Zealand) 177. The highest Th concentration found was 49 mgkg-1 at Bijawar Group (India). Uranium shows significant positive correlations with V (r = 0.41) and Cr (r = 0.30), and significant negative correlations with Co (r= -0.47). Other positive correlations are Cr with Cu (r=0.58), Cr with V (r=0.52) and Cr with Ni (r=0.51). Cu correlates positively with Ni (r=0.84) and with V (r=0.63). Ni correlates positively with V (r=0.72).

  13. Relativistic effects on the thermal expansion of the actinide elements

    SciTech Connect

    Soederlind, P.; Nordstroem, L.; Lou Yongming; Johansson, B. )

    1990-09-01

    The room-temperature linear thermal-expansion coefficient is calculated for the light actinides thorium, protactinium, uranium, neptunium, and plutonium for the fcc crystal structure. The relativistic spin-orbit interaction is included in these calculations. We show that the spin-orbit splitting of the 5{ital f} band gives rise to a considerable increase of the thermal expansion and to a large extent explains the observed anomalously large thermal expansion for the neptunium and plutonium metals.

  14. Acquisition of improved reference values for cesium, iodine, strontium, thorium, and uranium in selected NIST reference materials.

    PubMed

    Parr, R M; Kawamura, H; Iyengar, G V

    1999-01-01

    As part of a study on the ingestion and organ content of some trace elements of importance in radiological protection, additional work has been undertaken to acquire improved reference values for cesium, iodine, strontium, thorium, and uranium in four selected reference materials provided by the US National Institute of Standards and Technology. The materials are SRM-1548 Total Diet, SRM-1548a Typical Diet, SRM-1486 Bone Meal, and RM-8414 Bovine Muscle. A coordinated study was undertaken with the help of seven selected laboratories in five countries. Instrumental and radiochemical neutron activation analysis and inductively coupled plasma-mass spectrometry were the analytical main techniques used.

  15. Determination of lead, uranium, thorium, and thallium in silicate glass standard materials by isotope dilution mass spectrometry

    USGS Publications Warehouse

    Barnes, I.L.; Garner, E.L.; Gramlich, J.W.; Moore, L.J.; Murphy, T.J.; Machlan, L.A.; Shields, W.R.; Tatsumoto, M.; Knight, R.J.

    1973-01-01

    A set of four standard glasses has been prepared which have been doped with 61 different elements at the 500-, 50-, 1-, and 0.02-ppm level. The concentrations of lead, uranium, thorium, and thallium have been determined by isotope dilution mass spectrometry at a number of points in each of the glasses. The results obtained from independent determinations in two laboratories demonstrate the homogeneity of the samples and that precision of the order of 0.5% (95% L.E.) may be obtained by the method even at the 20-ppb level for these elements. The chemical and mass spectrometric procedures necessary are presented.

  16. 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.

  17. The United States Transuranium and Uranium Registries as sources for actinide dosimetry and bioeffects.

    PubMed

    Filipy, R E; Russell, J J

    2003-01-01

    The United States Transuranium and Uranium Registries (USTUR) has analysed tissues collected at autopsies of over 300 former radiation workers from actinide processing sites throughout the US, in addition to collecting the medical and radiation exposure histories of those workers. These data are included in a large USTUR database and they are available to research scientists throughout the world, either as public records or through collaborative projects with the USTUR. The USTUR also operates the National Human Radiobiological Tissue Repository (NHRTR), in which portions of tissue samples collected at autopsy are kept. These samples, frozen at -70 degrees C, may be used for molecular studies of the effects of radiation. Medical and radiation exposure histories of the tissue donors are available, as are the results of radiochemical analyses of adjacent portions of the samples. These materials are available to researchers who have collaborative agreements with the USTUR, which can be established by accessing USTUR staff members through the website, http://www.ustur.wsu.edu.

  18. Environmental Actinide Mobility: Plutonium and Uranium Interactions with Exopolysaccharides and Siderophores of Aerobic Soil Microbes

    SciTech Connect

    Neu, Mary P.; Vanderberg, Laura

    2001-06-01

    Research efforts into understanding the effect of siderophores and capsules on actinide speciation and resultant environmental behavior are ongoing. Investigations on both siderophores have progressed. The redox chemistry of Pu(VI) and Pu(V) with DFO under acidic conditions was examined by UV-Vis and NMR spectroscopies. Pu(VI) was instantly reduced to Pu(V) by DFO and DFO cleavage resulted. Neither DFO nor the cleavage product appeared to coordinate with Pu(V) in the pH range examined. Growth of S. pilosus for cellular translocation experiments was optimized and experiments to determine DFO-mediated uranium uptake by S. pilosus are underway. OFS siderophore(s) production has been optimized and product identification is underway. Siderophore-like molecules were positive for the Arnow assay and had UV absorbance bands at 250nm and 315nm, suggesting catecholates-type molecules. Siderophores were produced with C13 - C16 as carbon source in AM-1 salts medium with 1.0mM iron. Siderophore accumulation was slowest on C13 due to the slower growth of OFS on this substrate. The C16 concentration in the culture influenced siderophore production, with highest levels at 1.0% and 2.0%.

  19. [The assessment of no adverse effect doses for plant populations chronically exposed to radionuclides of uranium and thorium decay series].

    PubMed

    Evseeva, T I; Maĭstrenko, T A; Belykh, E S; Geras'kin, S A

    2010-01-01

    Dose rates cause no adverse effects on natural populations of Pinus sylvestris L. and Vicia cracca L. inhabiting territories contaminated by uranium mill tailings and radium production wastes (Vodny settlement, Komi Republic) were determined. A significant increase in embryonic lethal mutation frequency in V. cracca legumes and decrease in seedlings survival rate as compared with control values were registered at dose rate equal to 1.67 mGy/day, that is 280 times higher than the one calculated for the reference site. The adverse effects in P. sylvestris expressed in increased frequency of chromosome aberrations in meristematic root tips and decreased reproductive capacity of seeds were determined at absorbed dose rate equal to 0.083 mGy/day. Data obtained show that the decrease in plant reproductive capacity in case of chronic exposure of radionuclides of uranium and thorium decay series can observe at lower weighted absorbed dose rates than in case of environmental contamination by artificial radionuclides.

  20. High-Precision Isotope Analysis of Uranium and Thorium by TIMS

    NASA Astrophysics Data System (ADS)

    Neymark, L. A.; Paces, J. B.

    2006-12-01

    The U.S. Geological Survey (USGS) Yucca Mountain Project Branch laboratory in Denver, Colorado, conducts routine high-precision isotope analyses of uranium (U) and thorium (Th) using thermal ionization mass- spectrometry (TIMS). The measurements are conducted by a ThermoFinnigan Triton\\texttrademark equipped with a Faraday multi-collector system and an energy filter in front of an active-film-type secondary electron multiplier (SEM). The abundance sensitivity of the instrument (signal at mass 237 over 238U in natural U) with the energy filter is about 15 ppb and peak tails are reduced by a factor of about 100 relative to the Faraday cup measurements. Since instrument installation in April 2004, more than 500 rock and water samples have been analyzed in support of isotope-geochemical studies for the U.S. Department of Energy`s Yucca Mountain Project. Isotope ratios of sub-nanogram to microgram U and Th samples are measured on graphite-coated single- filament and double-filament assemblies using zone-refined rhenium filaments. Ion beams less than 5 mV are measured with the SEM, which is corrected for non-linearity on the basis of measurements of NIST U-500 and 4321B standards with ion beams ranging from 0.01 to 8 mV. Inter-calibration between the SEM and the Faraday multi-collector is performed for every mass cycle using a 5 mV beam switched between Faraday cup and SEM (bridging technique), because SEM-Faraday inter-calibrations prior to the measurement failed to produce acceptable results. Either natural (^{235}U) or artificial (^{236}U, ^{229}Th) isotopes were used for the bridging. Separate runs are conducted for minor isotopes using SEM only. These techniques result in high within-run precisions of less than 0.1 to 0.2 percent for 234U/238U and 0.2 to 0.5 percent for 230Th/238U. The performance of the instrument is monitored using several U and Th isotope standards. The mean measured 234U/238U in NIST SRM 4321B is (52.879±0.004)×10-6 (95 percent confidence, n

  1. Budgets and behaviors of uranium and thorium series isotopes in the Santa Monica Basin off the California Coast

    SciTech Connect

    Yu, Lei.

    1991-12-16

    Samples from three time-series sediment traps deployed in the Santa Monica Basin off the California coast were analyzed to study the flux and scavenging of uranium and thorium series isotopes. Variations of uranium and thorium series isotopes fluxes in the water column were obtained by integrating these time-series deployment results. Mass and radionuclide fluxes measured from bottom sediment traps compare favorably with fluxed determined from sediment core data. This agreement suggests that the near-bottom sediment traps are capable of collecting settling particles representative of the surface sediment. The phase distributions of {sup 234}Th in the water column were calculated by an inverse method using sediment trap data, which help to study the variations of {sup 234}Th scavenging in the water column. Scavenging and radioactive decay of {sup 234}Th are the two principal processes for balancing {sup 234}Th budget in the water column. The residence times of dissolved and particulate {sup 234}Th were determined by a {sup 234}Th scavenging model.

  2. Determination of uranium, thorium, and 18 other elements in high-purity molybdenum by radiochemical neutron activation analysis

    SciTech Connect

    Theimer, K.H.; Krivan, V. )

    1990-12-15

    A radiochemical neutron activation analysis technique for the determination of uranium and thorium in high-purity molybdenum via the indicator radionuclides {sup 239}Np for U and {sup 233}Pa for Th has been developed. Simultaneously, the elements Ag, Co, Cr, Cs, Cu, Fe, Ga, In, Ir, K, Mn, Na, Ni, Rb, Ru, Sc, Se, and Zn can be determined, too. The elements Hf, Sb, Ta, Sn, and W were determined by instrumental neutron activation analysis. The radiochemical separation is performed by anion exchange on a Dowex 1 {times} 8 column from a 20 M HF/3% H{sub 2}O{sub 2} medium. A limit of detection of 4 ng/g for uranium and 40 pg/g for thorium can be achieved. For the other elements, the limits of detection are between 1 pg/g and 100 ng/g. A modified more selective separation of the indicator radionuclide of Th, {sup 233}Pa, allows improvement of the limit of detection for Th by a factor up to 5. This technique was applied to the analysis of high-purity molybdenum, and the results of a number of elements were compared with those of other techniques.

  3. Uranium, Thorium, Potassium Contents of Materials in the Homestake Underground, Lead, SD

    NASA Astrophysics Data System (ADS)

    Roggenthen, W.; Smith, A.

    2008-12-01

    The uranium, thorium, and potassium contents (UTK) of materials in the underground laboratory at the Homestake DUSEL in Lead, SD, can significantly affect the radioactive backgrounds experienced by detectors in physics experiments planned for the facility. Many highly sensitive experiments require low activities both in terms of direct gamma and neutron radiation as well as radon that might emanate from the materials. Specific issues requiring characterization include evaluation of the rock in which laboratory rooms will be emplaced, the design of the cement and aggregate used in shotcreting the laboratory areas used for the physics experiments, estimates of requirements for shielding from radiation from the country rock, and estimates of radon emanation. The rocks of most importance from this standpoint in the laboratory underground include the Poorman Formation, the Yates Member of the Poorman Formation, and Tertiary igneous rocks. The laboratory at the 7400 level currently is planned for construction in the Yates, whereas the laboratories at the 4850 level are scheduled for construction in both the general Poorman Fm. and the Yates. The UTK contents of Poorman and Yates from the underground are generally very low (0.1 - 0.2 ppm U and 0.2 - 0.4 ppm Th). Rhyolitic intrusive rocks, which occur as thin dikes in the vicinity of the 4850 level laboratory, have substantially higher values that are reflective of their more silicic nature with typical U values in the range of 8 - 9 ppm. Many of the laboratory rooms for the detector experiments will have walls that have been shotcreted and floors finished with concrete. The concrete consists of at least two components, the cement and the aggregate. The choices for cement material are limited by local availability but the UTK content is in the 3 ppm range for U. Analyses of potential aggregates show that sources of aggregate from standard regional aggregate resources appear to have higher values of UTK content than is

  4. Simultaneous extraction and preconcentration of uranium and thorium in aqueous samples by new modified mesoporous silica prior to inductively coupled plasma optical emission spectrometry determination.

    PubMed

    Yousefi, Seyed Reza; Ahmadi, Seyed Javad; Shemirani, Farzaneh; Jamali, Mohammad Reza; Salavati-Niasari, Masoud

    2009-11-15

    A new synthesized modified mesoporous silica (MCM-41) using 5-nitro-2-furaldehyde (fural) was applied as an effective sorbent for the solid phase extraction of uranium(VI) and thorium(IV) ions from aqueous solution for the measurement by inductively coupled plasma optical emission spectrometry (ICP OES). The influences of some analytical parameters on the quantitative recoveries of the analyte ions were investigated in batch method. Under optimal conditions, the analyte ions were sorbed by the sorbent at pH 5.5 and then eluted with 1.0 mL of 1.0 mol L(-1) HNO(3). The preconcentration factor was 100 for a 100mL sample volume. The limits of detection (LOD) obtained for uranium(VI) and thorium(IV) were 0.3 microg L(-1). The maximum sorption capacity of the modified MCM-41 was found to be 47 and 49 mg g(-1) for uranium(VI) and thorium(IV), respectively. The sorbent exhibited good stability, reusability, high adsorption capacity and fast rate of equilibrium for sorption/desorption of uranium and thorium ions. The applicability of the synthesized sorbent was examined using CRM and real water samples.

  5. A novel aeration-assisted homogenous liquid-liquid microextration for determination of thorium and uranium in water and hair samples by inductively coupled plasma-mass spectroscopy.

    PubMed

    Veyseh, Somayeh; Niazi, Ali

    2016-01-15

    A novel method based on aeration-assisted homogeneous liquid-liquid microextraction using high density solvent is presented, which is combined with inductively coupled plasma-mass spectroscopy in which simultaneous preconcentration and determination of thorium and uranium with arsenazo III as the chelating reagent is carried out. To achieve optimum conditions, several parameters such as pH, concentration of arsenazo III, extraction and homogenous solvent types and their volumes, salt concentration and extraction time were investigated. Under which, the calibration graphs were linear in the range of 0.5-600.0ng L(-1) for thorium and 0.3-550.0ng L(-1) for uranium. Good linearities were obtained for both analytes with R(2) values larger than 0.9990. The limits of detection (LOD, 3Sb/m, n=5) of this method were 0.12 and 0.09ng L(-1), and the enrichment factors were estimated to be 370 and 410 for thorium and uranium, respectively. The proposed method was applied to determine the thorium and uranium in human hair and different environmental water samples. Acceptable recoveries ranged from 99.4% to 100.7% with standard deviation of 0.05 to 0.17.

  6. Thorium-phosphorus triamidoamine complexes containing Th-P single- and multiple-bond interactions

    NASA Astrophysics Data System (ADS)

    Wildman, Elizabeth P.; Balázs, Gábor; Wooles, Ashley J.; Scheer, Manfred; Liddle, Stephen T.

    2016-09-01

    Despite the burgeoning field of uranium-ligand multiple bonds, analogous complexes involving other actinides remain scarce. For thorium, under ambient conditions only a few multiple bonds to carbon, nitrogen, oxygen, sulfur, selenium and tellurium are reported, and no multiple bonds to phosphorus are known, reflecting a general paucity of synthetic methodologies and also problems associated with stabilising these linkages at the large thorium ion. Here we report structurally authenticated examples of a parent thorium(IV)-phosphanide (Th-PH2), a terminal thorium(IV)-phosphinidene (Th=PH), a parent dithorium(IV)-phosphinidiide (Th-P(H)-Th) and a discrete actinide-phosphido complex under ambient conditions (Th=P=Th). Although thorium is traditionally considered to have dominant 6d-orbital contributions to its bonding, contrasting to majority 5f-orbital character for uranium, computational analyses suggests that the bonding of thorium can be more nuanced, in terms of 5f- versus 6d-orbital composition and also significant involvement of the 7s-orbital and how this affects the balance of 5f- versus 6d-orbital bonding character.

  7. Evaluation of chelation preconcentration for the determination of actinide elements by flow injection ICP-MS

    SciTech Connect

    Evans, E.H.; Truscott, J.B.; Bromley, L.; Jones, P.; Turner, J.; Fairman, B.E.

    1998-12-31

    A chelation column preconcentration method has been developed for the determination of uranium and thorium in waters by ICP-MS. Detection limits of 24 pg and 60 pg respectively were obtained, but these were blank limited. Uranium and Thorium were determined in certified reference materials. Results for uranium were 121 {+-} 21 and 15 {+-} 3 ng/g in NIST 1566a and NIST 1575 compared with certified values of 132 {+-} 12 and 20 {+-} 4 ng/g respectively. Results for thorium were 29 {+-} 8 and 28 {+-} 5 ng/g in NIST 1566a and NIST 1575 compared with indicative and certified values of 40 and 37 {+-} 3 ng/g respectively. The on-line separation of actinide radionuclides was achieved by selective elution of U, Th, Pu, Np, and Am.

  8. Distinguishing Between Site Waste, Natural, and Other Sources of Contamination at Uranium and Thorium Contaminated Sites - 12274

    SciTech Connect

    Hays, David C.

    2012-07-01

    Uranium and thorium processing and milling sites generate wastes (source, byproduct, or technically enhanced naturally occurring material), that contain contaminants that are similar to naturally occurring radioactive material deposits and other industry wastes. This can lead to mis-identification of other materials as Site wastes. A review of methods used by the US Army Corps of Engineers and the Environmental Protection Agency to distinguish Site wastes from potential other sources, enhanced materials, and natural deposits, at three different thorium mills was conducted. Real case examples demonstrate the importance of understanding the methods of distinguishing wastes. Distinguishing between Site wastes and enhanced Background material can be facilitated by establishing and applying a formal process. Significant project cost avoidance may be realized by distinguishing Site wastes from enhanced NORM. Collection of information on other potential sources of radioactive material and physical information related to the potential for other radioactive material sources should be gathered and reported in the Historical Site Assessment. At a minimum, locations of other such information should be recorded. Site decision makers should approach each Site area with the expectation that non site related radioactive material may be present and have a process in place to distinguish from Site and non Site related materials. (authors)

  9. Potassium, rubidium, strontium, thorium, uranium, and the ratio of strontium-87 to strontium-86 in oceanic tholeiitic basalt

    USGS Publications Warehouse

    Tatsumoto, M.; Hedge, C.E.; Engel, A.E.J.

    1965-01-01

    The average concentrations of potassium, rubidium, strontium, thorium, and uranium in oceanic tholeiitic basalt are (in parts per million) K, 1400; Rb, 1.2; Sr, 120; Th, 0.2; and U, 0.1. The ratio Sr87 to Sr86 is about 0.702, that of K to U is 1.4 ?? 104, and of Th to U is 1.8. These amounts of K, Th, U, and radiogenic Sr87 are less than in other common igneous rocks. The ratios of Th to U and Sr87 to Sr 86 suggest that the source region of the oceanic tholeiites was differentiated from the original mantle material some time in the geologic past.

  10. Determination of trace impurities in uranium, thorium and plutonium matrices by solvent extraction and inductively coupled plasma atomic emission spectrometry.

    PubMed

    Gopalkrishnan, M; Radhakrishnan, K; Dhami, P S; Kulkarni, V T; Joshi, M V; Patwardhan, A B; Ramanujam, A; Mathur, J N

    1997-02-01

    Studies on the determination of trace metallic impurities in nuclear materials such as uranium, thorium and plutonium are described. The bulk of the matrix is separated by batch extraction from their nitric acid solutions using 2-ethylhexyl hydrogen 2-ethylhexyl phosphonate (KSM-17, equivalent to PC88-A). The final aqueous phase containing the metallic impurities is fed to a high-temperature source inductively coupled plasma and the analysis is carried out employing a computer-controlled multichannel direct-reading spectrometer. The studies also included the recovery of impurities at various acidities and spectral interferences of the above matrices over the analyte elements. Based on the above studies, methods were standardized for the determination of 19 elements, viz. Al, B, Be, Ca, Cd, Cr, Cu, Fe, Mg, Mn, Ni, Pb, Si, Zn, Ce, Dy, Eu, Gd and Sm, in U/Th/Pu solutions. The relative standard deviation for various elements is in the range 1-5%.

  11. Use of (77)Se and (125)Te NMR Spectroscopy to Probe Covalency of the Actinide-Chalcogen Bonding in [Th(En){N(SiMe3)2}3](-) (E = Se, Te; n = 1, 2) and Their Oxo-Uranium(VI) Congeners.

    PubMed

    Smiles, Danil E; Wu, Guang; Hrobárik, Peter; Hayton, Trevor W

    2016-01-27

    Reaction of [Th(I)(NR2)3] (R = SiMe3) (1) with 1 equiv of either [K(18-crown-6)]2[Se4] or [K(18-crown-6)]2[Te2] affords the thorium dichalcogenides, [K(18-crown-6)][Th(η(2)-E2)(NR2)3] (E = Se, 2; E = Te, 3), respectively. Removal of one chalcogen atom via reaction with Et3P, or Et3P and Hg, affords the monoselenide and monotelluride complexes of thorium, [K(18-crown-6)][Th(E)(NR2)3] (E = Se, 4; E = Te, 5), respectively. Both 4 and 5 were characterized by X-ray crystallography and were found to feature the shortest known Th-Se and Th-Te bond distances. The electronic structure and nature of the actinide-chalcogen bonds were investigated with (77)Se and (125)Te NMR spectroscopy accompanied by detailed quantum-chemical analysis. We also recorded the (77)Se NMR shift for a U(VI) oxo-selenido complex, [U(O)(Se)(NR2)3](-) (δ((77)Se) = 4905 ppm), which features the highest frequency (77)Se NMR shift yet reported, and expands the known (77)Se chemical shift range for diamagnetic substances from ∼3300 ppm to almost 6000 ppm. Both (77)Se and (125)Te NMR chemical shifts of given chalcogenide ligands were identified as quantitative measures of the An-E bond covalency within an isoelectronic series and supported significant 5f-orbital participation in actinide-ligand bonding for uranium(VI) complexes in contrast to those involving thorium(IV). Moreover, X-ray diffraction studies together with NMR spectroscopic data and density functional theory (DFT) calculations provide convincing evidence for the actinide-chalcogen multiple bonding in the title complexes. Larger An-E covalency is observed in the [U(O)(E)(NR2)3](-) series, which decreases as the chalcogen atom becomes heavier.

  12. 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.

  13. Dioxins, furans, biphenyls, arsenic, thorium and uranium in natural and anthropogenic sources of phosphorus and calcium used in agriculture.

    PubMed

    Avelar, A C; Ferreira, W M; Pemberthy, D; Abad, E; Amaral, M A

    2016-05-01

    The aim of this study was to assess the presence of dioxins, furans and biphenyls, and the inorganic contaminants such as arsenic (As), thorium (Th) and uranium (U) in three main products used in Agriculture in Brazil: feed grade dicalcium phosphate, calcined bovine bone meal and calcitic limestone. The first two are anthropogenic sources of phosphorus and calcium, while calcitic limestone is a natural unprocessed mineral. Regarding to dioxin-like substances, all samples analyzed exhibited dioxins (PCDD) and furans (PCDF) and dioxin-like polychlorinated biphenyls (dl-PCBs) concentrations below limit of detection (LOD). In general, achieved is in accordance with regulation in Brazil where is established a maximum limit in limestone used in the citric pulp production (0.50pg WHO-TEQ g(-1)). In addition, reported data revealed very low levels for limestone in comparison with similar materials reported by European legislation. As result for toxic metals, achieved data were obtained using Instrumental Neutron Activation Analysis (INAA). On one hand, limestone sample exhibits the largest arsenic concentration. On another hand, dicalcium phosphate exhibited the largest uranium concentration, which represents a standard in animal nutrition. Therefore, it is phosphorus source in the animal feed industry can be a goal of concern in the feed field.

  14. AN INTEGRAL REACTOR PHYSICS EXPERIMENT TO INFER ACTINIDE CAPTURE CROSS-SECTIONS FROM THORIUM TO CALIFORNIUM WITH ACCELERATOR MASS SPECTROMETRY

    SciTech Connect

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

    2010-04-01

    The principle of the proposed experiment is to irradiate very pure actinide samples in the Advanced Test Reactor (ATR) at INL and, after a given time, determine the amount of the different transmutation products. The determination of the nuclide densities before and after neutron irradiation will allow inference of effective neutron capture cross-sections. This approach has been used in the past and the novelty of this experiment is that the atom densities of the different transmutation products will be determined using the Accelerator Mass Spectroscopy (AMS) technique at the ATLAS facility located at ANL. It is currently planned to irradiate the following isotopes: 232Th, 235U, 236U, 238U, 237Np, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am, 243Am and 248Cm.

  15. Comparative uptake of uranium, thorium, and plutonium by biota inhabiting a contaminated Tennessee floodplain

    SciTech Connect

    Garten, C.T. Jr.; Bondietti, E.A.; Walker, R.L.

    1981-04-01

    The uptake of /sup 238/U, /sup 232/Th, and /sup 239/Pu from soil by fescue, grasshoppers, and small mammals was compared at the contaminated White Oak Creek floodplain in East Tennessee. Comparisons of actinide uptake were based on analyses of radionuclide ratios (U/Pu and Th/Pu) in soil and biota. U:Pu ratios in small mammal carcasses (shrews, mice, and rats) and bone samples from larger mammals (rabbit, woodchuck, opossum, and raccoon) were significantly greater (P less than or equal to 0.05) than U/Pu ratios in soil (based on 8M HNO/sub 3/ extractable). There was no significant difference between Th/Pu ratios in animals and soil. The order of actinide accumulation by biota from the site relative to contaminated soil was U > Th approx. = Pu.

  16. Standardless EDXRF application for quantification of thorium (Th), uranium (U) and rare earth elements (REEs) in various Malaysian rare earth ores

    NASA Astrophysics Data System (ADS)

    Ruf, Mohd Izzat Fahmi Mohd; Bahri, Che Nor Aniza Che Zainul; AL-Areqi, Wadeeah M.; Majid, Amran Ab.

    2016-11-01

    Our local rare earth ores contained substantial amount of Thorium and Uranium which the level exceed permissible limit adopted by Malaysia and many importing nation. X-ray fluorescence technique has been applied for determination of thorium (Th), uranium (U) and rare earth elements (REEs) in Malaysian rare earth ores as it's recognized as viable tool. XRF has been widely used in detecting elemental composition of unknown materials both qualitative and quantitatively because of its wide range of element detection alongside the non-destructive analytical technique with great accuracy and precision. Four types of minerals sample which is monazite, xenotime, ilmenite and zircon were collected from `amang' factory located in famous city of mining, Ipoh and analyzed using EDXRF.

  17. [Regularities of lateral distribution of uranium and thorium decay series radionuclides in the anthropogenically changed soils from the area of radium production waste storage].

    PubMed

    Evseeva, T I; Belykh, E S; Maĭstrenko, T A; Geras'kin, S A; Taskaev, A I; Vakhrusheva, O M

    2012-01-01

    Cartographical investigations of the territory of radium production waste storage has shown some changes in lateral differentiation of radionuclides of uranium and thorium decay series to occur during 27 years (1981-2008). Those changes are caused mostly by flat denudation typical for fluvial terrace. At present radionuclides of uranium and thorium decay series are concentrated mostly in flood lands and relief depressions. At the same time, decrease in the radionuclide activity concentration in 0-20 cm soil layer is observed with changes in lateral distribution. Total stocks of 226Ra, 210Pb and 210Po within catena soils studied in the northern and southern parts of the waste storage decreased 3-6 times, 238U - 2 times, and did not significantly change in case of 232Th during 27 years. Nonetheless, most of the samples studied are referred to radioactive waste both according to Russian standards (SPORO-2002) and IAEA safety norms (IAEA, 2004).

  18. Study on transfers of uranium, thorium and decay products from grain, water and soil to chicken meat and egg contents.

    PubMed

    Jeambrun, M; Pourcelot, L; Mercat, C; Boulet, B; Loyen, J; Cagnat, X; Gauthier-Lafaye, F

    2012-08-01

    Activity concentrations of the uranium and thorium series radionuclides were determined in chicken meat and eggs as well as in soil, water and other dietary intakes of poultry at five sites of the French territory. These data allow the calculation of transfer coefficients which enrich the database given by the technical report series no. 472 of the IAEA. In egg contents, the highest activity concentrations (in mBq kg(-1) fresh weight) are for (226)Ra, ranging between 136 and 190 and are much lower for uranium (between 0.51 and 1.30 for (238)U). In chicken meat, (238)U activity concentration is higher than in egg contents and ranges between 1.7 and 9.7. Concerning (232)Th, its activity concentration is lower than uranium and ranges between 0.5 and 4.9. Daily ingested activity concentration by the animals was assessed taking into account the activity concentrations measured in the grains, in the soil and in the drinking water. The activity concentration in grains and the daily intakes allow the calculation of concentration ratios and transfer coefficients for chicken meat and egg contents. In chicken meat the transfer coefficients (d kg(-1)) range between 0.0018 and 0.0073 for (238)U and between 0.0008 and 0.0028 for (232)Th. In egg contents they range from 0.00018 to 0.0018 for (238)U and are much higher for radium isotopes (0.10-0.23 for (226)Ra and 0.07-0.11 for (228)Ra).

  19. Uranium and thorium in soils, mineral sands, water and food samples in a tin mining area in Nigeria with elevated activity.

    PubMed

    Arogunjo, A M; Höllriegl, V; Giussani, A; Leopold, K; Gerstmann, U; Veronese, I; Oeh, U

    2009-03-01

    The activity concentrations of uranium and thorium have been determined in soils and mineral sands from the Nigerian tin mining area of Bisichi, located in the Jos Plateau, and from two control areas in Nigeria (Jos City and Akure) using high-purity germanium detectors (HPGe). High resolution sector field inductively coupled plasma mass spectroscopy (HR-SF-ICP-MS) was used to determine uranium and thorium in liquids and foodstuffs consumed locally in the mining area. The activities of uranium and thorium measured in the soils and mineral sands from Bisichi ranged from 8.7 kBq kg(-1) to 51 kBq kg(-1) for (238)U and from 16.8 kBq kg(-1) to 98 kBq kg(-1) for (232)Th, respectively. These values were significantly higher than those in the control areas of Jos City and Akure and than the reference values reported in the literature. They even exceeded the concentrations reported for areas of high natural radioactive background. Radionuclide concentrations in samples of the local foodstuffs and in water samples collected in Bisichi were found to be higher than UNSCEAR reference values. The results reveal the pollution potential of the mining activities on the surrounding areas.

  20. Determination of trace element concentrations and stable lead, uranium and thorium isotope ratios by quadrupole-ICP-MS in NORM and NORM-polluted sample leachates.

    PubMed

    Mas, J L; Villa, M; Hurtado, S; García-Tenorio, R

    2012-02-29

    This work focuses on the monitoring of the potential pollution in scenarios that involve NORM-related industrial activities (environmental or in-door scenarios). The objective was to develop a method to determine extent and origin of the contamination, suitable for monitoring (i.e. simple, fast and economical) and avoiding the use of too many different instruments. It is presented a radiochemical method that allows the determination of trace element concentrations and 206Pb/207Pb/208Pb, 238U/234U and 232Th/230Th isotope ratios using a single sample aliquot and a single instrument (ICP-QMS). Eichrom UTEVA® extraction chromatography minicolumns were used to separate uranium and thorium in sample leachates. Independent ICP-MS determinations of uranium and thorium isotope ratios were carried out afterwards. Previously a small aliquot of the leachate was used for the determination of trace element concentrations and lead isotope ratios. Several radiochemical arrangements were tested to get maximum performances and simplicity of the method. The performances of the method were studied in terms of chemical yields of uranium and thorium and removal of the potentially interfering elements. The established method was applied to samples from a chemical industry and sediments collected in a NORM-polluted scenario. The results obtained from our method allowed us to infer not only the extent, but also the sources of the contamination in the area.

  1. 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.

  2. 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.

  3. Thorium effect on the oxidation of uranium: Photoelectron spectroscopy (XPS/UPS) and cyclic voltammetry (CV) investigation on (U1 - xThx)O2 (x = 0 to 1) thin films

    NASA Astrophysics Data System (ADS)

    Cakir, P.; Eloirdi, R.; Huber, F.; Konings, R. J. M.; Gouder, T.

    2017-01-01

    Thin films of U1- xThxO2 (x = 0 to 1) have been deposited via reactive DC sputter technique and characterized by X-ray/Ultra-violet Photoelectron Spectroscopy (XPS/UPS), X-ray Powder Diffractometer (XRD) and Cyclic Voltammetry (CV) in order to understand the effect of Thorium on the oxidation mechanism. During the deposition, the competition between uranium and thorium for oxidation showed that thorium has a much higher affinity for oxygen. Deposition conditions, time and temperature were also the subject of this study, to look at the homogeneity and the stability of the films. While core level and valence band spectra were not altered by the time of deposition, temperature was affecting the oxidation state of uranium and the valence band due to the mobility increase of oxygen through the film. X-ray diffraction patterns, core level spectra obtained for U1 - xThxO2 versus the composition showed that lattice parameters follow the Vegard's law and together with the binding energies of U-4f and Th-4f are in good agreement with literature data obtained on bulk compounds. To study the effect of thorium on the oxidation of U1 - xThxO2 films, we used CV experiments at neutral pH of a NaCl solution in contact with air. The results indicated that thorium has an effect on the uranium oxidation as demonstrated by the decrease of the current of the oxidation peak of uranium. XPS measurements made before and after the CV, showed a relative enrichment of thorium at the extent of uranium at the surface supporting the formation at a longer term of a thorium protective layer at the surface of uranium-thorium mixed oxide.

  4. Spatial distribution of uranium and thorium in the surface soil around proposed uranium mining site at Lambapur and its vertical profile in the Nagarjuna Sagar Dam.

    PubMed

    Sartandel, S J; Jha, S K; Bara, S V; Tripathi, R M; Puranik, V D

    2009-10-01

    The understanding and evaluation of the possible interactions of various naturally occurring radionuclides in the world's third largest man-made dam, Nagarjuna Sagar located in Andhra Pradesh, India and built on river Krishna assumed significance with the finding of uranium deposits in locations near the dam. For the present work, surface soil samples from the mineralized area of Lambapur, Mallapuram, Peddagattu and sediment core samples from the Nagarjuna Sagar dam were analyzed for naturally occurring radionuclides namely uranium and thorium using gamma spectrometric technique. Also toxic elements lead and chromium were analysed by the Energy Dispersive X-ray Fluorescence Spectrometer (EDXRF) technique. Surface soil samples show a variation from 25 to 291 Bq/kg (2.02-23.5 mg/kg) for (238)U and 32-311 Bq/kg (7.9-76.9 mg/kg) for (232)Th. U/Th concentration ratio in surface soil samples ranged from 0.19 to 0.31 and was found comparable with the nation wise average of 0.26. The study of sediment core samples reflected higher U/Th concentration ratio of 0.30-0.33 in the bottom section of the core as compared to 0.22-0.25 in the upper section. The concentration ratio in the upper section of the core was similar to the ratio 0.23 found in the western Deccan Basalt region through which the river originates. A higher concentration of lead and chromium was observed in the upper section of the core compared to bottom section indicating the impact of river input on the geochemical character of dam sediment.

  5. The extraction of thorium by calix[6]arene columns for urine analysis.

    PubMed

    Mekki, S; Bouvier-Capely, C; Jalouali, R; Rebière, F

    2011-03-01

    Thorium is a natural alpha-emitting element occurring in various ores and has numerous industrial applications. Routine monitoring of potentially exposed workers is generally achieved through radiobioassay (urine and faeces). The procedures currently used for analysing actinides such as thorium in urine require lengthy chemical separation associated with long counting times by alpha-spectrometry due to low activity levels. Thus, their main drawback is that they are time-consuming, which limits the frequency and flexibility of individual monitoring. In this context, this study developed new radiochemical procedures based on the use of tertbutylcalix[6]arenes bearing three carboxylic acid groups or three hydroxamic acid groups. These previous works demonstrated that these macrocyclic molecules immobilised on an inert solid support are excellent extractants for uranium, plutonium and americium. In this study, the authors investigated the thorium extraction by calix[6]arene columns. Experiments were performed on synthetic solutions and on real urine samples. The influence of various parameters, such as the thorium solution pH and the column flow rate on thorium extraction, was studied. The results showed that both calix[6]arenes are efficient to extract thorium. Thorium extraction is quantitative from pH = 2 for synthetic solution and from pH = 3 for real urine samples. This study has demonstrated that the column flow rate is a crucial parameter since its value must not be too high to achieve the steady-state complexation equilibrium. Finally, these results will be compared with those obtained for other actinides (U, Pu and Am) and the conditions of actinides' separation will be discussed.

  6. Assessment of radionuclides (uranium and thorium) atmospheric pollution around Manjung district, Perak using moss as bio-indicator

    SciTech Connect

    Arshad, Nursyairah Hamzah, Zaini; Wood, Ab. Khalik; Saat, Ahmad

    2016-01-22

    Bio-monitoring method using mosses have been widely done around the world and the effectiveness has been approved. Mosses can be used to assess the levels of atmospheric pollution as mosses pick up nutrients from the atmosphere and deposition retaining many trace elements. In this study, the deposition of two radionuclides; uranium (U) and thorium (Th) around Manjung districts have been evaluated using Leucobryum aduncum as bio-monitoring medium. The samples were collected from 24 sampling sites covering up to 40 km radius to the North, North-East and South-East directions from Teluk Rubiah. The concentrations of U and Th in moss samples were analysed using Energy Dispersive X-Ray Fluorescence (EDXRF) Spectrometer. The concentrations of Th are in the range of 0.07-2.09 mg/kg. Meanwhile, the concentrations of U in the moss are in the range of 0.03-0.18 mg/kg. The Enrichment Factor (EF) was calculated to determine the origin of the radionuclides distributions. Other than that, the distribution maps were developed to observe the distribution of the radionuclides around the study area.

  7. Analysis of radon, uranium 238 and thorium 232 in potable waters: Dose to adult members of the Moroccan urban population

    NASA Astrophysics Data System (ADS)

    Misdaq, M. A.; Ouabi, H.; Merzouki, A.

    2007-10-01

    Uranium (238U) and thorium (232Th) concentrations as well as radon (222Rn) and thoron (220Rn) alpha-activities per unit volume have been measured inside various potable water samples collected from nineteen cities in Morocco by using CR-39 and LR-115 type II solid state nuclear track detectors (SSNTDs). Measured radon alpha-activities ranged from (0.37 ± 0.02) Bq l-1 to (13.6 ± 1.10) Bq l-1 for the potable water samples studied. Alpha-activities due to radon from the ingestion of the studied potable water samples were determined in different compartments of the gastrointestinal system by using the ICRP compartmental model for radon. Annual committed equivalent doses due to radon were evaluated in the gastrointestinal compartments from the ingestion of the potable water samples studied. The influence of the target tissue mass, radon intake and alpha-activity integral due to radon on the annual committed equivalent doses in the gastrointestinal compartments was investigated.

  8. Coupling of Uranium and Thorium Series Isotope Systematics for Age Determination of Late Pleistocene Zircons using LA-ICP-MS

    NASA Astrophysics Data System (ADS)

    Sakata, S.; Hirakawa, S.; Iwano, H.; Danhara, T.; Hirata, T.

    2014-12-01

    Zircon U-Th-Pb dating method is one of the most important tools for estimating the duration of magmatism by means of coupling of uranium, actinium and thorium decay series. Using U-Pb dating method, its reliability is principally guaranteed by the concordance between 238U-206Pb and 235U-207Pb ages. In case of dating Quaternary zircons, however, the initial disequilibrium effect on 230Th and 231Pa should be considered. On the other hands, 232Th-208Pb dating method can be a simple but powerful approach for investigating the age of crystallization because of negligible influence from initial disequilibrium effect. We have developed a new correction model for accurate U-Pb dating of the young zircon samples by taking into consideration of initial disequilibrium and a U-Pb vs Th-Pb concordia diagram for reliable age calibration was successfully established. Hence, the U-Th-Pb dating method can be applied to various zircons ranging from Hadean (4,600 Ma) to Quaternary (~50 ka) ages, and this suggests that further detailed information concerning the thermal history of the geological sequences can be made by the coupling of U-Th-Pb, fission track and Ar-Ar ages. In this presentation, we will show an example of U-Th-Pb dating for zircon samples from Sambe Volcano (3 to 100 ka), southwest Japan and the present dating technique using LA-ICP-MS.

  9. Uranium(iii) and thorium(iv) alkyl complexes as potential starting materials.

    PubMed

    Behrle, Andrew C; Myers, Alexander J; Rungthanaphatsophon, Pokpong; Lukens, Wayne W; Barnes, Charles L; Walensky, Justin R

    2016-12-13

    The synthesis and characterisation of a rare U(iii) alkyl complex, U[η(4)-Me2NC(H)C6H5]3, using the dimethylbenzylamine (DMBA) ligand has been accomplished. While attempting to prepare the U(iv) compound, reduction to the U(iii) complex occurred. In the analogous Th(iv) system, C-H bond activation of a methyl group of one dimethylamine was observed yielding Th[η(4)-Me2NC(H)C6H5]2[η(5)-(CH2)MeNC(H)C6H5] with a dianionic DMBA ligand. The utility of these complexes as starting materials has been analyzed using a bulky dithiocarboxylate ligand to yield tetravalent actinide species.

  10. 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).

  11. Design of a boiling water reactor equilibrium core using thorium-uranium fuel

    SciTech Connect

    Francois, J-L.; Nunez-Carrera, A.; Espinosa-Paredes, G.; Martin-del-Campo, C.

    2004-10-06

    In this paper the design of a Boiling Water Reactor (BWR) equilibrium core using thorium is presented; a heterogeneous blanket-seed core arrangement concept was adopted. The design was developed in three steps: in the first step two different assemblies were designed based on the integrated blanket-seed concept, they are the blanket-dummy assembly and the blanket-seed assembly. The integrated blanketseed concept comes from the fact that the blanket and the seed rods are located in the same assembly, and are burned-out in a once-through cycle. In the second step, a core design was developed to achieve an equilibrium cycle of 365 effective full power days in a standard BWR with a reload of 104 fuel assemblies designed with an average 235U enrichment of 7.5 w/o in the seed sub-lattice. The main operating parameters, like power, linear heat generation rate and void distributions were obtained as well as the shutdown margin. It was observed that the analyzed parameters behave like those obtained in a standard BWR. The shutdown margin design criterion was fulfilled by addition of a burnable poison region in the assembly. In the third step an in-house code was developed to evaluate the thorium equilibrium core under transient conditions. A stability analysis was also performed. Regarding the stability analysis, five operational states were analyzed; four of them define the traditional instability region corner of the power-flow map and the fifth one is the operational state for the full power condition. The frequency and the boiling length were calculated for each operational state. The frequency of the analyzed operational states was similar to that reported for BWRs; these are close to the unstable region that occurs due to the density wave oscillation phenomena in some nuclear power plants. Four transient analyses were also performed: manual SCRAM, recirculation pumps trip, main steam isolation valves closure and loss of feed water. The results of these transients are

  12. PROCESS FOR CONTINUOUSLY SEPARATING IRRADIATION PRODUCTS OF THORIUM

    DOEpatents

    Hatch, L.P.; Miles, F.T.; Sheehan, T.V.; Wiswall, R.H.; Heus, R.J.

    1959-07-01

    A method is presented for separating uranium-233 and protactinium from thorium-232 containing compositions which comprises irradiating finely divided particles of said thorium with a neutron flux to form uranium-233 and protactinium, heating the neutron-irradiated composition in a fluorine and hydrogen atmosphere to form volatile fluorides of uranium and protactinium and thereafter separating said volatile fluorides from the thorium.

  13. Determination of thorium-232 in Canadian soils by gamma-ray spectrometry via lead-212 and actinium-228, interference from uranium

    SciTech Connect

    Zikovsky, L.; Blagoeva, R.

    1994-12-31

    Thorium-232 background levels in non-cultivated Canadian soils (southern and northern Quebec and the Northwest Territories) are presented. Gamma-ray spectrometry was used to determine the activity of {sup 232}Th by measuring the activities of {sup 228}Ac and {sup 212}Pb at 37 sites. The specific activity levels ranged from 2.7 to 95.5 Bq/kg with an overall mean of 24.0 {+-} 15.4 Bq/kg. This activity generated an annual absorbed dose equivalent in air of 0.1 mSv. The activities of {sup 228}Ac and {sup 212}Pb in the soil increased with increasing depth. IT was found that uranium, via its decay product radium, can interfere with the determination of thorium in the soil.

  14. Chemical and isotopic studies of granitic Archean rocks, Owl Creek Mountains, Wyoming: Uranium-thorium-lead systematics of an Archean granite from the Owl Creek Mountains, Wyoming

    SciTech Connect

    Stuckless, J.S.; Nkomo, I.T.; Butt, K.A.

    1986-01-01

    Isotopic analyses of apparently unaltered whole-rock samples of a granite from the Owl Creek Mountains, Wyo., yield a lead-lead isochron age of 2730 {plus minus} 35 Ma, which is somewhat older than the age obtained by the rubidium-strontium whole-rock method. Thorium-lead data for the same samples deviate markedly from an isochronal relation; however, calculated initial {sup 208}Pb/{sup 204}Pb ratios correlate with whole-rock {delta}{sup 18}O values and lead to the conclusion that the {sup 232}Th-{sup 208}Pb data are not colinear because of an originally heterogeneous granitic magma. Relationships in the {sup 207}Pb/{sup 235}U-{sup 206}Pb/{sup 238}U system show that uranium was mobilized during early Laramide time or shortly before, such that most surface and shallow drill-core samples lost 60-80 percent of their uranium, and some fractured, deeper drill-core samples gained from 50 to 10,000 percent uranium. Fission-track maps show that much uranium is located along edges and cleavages of biotite and magnetic where it is readily accessible to oxidizing ground water. Furthermore, qualitative comparisons of uranium distribution in samples with excess radiogenic lead and in samples with approximately equilibrium amounts of uranium and lead suggest that the latter contain more uranium in these readily accessible sites. Unlike other granites that have uranium distributions and isotopic systematics similar to those observed in this study, the granite of the Owl Creek Mountains is not associated with economic uranium deposits.

  15. The Thermodynamics of Thorium-Oxygen and Uranium-Oxygen Systems

    DTIC Science & Technology

    1975-02-19

    i 2 Thermodynamic functions for UO2 (g) .................- 15 3 Thermodynamic functions for TlO(g) --------- ---- - - - -- 25 4 Thermodynamic...The vapor above uranium oxide condensed phases includes U, 110, 蓥 and U03* The composition of the vapor is strongly dependent upon theL0 ratio. In...the three phase system U(L)/U02(s) and vapor (O/U < 1.7) the principal vapor phlast species is UO with smaller amounts of U and to2 vapors. For UO2 a

  16. 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

  17. Synthesis of Coordination Polymers of Tetravalent Actinides (Uranium and Neptunium) with a Phthalate or Mellitate Ligand in an Aqueous Medium.

    PubMed

    Martin, Nicolas P; März, Juliane; Volkringer, Christophe; Henry, Natacha; Hennig, Christoph; Ikeda-Ohno, Atsushi; Loiseau, Thierry

    2017-03-06

    Four metal-organic coordination polymers bearing uranium or neptunium have been hydrothermally synthesized from a tetravalent actinide chloride (AnCl4) and phthalic (1,2-H2bdc) or mellitic (H6mel) acid in aqueous media at 130 °C. With the phthalate ligand, two analogous assemblies ([AnO(H2O)(1,2-bdc)]2·H2O; An = U(4+) (1) or Np(4+) (2)) have been isolated, in which the square-antiprismatic polyhedra of AnO8 are linked to each other via μ3-oxo groups with an edge-sharing mode to materialize infinite zigzag ribbons. The phthalate molecules play a role in connecting the adjacent zigzag chains to build a two-dimensional (2D) network. Water molecules are bonded to the actinide center or found intercalated between the layers. With the mellitate ligand, two distinct structures have been identified. The uranium-based compound [U2(OH)2(H2O)2(mel)] (3) exhibits a three-dimensional (3D) structure composed of the dinuclear units of UO8 polyhedra (square antiprism), which are further linked via the μ2-hydroxo groups. The mellitate linkers use their carboxylate groups to connect the dinuclear units, eventually building a 3D framework. The compound obtained for the neptunium mellitate ([(NpO2)10(H2O)14(Hmel)2]·12H2O (4)) reveals oxidation of the initial Np(IV) to Np(V) under the applied hydrothermal synthetic conditions, yielding the neptunyl(V) (NpO2(+)) unit with a pentagonal-bipyramidal NpO7 environment. This further leads to the formation of a layered assembly of the square-frame NpO7 sheets via the bridging oxygen atoms from the neptunyl oxo groups, which further coordinate to the pentagonal equatorial coordination plane of the adjacent neptunium unit (i.e., cation-cation interactions). In compound 4, the mellitate molecules act as bridging linkers between the NpO7 sheets by using four of their carboxylage groups, eventually building up a 3D structure.

  18. Thorium-uranium disequilibrium dating of Late Quaternary ferruginous concretions and rinds

    NASA Astrophysics Data System (ADS)

    Short, Stephen A.; Lowson, Richard T.; Ems, John; Price, David M.

    1989-06-01

    Radioactive ferruginous nodules from the Alligator Rivers Uranium Province, Northern Territory, Australia, were systematically examined by optical microscopy, XRD, alpha- and fission-track autoradiography, and analysed for U, Th, Ra and major stable elements. Correlation of autoradiographs with microscopic structure and analyses of selective extractions confirmed that U and Th were strongly associated with Fe oxides. Fission-track autoradiography showed no concentration gradient evidence for postdepositional leaching of uranium. Strong acid leaching studies showed that irreversibly adsorbed U, and authigenic 234U and 230Th, but not 226Ra, are quantitatively retained by accumulated oxide/oxyhydroxide. Correlation of the groundwater activity ratio with oxidic 234U/ 238U activity ratios indicated the latter was radiogenically consistent with oxidic 230Th/ 234U activity ratios < 1. Dense, accumulated Fe/Mn oxide matrices are apparently capable of forming radiogenic closed systems in respect of the 230U → 234U → 230Th decay set. 234U/ 238U and 230Th/ 234U activity ratios were used to derive similar mean ages of rinds for four nodules in the same horizon. Th/U ages were also determined, using a Th-index detrital correction method previously used for impure carbonates, of pedogenic Fe/Mn accumulations having background concentrations of U and Th from other locations in Australia. These ages were compared with TL and 14C ages of the-host sediments. The comparisions suggest that Th/U dating could be used to age indurated layers of Fe/Mn oxides in soil horizons < 350 ka old.

  19. Sequential extraction procedure for determination of uranium, thorium, radium, lead and polonium radionuclides by alpha spectrometry in environmental samples

    NASA Astrophysics Data System (ADS)

    Oliveira, J. M.; Carvalho, F. P.

    2006-01-01

    A sequential extraction technique was developed and tested for common naturally-occurring radionuclides. This technique allows the extraction and purification of uranium, thorium, radium, lead, and polonium radionuclides from the same sample. Environmental materials such as water, soil, and biological samples can be analyzed for those radionuclides without matrix interferences in the quality of radioelement purification and in the radiochemical yield. The use of isotopic tracers (232U, 229Th, 224Ra, 209Po, and stable lead carrier) added to the sample in the beginning of the chemical procedure, enables an accurate control of the radiochemical yield for each radioelement. The ion extraction procedure, applied after either complete dissolution of the solid sample with mineral acids or co-precipitation of dissolved radionuclide with MnO2 for aqueous samples, includes the use of commercially available pre-packed columns from Eichrom® and ion exchange columns packed with Bio-Rad resins, in altogether three chromatography columns. All radioactive elements but one are purified and electroplated on stainless steel discs. Polonium is spontaneously plated on a silver disc. The discs are measured using high resolution silicon surface barrier detectors. 210Pb, a beta emitter, can be measured either through the beta emission of 210Bi, or stored for a few months and determined by alpha spectrometry through the in-growth of 210Po. This sequential extraction chromatography technique was tested and validated with the analysis of certified reference materials from the IAEA. Reproducibility was tested through repeated analysis of the same homogeneous material (water sample).

  20. Use of uranium-thorium dating to determine past 14C reservoir effects in lakes: examples from Antarctica

    NASA Astrophysics Data System (ADS)

    Hall, Brenda L.; Henderson, Gideon M.

    2001-12-01

    The chronologies of many lacustrine records suffer from radiocarbon reservoir effects due to the presence of dissolved 'dead' carbon or to slow air-water exchange. Here we use the TIMS uranium-thorium disequilibrium method, in conjunction with AMS radiocarbon dating, to determine the age of lacustrine carbonates and to quantify the past radiocarbon reservoir effect in two Antarctic lakes with differing characteristics. By correcting a single-sample U/Th age for detrital contamination, a 14C offset of ˜18 000 yr was obtained for carbonates from the former grounding line of the Ross Sea ice sheet in Glacial Lake Trowbridge. This large reservoir effect is believed to result from the direct input of old CO 2 from glacial meltwater. In the second example, an isochron approach on coeval samples formed at the bottom of Lake Vida (now exposed due to lower lake level) yielded an age of 9550±340 yr B.P. and a radiocarbon reservoir age of 3600 yr. This offset was probably the result of lack of aeration due to perennial ice cover and/or strong density stratification. This evidence for long-term isolation of the lake bottom indicates another level of hardship for life in the Dry Valley lacustrine environment - an environment studied as an analogue for extreme periods of Earth history, as well as for exobiological implications. The success of the U/Th technique on these two examples indicates that TIMS U/Th dating will be of widespread use in dating the important climate information recorded in the Dry Valleys both within and beyond the 14C age range.

  1. A PWR Thorium Pin Cell Burnup Benchmark

    SciTech Connect

    Weaver, Kevan Dean; Zhao, X.; Pilat, E. E; Hejzlar, P.

    2000-05-01

    As part of work to evaluate the potential benefits of using thorium in LWR fuel, a thorium fueled benchmark comparison was made in this study between state-of-the-art codes, MOCUP (MCNP4B + ORIGEN2), and CASMO-4 for burnup calculations. The MOCUP runs were done individually at MIT and INEEL, using the same model but with some differences in techniques and cross section libraries. Eigenvalue and isotope concentrations were compared on a PWR pin cell model up to high burnup. The eigenvalue comparison as a function of burnup is good: the maximum difference is within 2% and the average absolute difference less than 1%. The isotope concentration comparisons are better than a set of MOX fuel benchmarks and comparable to a set of uranium fuel benchmarks reported in the literature. The actinide and fission product data sources used in the MOCUP burnup calculations for a typical thorium fuel are documented. Reasons for code vs code differences are analyzed and discussed.

  2. Solid-state syntheses and single-crystal characterizations of three tetravalent thorium and uranium silicates

    SciTech Connect

    Jin, Geng Bang Soderholm, L.

    2015-01-15

    Colorless crystals of ThSiO{sub 4} (huttonite) (1) and (Ca{sub 0.5}Na{sub 0.5}){sub 2}NaThSi{sub 8}O{sub 20} (2) have been synthesized by the solid-state reactions of ThO{sub 2}, CaSiO{sub 3}, and Na{sub 2}WO{sub 4} at 1073 K. Green crystals of (Ca{sub 0.5}Na{sub 0.5}){sub 2}NaUSi{sub 8}O{sub 20} (3) have been synthesized by the solid-state reactions of UO{sub 2}, CaSiO{sub 3}, and Na{sub 2}WO{sub 4} at 1003 K. All three compounds have been characterized by single-crystal X-ray diffraction. Compound 1 adopts a monazite-type three-dimensional condensed structure, which is built from edge- and corner-shared ThO{sub 9} polyhedra and SiO{sub 4} tetrahedra. Compounds 2 and 3 are isostructural and they crystallize in a steacyite-type structure. The structure consists of discrete pseudocubic [Si{sub 8}O{sub 20}]{sup 8−} polyanions, which are connected by An{sup 4+} cations into a three-dimensional framework. Each An atom coordinates to eight monodentate [Si{sub 8}O{sub 20}]{sup 8−} moieties in a square antiprismatic geometry. Na{sup +} and Ca{sup 2+} ions reside in the void within the framework. Raman spectra of 1, 2, and 3 were collected on single crystal samples. 1 displays more complex vibrational bands than thorite. Raman spectra of 2 and 3 are analogous with most of vibrational bands located at almost the same regions. - Graphical abstract: A Raman spectrum and crystal structures of (Ca{sub 0.5}Na{sub 0.5}){sub 2}NaAnSi{sub 8}O{sub 20} (An=Th, U), which contain pseudocubic [Si{sub 8}O{sub 20}]{sup 8−} polyanions and eight-coordinate An{sup 4+} cations. - Highlights: • Single crystal growth of three tetravalent actinide silicates from melts. • Single-crystal structures and Raman spectra of (Ca{sub 0.5}Na{sub 0.5}){sub 2}NaAnSi{sub 8}O{sub 20} (An=Th, U). • First report of Raman spectrum of huttonite on single crystal samples.

  3. Uranium series disequilibrium and high thorium and radium enrichments in Karst formations

    SciTech Connect

    Gunten, H.R. von; Roessler, E.; Surbeck, H.

    1996-04-01

    We found, in limestone Karst soils of the Jura Mountains and of the mountains in the central part of Switzerland, an enrichment up to a factor 20 of {sup 230}Th and {sup 226}Ra with respect to the activities of their progenitors, {sup 234}U and {sup 238}U. Thus, a significant radioactive disequilibrium exists between {sup 238/234}U and {sup 230}Th and {sup 226}Ra. The enrichment of {sup 226}Ra leads to locally high concentrations of its decay product, the noble gas {sup 222}Rn. We propose continuous chemical weathering of limestone (calcite) fragments within the soil column as a plausible cause for the high {sup 230}Th, {sup 226}Ra, and {sup 222}Rn activities. Uranium, contained within calcite, is released during weathering and migrates as stable uranyl carbonate complexes through the soil column. In contrast, its decay products ({sup 230}Th and {sup 226}Ra) hydrolyze, are strongly sorbed to soil particles, and/or form insoluble compounds that become more and more enriched in the soil as this process continues in time. 39 refs., 3 figs., 5 tabs.

  4. 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

    inorganic complexants are expected to be carbonate/bicarbonate and hydroxide. There are also organic complexants in TRU waste with the potential to strongly influence actinide solubility. (3) Intrinsic and pseudo-actinide colloid formation - Many actinide species in their expected oxidation states tend to form colloids or strongly associate with non actinide colloids present (e.g., microbial, humic and organic). In this context, the relative importance of actinides, based on the TRU waste inventory, with respect to the potential release of actinides from the WIPP, is greater for plutonium and americium, and to less extent for uranium and thorium. The most important oxidation states for WIPP-relevant conditions are III and IV. We will present an update of the literature on WIPP-specific data, and a summary of the ongoing research related to actinide chemistry in the WIPP performed by the Los Alamos National Laboratory (LANL) Actinide Chemistry and Repository Science (ACRSP) team located in Carlsbad, NM [Reed 2007, Lucchini 2007, and Reed 2006].

  5. Reversed-phase liquid chromatography using mandelic acid as an eluent for the determination of uranium in presence of large amounts of thorium.

    PubMed

    Jaison, P G; Telmore, Vijay M; Kumar, Pranaw; Aggarwal, Suresh K

    2009-02-27

    Studies were carried out for the separation of uranium (U) and thorium (Th) on reversed-phase (RP) C18 columns using mandelic acid as an eluent. Retention of thorium-mandelate on the unmodified stationary phase was found to be greater than that of uranyl-mandelate under the pH conditions employed. Th retention capacity of the stationary phase was determined as a function of pH and MeOH content of the mobile phase. The optimised parameters allowing U elution prior to Th were utilized for the determination of small amounts of U in the presence of large amounts of Th. The method has been used for the determination of U in synthetic samples with Th/U amount ratios up to 100,000 (10 microg/g of U) without any pre-separation, employing a particulate C18 column. Effect of concentration of ion interaction reagents (IIRs) on the retention was studied to understand the mechanism of adsorption of their mandelate complexes onto the stationary phase. The experiments conducted unequivocally prove that thorium-mandelate complex is neutral whereas uranyl-mandelate complex is anionic in nature.

  6. Impact of vegetation change on the mobility of uranium- and thorium-series nuclides in soils

    NASA Astrophysics Data System (ADS)

    Gontier, A.; Rihs, S.; Turpault, M.-P.; Chabaux, F.

    2012-04-01

    The effect of land cover change on chemical mobility and soil response was investigated using short- and long-lived nuclides from the U- and Th series. Indeed, the matching of these nuclides half-live to the pedogenic processes rates make these nuclides especially suitable to investigate either time or mechanism of transfers within a soil-water-plant system. This study was carried out from the experimental Breuil-Chenue site (Morvan mountains, France). The native forest (150 year-old) was partially clear-felled and replaced in 1976 by mono-specific plantations distributed in different stands. Following this cover-change, some mineralogical changes in the acid brown soil were recognized (Mareschal, 2008). Three soil sections were sampled under the native forest and the replanted oak and Douglas spruce stands respectively. The (238U), (234U), (230Th), (226Ra), (232Th) and (228Ra) activities were analysed by thermal ionization mass spectrometry (TIMS), inductively coupled plasma mass spectrometry (MC-ICPMS) and gamma spectrometry. Significant differences in U, Th, and Ra activities were observed between the soils located under the native forest or the replanted-trees stands, mostly dominated by a large uranium mobilization from the replanted soils. Moreover, all the investigated U and Th-series activity ratios show a contrasted trend between the shallowest horizons (0-50cm) and the deepest one (below 50cm), demonstrating the chemical effect of the vegetation change on the shallow soil layers. Using a continuous open-system leaching model, the coupled radioactive disequilibria measured in the different soil layers permit to quantify the rate of the radionuclides mobilities. Reference: Mareschal, L., 2008. Effet des substitutions d'essences forestières sur l'évolution des sols et de leur minéralogie : bilan après 28 ans dans le site expérimental de Breuil (Morvan) Université Henri Poincaré, Nancy-I.

  7. Distribution and mobility of uranium and thorium in the Peralkaline Soldier Meadow Tuff, Northerwestern Nevada

    SciTech Connect

    Stuart, E.J.; Bornhorst, T.J.; Noble, D.C.; Rose, W.J.

    1983-03-01

    The peralkaline Soldier Meadow Tuff represents a differentiated magma body which had two-fold variations in the amounts of Zr, Fe, Rb, Th, and U. The initial Th/U ratio for the unit was about 2.5. Primarily crystallized specimens of the Soldier Meadow Tuff show as much as 85 percent U loss; average loss is about 50 percent. In general, less U was lost from oxidized rocks in which U is concentrated in and around altered ferromagnesian minerals. Some Th loss (greater than or equal to40%) probably occurred from the lava member; this may be the result of unusually long periods of high temperature during granophyric crystallization. Variable amounts of F, La, Y, and Pb also were preferentially lost from crystallized samples of the formation. Variably hydrated glassy samples have lost little or no U and Th, confirming the results of earlier studies. Based on our data and volume estimates of Korringa (1973), we estimate that 5 million tons or more of U were lost from the Soldier Meadow Tuff, making this a possible important source rock for uranium deposits. The data does not permit an estimate of the timing of U loss. If the loss occurred gradually after crystallization (Zielinski, 1978), then the probability of forming a U deposit seems less than if the loss occurred over a short time span during and/or immediately after crystallization. The conclusions drawn in this paper are applicable to rocks of peralkalic affinity and may not apply to the volumetrically more important volcanics of subalkalic composition that occur in the western United States.

  8. Performance of Thorium-Based Mixed Oxide Fuels for the Consumption of Plutonium in Current and Advanced Reactors

    SciTech Connect

    Weaver, Kevan Dean; Herring, James Stephen

    2003-07-01

    A renewed interest in thorium-based fuels has arisen lately based on the need for proliferation resistance, longer fuel cycles, higher burnup, and improved waste form characteristics. Recent studies have been directed toward homogeneously mixed, heterogeneously mixed, and seed-and-blanket thorium-uranium oxide fuel cycles that rely on "in situ" use of the bred-in 233U. However, due to the higher initial enrichment required to achieve acceptable burnups, these fuels are encountering economic constraints. Thorium can nevertheless play a large role in the nuclear fuel cycle, particularly in the reduction of plutonium inventories. While uranium-based mixed-oxide (MOX) fuel will decrease the amount of plutonium in discharged fuel, the reduction is limited due to the breeding of more plutonium (and higher actinides) from the 238U. Here, we present calculational results and a comparison of the potential burnup of a thorium-based and uranium-based mixed-oxide fuel in a light water reactor. Although the uranium-based fuels outperformed the thorium-based fuels in achievable burnup, a depletion comparison of the initially charged plutonium (both reactor and weapons grade) showed that the thorium-based fuels outperformed the uranium-based fuels by more that a factor of 2, where >70% of the total plutonium in the thorium-based fuel is consumed during the cycle. This is significant considering that the achievable burnups of the thorium-based fuels were 1.4 to 4.6 times less than the uranium-based fuels for similar plutonium enrichments. For equal specific burnups of ~60 MWd/kg (i.e., using variable plutonium weight percentages to give the desired burnup), the thorium-based fuels still outperform the uranium-based fuels by more than a factor of 2, where the total plutonium consumption in a three-batch, 18-month cycle was 60 to 70%. This is fairly significant considering that 10 to 15% (by weight) more plutonium is needed in the thorium-based fuels as compared to the uranium

  9. Thorium Energy Futures

    SciTech Connect

    Peggs, Stephen; Roser, Thomas; Parks, G; Lindroos, Mats; Seviour, Rebecca; Henderson, Stuart; Barlow, R; Cywinski, R; Biarrote, J -L; Norlin, A; Ashley, V; Ashworth, R; Hutton, Andrew; Owen, H; McIntyre, Peter; Kelly, J

    2012-07-01

    The potential for thorium as an alternative or supplement to uranium in fission power generation has long been recognised, and several reactors, of various types, have already operated using thorium-based fuels. Accelerator Driven Subcritical (ADS) systems have benefits and drawbacks when compared to conventional critical thorium reactors, for both solid and molten salt fuels. None of the four options - liquid or solid, with or without an accelerator - can yet be rated as better or worse than the other three, given today's knowledge. We outline the research that will be necessary to lead to an informed choice.

  10. Laboratory Enrichment of Radioactive Assemblages and Estimation of Thorium and Uranium Radioactivity in Fractions Separated from Placer Sands in Southeast Bangladesh

    SciTech Connect

    Sasaki, Takayuki; Rajib, Mohammad; Akiyoshi, Masafumi; Kobayashi, Taishi; Takagi, Ikuji; Fujii, Toshiyuki; Zaman, Md. Mashrur

    2015-06-15

    The present study reports the likely first attempt of separating radioactive minerals for estimation of activity concentration in the beach placer sands of Bangladesh. Several sand samples from heavy mineral deposits located at the south-eastern coastal belt of Bangladesh were processed to physically upgrade their radioactivity concentrations using plant and laboratory equipment. Following some modified flow procedure, individual fractions were separated and investigated using gamma-ray spectrometry and powder-XRD analysis. The radioactivity measurements indicated contributions of the thorium and uranium radioactive series and of {sup 40}K. The maximum values of {sup 232}Th and {sup 238}U, estimated from the radioactivity of {sup 208}Tl and {sup 234}Th in secular equilibrium, were found to be 152,000 and 63,300 Bq/kg, respectively. The fraction of the moderately conductive part in electric separation contained thorium predominantly, while that of the non-conductive part was found to be uranium rich. The present arrangement of the pilot plant cascade and the fine tuning of setting parameters were found to be effective and economic separation process of the radioactive minerals from placer sands in Bangladesh. Probable radiological impacts and extraction potentiality of such radioactive materials are also discussed.

  11. Kinetic, equilibrium and thermodynamic studies on sorption of uranium and thorium from aqueous solutions by a selective impregnated resin containing carminic acid.

    PubMed

    Rahmani-Sani, Abolfazl; Hosseini-Bandegharaei, Ahmad; Hosseini, Seyyed-Hossein; Kharghani, Keivan; Zarei, Hossein; Rastegar, Ayoob

    2015-04-09

    In this work, the removal of uranium and thorium ions from aqueous solutions was studied by solid-liquid extraction using an advantageous extractant-impregnated resin (EIR) prepared by loading carminic acid (CA) onto Amberlite XAD-16 resin beads. Batch sorption experiments using CA/XAD-16 beads for the removal of U(VI) and Th(IV) ions were carried out as a function of several parameters, like equilibration time, metal ion concentration, etc. The equilibrium data obtained from the sorption experiments were adjusted to the Langmuir isotherm model and the calculated maximum sorption capacities in terms of monolayer sorption were in agreement with those obtained from the experiments. The experimental data on the sorption behavior of both metal ions onto the EIR beads fitted well in both Bangham and intra-particle diffusion kinetic models, indicating that the intra-particle diffusion is the rate-controlling step. The thermodynamic studies at different temperatures revealed the feasibility and the spontaneous nature of the sorption process for both uranium and thorium ions.

  12. 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

  13. Uranium-238, Thorium-232, Potassium-40 and Cesium-137 in the surface layers of soils from Lehliu area, Romania

    NASA Astrophysics Data System (ADS)

    Ion, Adriana

    2014-05-01

    Cs-137 from soil decreases with depth, clay minerals and soils rich in exchangeable potassium adsorb cesium by binding the cations to interlayer positions of the clay particles. Unlike uranium which is mobile element in soil surface, thorium, potassium and cesium has low mobility and their concentrations in soil reflect these variation in parental material, their distribution in soil being dependents by pH, organic matter content, clay minerals from soils.

  14. Distribution and transport of radionuclides in a boreal mire--assessing past, present and future accumulation of uranium, thorium and radium.

    PubMed

    Lidman, Fredrik; Ramebäck, Henrik; Bengtsson, Åsa; Laudon, Hjalmar

    2013-07-01

    The spatial distribution of (238)U, (226)Ra, (40)K and the daughters of (232)Th, (228)Ra and (228)Th, were measured in a small mire in northern Sweden. High activity concentrations of (238)U and (232)Th (up to 41 Bq (238)U kg(-1)) were observed in parts of the mire with a historical or current inflow of groundwater from the surrounding till soils, but the activities declined rapidly further out in the mire. Near the outlet and in the central parts of the mire the activity concentrations were low, indicating that uranium and thorium are immobilized rapidly upon their entering the peat. The (226)Ra was found to be more mobile with high activity concentrations further out into the mire (up to 24 Bq kg(-1)), although the central parts and the area near the outlet of the mire still had low activity concentrations. Based on the fluxes to and from the mire, it was estimated that approximately 60-70% of the uranium and thorium entering the mire currently is retained within it. The current accumulation rates were found to be consistent with the historical accumulation, but possibly lower. Since much of the accumulation still is concentrated to the edges of the mire and the activities are low compared to other measurements of these radionuclides in peat, there are no indications that the mire will be saturated with respect to radionuclides like uranium, thorium and radium in the foreseen future. On the contrary, normal peat growth rates for the region suggest that the average activity concentrations of the peat currently may be decreasing, since peat growth may be faster than the accumulation of radionuclides. In order to assess the total potential for accumulation of radionuclides more thoroughly it would, however, be necessary to also investigate the behaviour of other organophilic elements like aluminium, which are likely to compete for binding sites on the organic material. Measurements of the redox potential and other redox indicators demonstrate that uranium possibly

  15. REE, Uranium (U) and Thorium (Th) contents in Betula pendula leaf growing around Komsomolsk gold concentration plant tailing (Kemerovo region, Western Siberia, Russia)

    NASA Astrophysics Data System (ADS)

    Yusupov, D. V.; Karpenko, Yu A.

    2016-09-01

    The article deals with the research findings of peculiarities of REE, Uranium and Thorium distribution in the territory surrounding the tailing of former Komsomolsk gold concentration plant according to the data from Betula pendula leaf testing. In the leaf element composition the slight deficiency of MREE and substantial excess of HREE are presented. In the nearest impacted area around the tailing, La, Yb, U and Th content, and Th/U ratio are lower than in the distant buffer area. It is shown, that value of Th/U ratio and REE can be an indicator for geochemical transformations of technogenic landscapes in mining districts. The results of the research can be used for biomonitoring of the territory around the tailing.

  16. Triamidoamine thorium-arsenic complexes with parent arsenide, arsinidiide and arsenido structural motifs

    NASA Astrophysics Data System (ADS)

    Wildman, Elizabeth P.; Balázs, Gábor; Wooles, Ashley J.; Scheer, Manfred; Liddle, Stephen T.

    2017-03-01

    Despite a major expansion of uranium-ligand multiple bond chemistry in recent years, analogous complexes involving other actinides (An) remain scarce. For thorium, under ambient conditions only a few multiple bonds to carbon, nitrogen, phosphorus and chalcogenides are reported, and none to arsenic are known; indeed only two complexes with thorium-arsenic single bonds have been structurally authenticated, reflecting the challenges of stabilizing polar linkages at the large thorium ion. Here, we report thorium parent-arsenide (ThAsH2), -arsinidiides (ThAs(H)K and ThAs(H)Th) and arsenido (ThAsTh) linkages stabilized by a bulky triamidoamine ligand. The ThAs(H)K and ThAsTh linkages exhibit polarized-covalent thorium-arsenic multiple bonding interactions, hitherto restricted to cryogenic matrix isolation experiments, and the AnAs(H)An and AnAsAn linkages reported here have no precedent in f-block chemistry. 7s, 6d and 5f orbital contributions to the Th-As bonds are suggested by quantum chemical calculations, and their compositions unexpectedly appear to be tensioned differently compared to phosphorus congeners.

  17. Promises and Challenges of Thorium Implementation for Transuranic Transmutation - 13550

    SciTech Connect

    Franceschini, F.; Lahoda, E.; Wenner, M.; Lindley, B.; Fiorina, C.; Phillips, C.

    2013-07-01

    This paper focuses on the challenges of implementing a thorium fuel cycle for recycle and transmutation of long-lived actinide components from used nuclear fuel. A multi-stage reactor system is proposed; the first stage consists of current UO{sub 2} once-through LWRs supplying transuranic isotopes that are continuously recycled and burned in second stage reactors in either a uranium (U) or thorium (Th) carrier. The second stage reactors considered for the analysis are Reduced Moderation Pressurized Water Reactors (RMPWRs), reconfigured from current PWR core designs, and Fast Reactors (FRs) with a burner core design. While both RMPWRs and FRs can in principle be employed, each reactor and associated technology has pros and cons. FRs have unmatched flexibility and transmutation efficiency. RMPWRs have higher fuel manufacturing and reprocessing requirements, but may represent a cheaper solution and the opportunity for a shorter time to licensing and deployment. All options require substantial developments in manufacturing, due to the high radiation field, and reprocessing, due to the very high actinide recovery ratio to elicit the claimed radiotoxicity reduction. Th reduces the number of transmutation reactors, and is required to enable a viable RMPWR design, but presents additional challenges on manufacturing and reprocessing. The tradeoff between the various options does not make the choice obvious. Moreover, without an overarching supporting policy in place, the costly and challenging technologies required inherently discourage industrialization of any transmutation scheme, regardless of the adoption of U or Th. (authors)

  18. Mineral resource assessment of rare-earth elements, thorium, titanium, and uranium in the Greenville 1 degree by 2 degrees Quadrangle, South Carolina, Georgia, and North Carolina

    USGS Publications Warehouse

    Lesure, Frank G.; Curtin, Gary C.; Daniels, David L.; Jackson, John C.

    1993-01-01

    Mineral resources of the Greenville 1° x 2° quadrangle, South Carolina, Georgia, and North Carolina, were assessed between 1984 and 1990 under the Conterminuous United States Mineral Assessment Program (CUSMAP) of the U.S. Geological Survey (USGS). The mineral resource assessments were made on the basis of geologic, geochemical, and geophysical investigations and the presence of mines, prospects, and mineral occurrences from the literature. This report is an assessment of the rare-earth elements (REE), thorium, titanium, and uranium resources in the Greenville quadrangle and is based on heavy mineral concentrates collected in 1951-54 by the USGS (Overstreet and others, 1968; Caldwell and White, 1973; Cuppels and White, 1973); on the results of the U.S. Department of Energy, National Uranium Resource Evaluation (NURE) sampling program (Ferguson, 1978, 1979); on analyses of stream-sediment and heavy-mineral-concentrate samples (Jackson and Moore, 1992, G.C Cullin, USGS, unpub. data, 1992) on maps showing aerial gamma radiation in the Greenville quadrangle (D.L. Daniels, USGS, unpub. data, 1992); and on the geology as mapped by Nelson and others (1987, 1989).

  19. 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.

  20. Simultaneous spectrophotometric determination of trace amounts of uranium, thorium, and zirconium using the partial least squares method after their preconcentration by alpha-benzoin oxime modified Amberlite XAD-2000 resin.

    PubMed

    Ghasemi, Jahan B; Zolfonoun, E

    2010-01-15

    A new solid phase extraction method for separation and preconcentration of trace amounts of uranium, thorium, and zirconium in water samples is proposed. The procedure is based on the adsorption of U(VI), Th(IV) and Zr(IV) ions on a column of Amberlite XAD-2000 resin loaded with alpha-benzoin oxime prior to their simultaneous spectrophotometric determination with Arsenazo III using orthogonal signal correction partial least squares method. The enrichment factor for preconcentration of uranium, thorium, and zirconium was found to be 100. The detection limits for U(VI), Th(IV) and Zr(IV) were 0.50, 0.54, and 0.48microgL(-1), respectively. The precision of the method, evaluated as the relative standard deviation obtained by analyzing a series of 10 replicates, was below 4% for all elements. The practical applicability of the developed sorbent was examined using synthetic seawater, natural waters and ceramic samples.

  1. Thorium: Crustal abundance, joint production, and economic availability

    SciTech Connect

    Jordan, Brett W.; Eggert, Roderick G.; Dixon, Brent W.; Carlsen, Brett W.

    2015-03-02

    Recently, interest in thorium's potential use in a nuclear fuel cycle has been renewed. Thorium is more abundant, at least on average, than uranium in the earth's crust and, therefore, could theoretically extend the use of nuclear energy technology beyond the economic limits of uranium resources. This paper provides an economic assessment of thorium availability by creating cumulative-availability and potential mining-industry cost curves, based on known thorium resources. These tools provide two perspectives on the economic availability of thorium. In the long term, physical quantities of thorium likely will not be a constraint on the development of a thorium fuel cycle. In the medium term, however, thorium supply may be limited by constraints associated with its production as a by-product of rare earth elements and heavy mineral sands. As a result, environmental concerns, social issues, regulation, and technology also present issues for the medium and long term supply of thorium.

  2. Thorium: Crustal abundance, joint production, and economic availability

    DOE PAGES

    Jordan, Brett W.; Eggert, Roderick G.; Dixon, Brent W.; ...

    2015-03-02

    Recently, interest in thorium's potential use in a nuclear fuel cycle has been renewed. Thorium is more abundant, at least on average, than uranium in the earth's crust and, therefore, could theoretically extend the use of nuclear energy technology beyond the economic limits of uranium resources. This paper provides an economic assessment of thorium availability by creating cumulative-availability and potential mining-industry cost curves, based on known thorium resources. These tools provide two perspectives on the economic availability of thorium. In the long term, physical quantities of thorium likely will not be a constraint on the development of a thorium fuelmore » cycle. In the medium term, however, thorium supply may be limited by constraints associated with its production as a by-product of rare earth elements and heavy mineral sands. As a result, environmental concerns, social issues, regulation, and technology also present issues for the medium and long term supply of thorium.« less

  3. Thorium-Based Transmuter Fuels for Light Water Reactors

    SciTech Connect

    J. Stephen Herring; P. E. MacDonald; K. Weaver

    2004-04-01

    A light water reactor (LWR) fuel cycle is proposed where the reactor core mainly consists of standard uranium-dioxide (UO2) fuel rods with typical 235U enrichment, along with thoria-urania (ThO2-UO2) or yttria-stablized zirconia fertile-free fuel rods containing the plutonium and minor actinides typical of 30-yr old UO2 fuel in 1/9 to 1/3 of the positions. The goals of this mono-recycling strategy or "twice through fuel cycle" are to transmute the great majority of the long lived actinides in existing LWRs and to discharge a fuel form that is a very robust waste form and whose isotopic content is very proliferation resistant. The incorporation of plutonium into a ThO2 or yttria-stablized zirconia fertile-free matrix results in the consumption of already-separated plutonium without breeding significant additional 239Pu. The minor actinides (i.e., neptunium, americium, curium, berkelium, californium, etc.) are also included in the ThO2 or fertile-free transmuter fuel rods to further reduce the overall long-term radiotoxicity of the fuel cycle. Our analyses have shown that thorium-based or fertile-free fuels can reduce the amount of 239Pu needing further transmutation or going to a repository by ~90%. Also, thorium-based fuels produce a mixture of plutonium isotopes high in 238Pu. Because of the high decay heat and spontaneous neutron generation of 238Pu, this isotope provides intrinsic proliferation resistance.

  4. Thorium-Based Transmuter Fuels for Light Water Reactors

    SciTech Connect

    Herring, J. Stephen; MacDonald, Philip E.; Weaver, Kevan D.

    2004-07-15

    A light water reactor (LWR) fuel cycle is proposed where the reactor core mainly consists of standard uranium-dioxide (UO{sub 2}) fuel rods with typical {sup 235}U enrichment, along with thoria-urania (ThO{sub 2}-UO{sub 2}) or yttria-stablized zirconia fertile-free fuel rods containing the plutonium and minor actinides typical of 30-yr old UO{sub 2} fuel in 1/9 to 1/3 of the positions. The goals of this mono-recycling strategy or 'twice through fuel cycle' are to transmute the great majority of the long lived actinides in existing LWRs and to discharge a fuel form that is a very robust waste form and whose isotopic content is very proliferation resistant. The incorporation of plutonium into a ThO{sub 2} or yttria-stablized zirconia fertile-free matrix results in the consumption of already-separated plutonium without breeding significant additional {sup 239}Pu. The minor actinides (i.e., neptunium, americium, curium, berkelium, californium, etc.) are also included in the ThO{sub 2} or fertile-free transmuter fuel rods to further reduce the overall long-term radiotoxicity of the fuel cycle. Our analyses have shown that thorium-based or fertile-free fuels can reduce the amount of {sup 239}Pu needing further transmutation or going to a repository by {approx}90%. Also, thorium-based fuels produce a mixture of plutonium isotopes high in {sup 238}Pu. Because of the high decay heat and spontaneous neutron generation of {sup 238}Pu, this isotope provides intrinsic proliferation resistance.

  5. SEPARATION PROCESS FOR THORIUM SALTS

    DOEpatents

    Bridger, G.L.; Whatley, M.E.; Shaw, K.G.

    1957-12-01

    A process is described for the separation of uranium, thorium, and rare earths extracted from monazite by digesting with sulfuric acid. By carefully increasing the pH of the solution, stepwise, over the range 0.8 to 5.5, a series of selective precipitations will be achieved, with the thorium values coming out at lower pH, the rare earths at intermediate pH and the uranium last. Some mixed precipitates will be obtained, and these may be treated by dissolving in HNO/sub 3/ and contacting with dibutyl phosphate, whereby thorium or uranium are taken up by the organic phase while the rare earths preferentially remain in the aqueous solution.

  6. High-precision measurements of uranium and thorium isotopic ratios by multi-collector inductively coupled plasma mass spectrometry (MC-ICPMS)

    NASA Astrophysics Data System (ADS)

    Wang, Lisheng; Ma, Zhibang; Duan, Wuhui

    2015-04-01

    Isotopic compositions of U-Th and 230Th dating have been widely used in earth sciences, such as chronology, geochemistry, oceanography and hydrology. In this study, five ages of different carbonate samples were measured using 230Th dating technique with U-Th high-precision isotopic measurements by multi-collector inductively coupled plasma mass spectrometry, in Uranium-series Chronology Laboratory, Institute of Geology and Geophysics, Chinese Academy of Sciences.In this study, the precision and accuracy of uranium isotopic composition were estimated by measuring the uranium ratios of NBS-CRM 112A, NBS-CRM U500 and HU-1. The mean measured ratios, 234U/238U = 52.86 (±0.04) × 10-6 and δ234U = -38.36 (±0.77) × 10-3 for NBS-CRM 112A, 234U/238U = 10.4184 (±0.0001) × 10-3, 236U/238U = 15.43 (±0.01) × 10-4 and 238U/235U = 1.00021 (±0.00002) for NBS-CRM U500, 234U/238U = 54.911 (±0.007) and δ234U = -1.04 (±0.13) × 10-3 for HU-1 (95% confidence levels). The U isotope data for standard reference materials are in excellent agreement with previous studies, further highlighting the reliability and analytical capabilities of our technique. We measured the thorium isotopic ratios of three different thorium standards by MC-ICPMS. The three standards (Th-1, Th-2 and Th-3) were mixed by HU-1 and NBS 232Th standard, with the 230Th/232Th ratios from 10-4 to 10-6. The mean measured atomic ratios, 230Th/232Th = 2.1227 (±0.0024) × 10-6, 2.7246 (±0.0026) × 10-5, and 2.8358 (±0.0007) × 10-4 for Th-1, Th-2 and Th-3 (95% confidence levels), respectively. Using this technique, the following standard samples were dated by MC-ICPMS. Sample RKM-4, collected from Babardos Kendal Hill terrace, was used during the first stage of the Uranium-Series Intercomparison Project (USIP-I). Samples 76001, RKM-5 and RKM-6 were studied during the second stage of the USIP program (USIP-II). Sample 76001 is a laminated flowstone, collected from Sumidero Terejapa, Chiapas, Mexico, and samples

  7. MANTRA: An Integral Reactor Physics Experiment to Infer Actinide Capture Cross-sections from Thorium to Californium with Accelerator Mass Spectrometry

    SciTech Connect

    G. Youinou; C. McGrath; G. Imel; M. Paul; R. Pardo; F. Kondev; M. Salvatores; G. Palmiotti

    2011-08-01

    The principle of the proposed experiment is to irradiate very pure actinide samples in the Advanced Test Reactor at INL and, after a given time, determine the amount of the different transmutation products. The determination of the nuclide densities before and after neutron irradiation will allow inference of effective neutron capture cross-sections. This approach has been used in the past and the novelty of this experiment is that the atom densities of the different transmutation products will be determined using the Accelerator Mass Spectrometry technique at the ATLAS facility located at ANL. It is currently planned to irradiate the following isotopes: 232Th, 235U, 236U, 238U, 237Np, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, 241Am, 243Am, 244Cm and 248Cm.

  8. Effect of successive alkylation of N,N-dialkyl amides on the complexation behavior of uranium and thorium: solvent extraction, small angle neutron scattering, and computational studies.

    PubMed

    Verma, Parveen Kumar; Pathak, Priyanath N; Kumari, Neelam; Sadhu, Biswajit; Sundararajan, Mahesh; Aswal, Vinod Kumar; Mohapatra, Prasanta Kumar

    2014-12-11

    The effect of successive alkylation of the Cα atom adjacent to the carbonyl group in N,N-dialkyl amides (i.e., di(2-ethylhexyl)acetamide (D2EHAA), di(2-ethylhexyl)propionamide (D2EHPRA), di(2-ethylhexyl)isobutyramide (D2EHIBA), and di(2-ethylhexyl)pivalamide (D2EHPVA)) on the extraction behavior of hexavalent uranium (U(VI)) and tetravalent thorium (Th(IV)) ions has been investigated. These studies show that the extraction of Th(IV) is significantly suppressed compared to that of U(VI) with increased branching at the Cα atom adjacent to the carbonyl group. Small angle neutron scattering (SANS) studies showed an increased aggregation tendency in the presence of nitric acid and metal ions. D2EHAA showed more aggregation compared to its branched homologues, which explains its capacity for higher extraction of metal ions. These experimental observations were further supported by density function theory calculations, which provided structural evidence of differential binding affinities of these extractants for uranyl cations. The complexation process is primarily controlled by steric and electronic effects. Quantum chemical calculations showed that local hardness and polarizability can be extremely useful inputs for designing novel extractants relevant to a nuclear fuel cycle.

  9. Behavior and distribution of heavy metals including rare Earth elements, thorium, and uranium in sludge from industry water treatment plant and recovery method of metals by biosurfactants application.

    PubMed

    Gao, Lidi; Kano, Naoki; Sato, Yuichi; Li, Chong; Zhang, Shuang; Imaizumi, Hiroshi

    2012-01-01

    In order to investigate the behavior, distribution, and characteristics of heavy metals including rare earth elements (REEs), thorium (Th), and uranium (U) in sludge, the total and fractional concentrations of these elements in sludge collected from an industry water treatment plant were determined and compared with those in natural soil. In addition, the removal/recovery process of heavy metals (Pb, Cr, and Ni) from the polluted sludge was studied with biosurfactant (saponin and sophorolipid) elution by batch and column experiments to evaluate the efficiency of biosurfactant for the removal of heavy metals. Consequently, the following matters have been largely clarified. (1) Heavy metallic elements in sludge have generally larger concentrations and exist as more unstable fraction than those in natural soil. (2) Nonionic saponin including carboxyl group is more efficient than sophorolipid for the removal of heavy metals in polluted sludge. Saponin has selectivity for the mobilization of heavy metals and mainly reacts with heavy metals in F3 (the fraction bound to carbonates) and F5 (the fraction bound to Fe-Mn oxides). (3) The recovery efficiency of heavy metals (Pb, Ni, and Cr) reached about 90-100% using a precipitation method with alkaline solution.

  10. Ethyl thiosemicarbazide intercalated organophilic calcined hydrotalcite as a potential sorbent for the removal of uranium(VI) and thorium(IV) ions from aqueous solutions.

    PubMed

    Anirudhan, T S; Jalajamony, S

    2013-04-01

    This work was conducted to determine the practicability of using a new adsorbent 4-ethyl thiosemicarbazide intercalated, organophilic calcined hydrotalcite (ETSC-OHTC) for the removal of uranium (U(VI)), and thorium (Th(IV)) from water and wastewater. The FTIR analysis helped in realizing the involvement of nitrogen and sulphur atoms of ETSC in binding the metal ions through complex formation. Parameters like adsorbent dosage, solution pH, initial metal ions concentration, contact time and ionic strength, that influence adsorption phenomenon, were studied. The optimum pH for maximum adsorption of U(VI) and Th(IV) was found to be in the range 4.0-6.0. The contact time required for reaching equilibrium was 4 hr. The pseudo second-order kinetic model was the best fit to represent the kinetic data. Analysis of the equilibrium adsorption data using Langmuir, Freundlich and Sips models showed that the Freundlich model was well suited to describe the metal ions adsorption. The K(F) values were 25.43 and 29.11 mg/g for U(VI) and Th(IV), respectively, at 30 degrees C. The adsorbent can be regenerated effectively from U(VI) and Th(IV) loaded ones using 0.01 mol/L HCl. The new adsorbent was quite stable for many cycles, without much reduction in its adsorption capacity towards the metals.

  11. ALPHA SPECTROMETRIC EVALUATION OF SRM-995 AS A POTENTIAL URANIUM/THORIUM DOUBLE TRACER SYSTEM FOR AGE-DATING URANIUM MATERIALS

    SciTech Connect

    Beals, D.

    2011-12-06

    Uranium-233 (t{sub 1/2} {approx} 1.59E5 years) is an artificial, fissile isotope of uranium that has significant importance in nuclear forensics. The isotope provides a unique signature in determining the origin and provenance of uranium-bearing materials and is valuable as a mass spectrometric tracer. Alpha spectrometry was employed in the critical evaluation of a {sup 233}U standard reference material (SRM-995) as a dual tracer system based on the in-growth of {sup 229}Th (t{sub 1/2} {approx} 7.34E3 years) for {approx}35 years following radiochemical purification. Preliminary investigations focused on the isotopic analysis of standards and unmodified fractions of SRM-995; all samples were separated and purified using a multi-column anion-exchange scheme. The {sup 229}Th/{sup 233}U atom ratio for SRM-995 was found to be 1.598E-4 ({+-} 4.50%) using recovery-corrected radiochemical methods. Using the Bateman equations and relevant half-lives, this ratio reflects a material that was purified {approx} 36.8 years prior to this analysis. The calculated age is discussed in contrast with both the date of certification and the recorded date of last purification.

  12. 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.

  13. 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.

  14. REGENERATION OF FISSION-PRODUCT-CONTAINING MAGNESIUM-THORIUM ALLOYS

    DOEpatents

    Chiotti, P.

    1964-02-01

    A process of regenerating a magnesium-thorium alloy contaminated with fission products, protactinium, and uranium is presented. A molten mixture of KCl--LiCl-MgCl/sub 2/ is added to the molten alloy whereby the alkali, alkaline parth, and rare earth fission products (including yttrium) and some of the thorium and uranium are chlorinated and

  15. Solvent extraction of thorium(IV), uranium(VI), and europium(III) with lipophilic alkyl-substituted pyridinium salts. Final report for subcontract 9-XZ2-1123E-1, June 1, 1992--December 1, 1995

    SciTech Connect

    Ensor, D.D.

    1997-01-01

    In the treatment of high level nuclear wastes, aromatic pyridinium salts which are radiation-resistant are desired for the extraction of actinides and lanthanides. The solvent extraction of Th{sup +4}, UO{sub 2}{sup +2}, and Eu{sup +3} by three aromatic extractants, 3,5-didodecylpyridinium nitrate (35PY), 2,6-didodecylpyridinium nitrate (26PY), and 1-methyl-3,5-didodecyl-pyridinium iodide (1M35PY) has been studied in nitric acid media. The general order of extractability of the three extractants in toluene was 1M35PY>> 26PY > 35PY. The overall extraction efficiency of the metal ions was Th{sup +4} >UO{sub 2}{sup +2} > Eu{sup +3}. The extraction of HNO{sub 3}, which was competitive with the extraction of metal ions, was quantitatively investigated by NaOH titration and UV spectrometry. The loading capacity suggested that the extracted species in the organic phase for thorium was (R{sub 4}N{sup +}){sub 2}Th(NO{sub 3}{sup -}){sub 6}, where R{sub 4}N{sup +} denotes 1M35PY. A comparison of 1M35PY to the well-characterized extractant, Aliquat-336, an aliphatic ammonium salt was made. At the same extractant concentration, 1M35PY extracted thorium more efficiently than Aliquat-336 at high acidity. Thorium could be readily stripped with dilute nitric acid from 1M35PY. After irradiation of 0.1M 1M35PY with {sup 60}Co at 40R/min for 48 hours, no change in the extraction efficiency of thorium was observed.

  16. Tetrapositive plutonium, neptunium, uranium, and thorium coordination complexes: chemistry revealed by electron transfer and collision induced dissociation.

    PubMed

    Gong, Yu; Tian, Guoxin; Rao, Linfeng; Gibson, John K

    2014-04-17

    The Pu(4+), Np(4+), and U(4+) ions, which have large electron affinities of ∼34.6, ∼33.6, and ∼32.6 eV, respectively, were stabilized from solution to the gas phase upon coordination by three neutral tetramethyl-3-oxa-glutaramide ligands (TMOGA). Both collision induced dissociation (CID) and electron transfer dissociation (ETD) of Pu(TMOGA)3(4+) reveal the propensity for reduction of Pu(IV) to Pu(III), by loss of TMOGA(+) in CID and by simple electron transfer in ETD. The reduction of Pu(IV) is in distinct contrast to retention of Th(IV) in both CID and ETD of Th(TMOGA)3(4+), where only the C-Oether bond cleavage product was observed. U(TMOGA)3(4+) behaves similarly to Th(TMOGA)3(4+) upon CID and ETD, while the fragmentation patterns of Np(TMOGA)3(4+) lie between those of Pu(TMOGA)3(4+) and U(TMOGA)3(4+). It is notable that the gas-phase fragmentation behaviors of these exceptional tetrapositive complexes parallel fundamental differences in condensed phase chemistry within the actinide series, specifically the tendency for reduction from the IV to III oxidation states.

  17. Liquid fuel molten salt reactors for thorium utilization

    SciTech Connect

    Gehin, Jess C.; Powers, Jeffrey J.

    2016-04-08

    Molten salt reactors (MSRs) represent a class of reactors that use liquid salt, usually fluoride- or chloride-based, as either a coolant with a solid fuel (such as fluoride salt-cooled high temperature reactors) or as a combined coolant and fuel with fuel dissolved in a carrier salt. For liquid-fuelled MSRs, the salt can be processed online or in a batch mode to allow for removal of fission products as well as introduction of fissile fuel and fertile materials during reactor operation. The MSR is most commonly associated with the 233U/thorium fuel cycle, as the nuclear properties of 233U combined with the online removal of parasitic absorbers allow for the ability to design a thermal-spectrum breeder reactor; however, MSR concepts have been developed using all neutron energy spectra (thermal, intermediate, fast, and mixed-spectrum zoned concepts) and with a variety of fuels including uranium, thorium, plutonium, and minor actinides. Early MSR work was supported by a significant research and development (R&D) program that resulted in two experimental systems operating at ORNL in the 1960s, the Aircraft Reactor Experiment and the Molten Salt Reactor Experiment. Subsequent design studies in the 1970s focusing on thermal-spectrum thorium-fueled systems established reference concepts for two major design variants: (1) a molten salt breeder reactor (MSBR), with multiple configurations that could breed additional fissile material or maintain self-sustaining operation; and (2) a denatured molten salt reactor (DMSR) with enhanced proliferation-resistance. T MSRs has been selected as one of six most promising Generation IV systems and development activities have been seen in fast-spectrum MSRs, waste-burning MSRs, MSRs fueled with low-enriched uranium (LEU), as well as more traditional thorium fuel cycle-based MSRs. This study provides an historical background of MSR R&D efforts, surveys and summarizes many of the recent development, and provides

  18. Liquid fuel molten salt reactors for thorium utilization

    DOE PAGES

    Gehin, Jess C.; Powers, Jeffrey J.

    2016-04-08

    Molten salt reactors (MSRs) represent a class of reactors that use liquid salt, usually fluoride- or chloride-based, as either a coolant with a solid fuel (such as fluoride salt-cooled high temperature reactors) or as a combined coolant and fuel with fuel dissolved in a carrier salt. For liquid-fuelled MSRs, the salt can be processed online or in a batch mode to allow for removal of fission products as well as introduction of fissile fuel and fertile materials during reactor operation. The MSR is most commonly associated with the 233U/thorium fuel cycle, as the nuclear properties of 233U combined with themore » online removal of parasitic absorbers allow for the ability to design a thermal-spectrum breeder reactor; however, MSR concepts have been developed using all neutron energy spectra (thermal, intermediate, fast, and mixed-spectrum zoned concepts) and with a variety of fuels including uranium, thorium, plutonium, and minor actinides. Early MSR work was supported by a significant research and development (R&D) program that resulted in two experimental systems operating at ORNL in the 1960s, the Aircraft Reactor Experiment and the Molten Salt Reactor Experiment. Subsequent design studies in the 1970s focusing on thermal-spectrum thorium-fueled systems established reference concepts for two major design variants: (1) a molten salt breeder reactor (MSBR), with multiple configurations that could breed additional fissile material or maintain self-sustaining operation; and (2) a denatured molten salt reactor (DMSR) with enhanced proliferation-resistance. T MSRs has been selected as one of six most promising Generation IV systems and development activities have been seen in fast-spectrum MSRs, waste-burning MSRs, MSRs fueled with low-enriched uranium (LEU), as well as more traditional thorium fuel cycle-based MSRs. This study provides an historical background of MSR R&D efforts, surveys and summarizes many of the recent development, and provides analysis comparing

  19. 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.

  20. Advanced Proliferation Resistant, Lower Cost, Uranium-Thorium Dioxide Fuels for Light Water Reactors (Progress report for work through June 2002, 12th quarterly report)

    SciTech Connect

    Mac Donald, Philip Elsworth

    2002-09-01

    The overall objective of this NERI project is to evaluate the potential advantages and disadvantages of an optimized thorium-uranium dioxide (ThO2/UO2) fuel design for light water reactors (LWRs). The project is led by the Idaho National Engineering and Environmental Laboratory (INEEL), with the collaboration of three universities, the University of Florida, Massachusetts Institute of Technology (MIT), and Purdue University; Argonne National Laboratory; and all of the Pressurized Water Reactor (PWR) fuel vendors in the United States (Framatome, Siemens, and Westinghouse). In addition, a number of researchers at the Korean Atomic Energy Research Institute and Professor Kwangheon Park at Kyunghee University are active collaborators with Korean Ministry of Science and Technology funding. The project has been organized into five tasks: · Task 1 consists of fuel cycle neutronics and economics analysis to determine the economic viability of various ThO2/UO2 fuel designs in PWRs, · Task 2 will determine whether or not ThO2/UO2 fuel can be manufactured economically, · Task 3 will evaluate the behavior of ThO2/UO2 fuel during normal, off-normal, and accident conditions and compare the results with the results of previous UO2 fuel evaluations and U.S. Nuclear Regulatory Commission (NRC) licensing standards, · Task 4 will determine the long-term stability of ThO2/UO2 high-level waste, and · Task 5 consists of the Korean work on core design, fuel performance analysis, and xenon diffusivity measurements.

  1. Solubility of uranium and thorium from a healing earth in synthetic gut fluids: a case study for use in dose assessments.

    PubMed

    Höllriegl, Vera; Li, Wei Bo; Leopold, Karsten; Gerstmann, Udo; Oeh, Uwe

    2010-11-01

    The aim of this case study was to estimate the bioaccessibility of uranium ((238)U) and thorium ((232)Th) from a healing earth by analysing the solubility of these radionuclides in synthetic gastric and intestinal fluids. An easy applicable in vitro test system was used to investigate the fractional mobilization of the soil contaminants being potentially available for absorption under human in vivo conditions. These findings provided the basis for a prospective dose assessment. The solubility experiments were performed using two different in vitro digestion methods. The concentrations of (238)U and (232)Th in the solutions extracted from the soil were measured by inductively coupled plasma mass spectrometry (ICP-MS). The dissolved fractions in the synthetic gastrointestinal fluid ranged in average from 10.3% to 13.8% for (238)U and from 0.3% to 1.6% for (232)Th, respectively, depending on the digestion method. Subsequently, the committed effective doses from intake of (238)U and (232)Th after ingestion of the healing earth during 1 year were evaluated for adult persons. Thereby ingestion dose coefficients calculated as a function of bioaccessibility were used. The dose assessments ranged between 4.3 × 10(-7)-1.9 × 10(-6) Sv y(-1) for (238)U and 5.6 × 10(-7)-3.3 × 10(-6) Sv y(-1) for (232)Th, respectively. On the basis of the assumptions and estimations made, the present work indicates a relatively low radiation risk due to (238)U and (232)Th after internal exposure of the healing earth.

  2. Tissue studies of persons with intakes of the actinide elements: the U.S. Transuranium and Uranium Registries.

    PubMed

    Kathren, R L

    2001-01-01

    For more than three decades, the United States Transuranium and Uranium Registries (USTUR) have studied the biokinetics, dosimetry, and biological effects of plutonium, uranium, and americium through voluntary postmortem tissues from persons with known intakes. Radiochemical analyses of tissue obtained at autopsy have shown that plutonium and americium have different biokinetics and an appreciable deposition in the soft tissues of the body as well as the known depots in skeleton and liver. Studies of whole-body Thorotrast donors to the USTUR indicate that commonly accepted risk coefficients for alpha induction of bone sarcoma may be too high while those for leukemia are a factor of six too low. This review considers these and other major contributions of the USTUR.

  3. A simple-rapid method to separate uranium, thorium, and protactinium for U-series age-dating of materials.

    PubMed

    Knight, Andrew W; Eitrheim, Eric S; Nelson, Andrew W; Nelson, Steven; Schultz, Michael K

    2014-08-01

    Uranium-series dating techniques require the isolation of radionuclides in high yields and in fractions free of impurities. Within this context, we describe a novel-rapid method for the separation and purification of U, Th, and Pa. The method takes advantage of differences in the chemistry of U, Th, and Pa, utilizing a commercially-available extraction chromatographic resin (TEVA) and standard reagents. The elution behavior of U, Th, and Pa were optimized using liquid scintillation counting techniques and fractional purity was evaluated by alpha-spectrometry. The overall method was further assessed by isotope dilution alpha-spectrometry for the preliminary age determination of an ancient carbonate sample obtained from the Lake Bonneville site in western Utah (United States). Preliminary evaluations of the method produced elemental purity of greater than 99.99% and radiochemical recoveries exceeding 90% for U and Th and 85% for Pa. Excellent purity and yields (76% for U, 96% for Th and 55% for Pa) were also obtained for the analysis of the carbonate samples and the preliminary Pa and Th ages of about 39,000 years before present are consistent with (14)C-derived age of the material.

  4. URANIUM SEPARATION PROCESS

    DOEpatents

    Hyde, E.K.; Katzin, L.I.; Wolf, M.J.

    1959-07-14

    The separation of uranium from a mixture of uranium and thorium by organic solvent extraction from an aqueous solution is described. The uranium is separrted from an aqueous mixture of uranium and thorium nitrates 3 N in nitric acid and containing salting out agents such as ammonium nitrate, so as to bring ihe total nitrate ion concentration to a maximum of about 8 N by contacting the mixture with an immiscible aliphatic oxygen containing organic solvent such as diethyl carbinol, hexone, n-amyl acetate and the like. The uranium values may be recovered from the organic phase by back extraction with water.

  5. DECONTAMINATION OF URANIUM

    DOEpatents

    Feder, H.M.; Chellew, N.R.

    1958-02-01

    This patent deals with the separation of rare earth and other fission products from neutron bombarded uranium. This is accomplished by melting the uranium in contact with either thorium oxide, maguesium oxide, alumnum oxide, beryllium oxide, or uranium dioxide. The melting is preferably carried out at from 1150 deg to 1400 deg C in an inert atmosphere, such as argon or helium. During this treatment a scale of uranium dioxide forms on the uranium whtch contains most of the fission products.

  6. 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)

  7. Thorium impact on tobacco root transcriptome.

    PubMed

    Mazari, Kateřina; Landa, Přemysl; Přerostová, Sylva; Müller, Karel; Vaňková, Radomíra; Soudek, Petr; Vaněk, Tomáš

    2017-03-05

    Thorium is natural actinide metal with potential use in nuclear energetics. Contamination by thorium, originated from mining activities or spills, represents environmental risk due to its radioactivity and chemical toxicity. A promising approach for cleaning of contaminated areas is phytoremediation, which need to be based, however, on detail understanding of the thorium effects on plants. In this study we investigated transcriptomic response of tobacco roots exposed to 200μM thorium for one week. Thorium application resulted in up-regulation of 152 and down-regulation of 100 genes (p-value <0.01, fold change ≥2). The stimulated genes were involved in components of jasmonic acid and salicylic acid signaling pathways and various abiotic (e.g. oxidative stress) and biotic stress (e.g. pathogens, wounding) responsive genes. Further, up-regulation of phosphate starvation genes and down-regulation of genes involved in phytic acid biosynthesis indicated that thorium disturbed phosphate uptake or signaling. Also expression of iron responsive genes was influenced. Negative regulation of several aquaporins indicated disturbance of water homeostasis. Genes potentially involved in thorium transport could be zinc-induced facilitator ZIF2, plant cadmium resistance PCR2, and ABC transporter ABCG40. This study provides the first insight at the processes in plants exposed to thorium.

  8. 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.

  9. Metal-silicate Partitioning of Uranium and Thorium up to 138 GPa and 5500 K and Implications for Stratified Layer at the Top of the Outer Core

    NASA Astrophysics Data System (ADS)

    Nomura, R.; Hirose, K.; Kimura, J. I.; Chang, Q.

    2014-12-01

    The excess abundances of siderophile elements in the mantle can be explained by metal-silicate equilibrium at mid-mantle depths in magma ocean of the growing Earth. The final equilibrium pressure and temperature would reach 37-60 GPa and melting temperature of the mantle at this pressure (Wade et al. 2012; Siebert et al., 2013). Much severe conditions (>6000 K) have been supposed at the final stage of the Earth's formation immediate aftermath the moon-forming giant impact (e.g. Canup, 2004), evoking the additional chemical equilibrium between core materials of the giant impactor and the surrounding silicate materials. Previous studies on partitioning of U up to 20 GPa and 2700 K by multi-anvil press have shown very small partition coefficients (D ~10^-5) in S-poor system with oxygen fugacity at around IW-1.5 (Wheeler et al., 2006; Bouhifd et al., 2013). Such a very small D make it difficult to examine the partitioning at higher P-T using laser-heated diamond anvil cell (LH-DAC) and electron microprobe since the small size of each phase introduce artificial error by such as secondary fluorescent effect (Wade and Wood, 2012). 1% contamination from surrounding silicate may increase D by three orders (i.e. D =10^-2), artificially. One solution is to use laser ablation ICP-MS by carefully ablating only a metallic portion. Here, we introduced FIB to isolate the metallic phase from the surrounding silicate melt by slicing off surrounding silicate potion. Consequently, we have successfully obtained the metal-silicate partitioning data of U and Th up to 138 GPa and 5500 K in S-free/S-poor system using LH-DAC. The results show a large temperature dependence of partition coefficient of uranium and thorium, approaching to 0.1~1 at temperature near 5500 K. The pressure dependence was not observed clearly. The large temperature dependence suggests that only the core material of the giant impactor can be enriched in U and Th, which may stratify at the top of the liquid core.

  10. Uranium industry annual 1996

    SciTech Connect

    1997-04-01

    The Uranium Industry Annual 1996 (UIA 1996) provides current statistical data on the US uranium industry`s activities relating to uranium raw materials and uranium marketing. The UIA 1996 is prepared for use by the Congress, Federal and State agencies, the uranium and nuclear electric utility industries, and the public. Data on uranium raw materials activities for 1987 through 1996 including exploration activities and expenditures, EIA-estimated reserves, mine production of uranium, production of uranium concentrate, and industry employment are presented in Chapter 1. Data on uranium marketing activities for 1994 through 2006, including purchases of uranium and enrichment services, enrichment feed deliveries, uranium fuel assemblies, filled and unfilled market requirements, uranium imports and exports, and uranium inventories are shown in Chapter 2. A feature article, The Role of Thorium in Nuclear Energy, is included. 24 figs., 56 tabs.

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

    NASA Astrophysics Data System (ADS)

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

    2001-03-01

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

  12. Fabrication of thorium bearing carbide fuels

    DOEpatents

    Gutierrez, Rueben L.; Herbst, Richard J.; Johnson, Karl W. R.

    1981-01-01

    Thorium-uranium carbide and thorium-plutonium carbide fuel pellets have been fabricated by the carbothermic reduction process. Temperatures of 1750.degree. C. and 2000.degree. C. were used during the reduction cycle. Sintering temperatures of 1800.degree. C. and 2000.degree. C. were used to prepare fuel pellet densities of 87% and >94% of theoretical, respectively. The process allows the fabrication of kilogram quantities of fuel with good reproducibility of chemicals and phase composition. Methods employing liquid techniques that form carbide microspheres or alloying-techniques which form alloys of thorium-uranium or thorium-plutonium suffer from limitation on the quantities processed of because of criticality concerns and lack of precise control of process conditions, respectively.

  13. Silver Plume Granite; possible source of uranium in sandstone uranium deposits, Tallahassee Creek and High Park areas, Fremont and Teller counties, Colorado

    USGS Publications Warehouse

    Hills, F.A.; Dickinson, K.A.

    1982-01-01

    Anomalously high concentrations of thorium and of the light rare earth elements lanthanum and cerium suggest that the actinides and light lanthanides were enriched to an abnormal degree by the magmatic processes that formed the Proterozoic Y Silver Plume Granite in areas adjoining Tallahassee Creek and High Park. However, no such enrichment is found in the Proterozoic X Boulder Creek Granodiorite. Although uranium presently does not appear to be significantly enriched in sampled outcrops of Silver Plume Granite, a large part of the original uranium content of Silver Plume may have been removed by oxidizing ground waters, leaving behind mainly the uranium bound in resistate minerals such as zircon and monazite. Lead isotopic compositions of acid leachate from barren shale and sandstone associated with the Hansen uranium deposit (Tallahassee Creek area) indicate that (1) the predominant source of acid-soluble lead is 1410 m.y: old (Silver Plume age); (2) the source of the lead is characterized by Th/U around 1 (this ratio in the source may apply to soluble minerals only and may exclude thorium and uranium in resistate minerals), and the mean uranium content of this source may be as high as 30 ppm; and (3) at the time of sediment deposition, a paleohydrologic system existed that was capable of transporting Silver Plume lead and, therefore, Silver Plume uranium to the Hansen deposit. Although a significant contribution of uranium from Tertiary volcanic rocks cannot be ruled out and is even probable (Dickinson and Hills, 1982), it appears probable that some of the uranium in deposits of the Tallahassee Creek area was derived from Silver Plume Granite.

  14. Fabrication of thorium bearing carbide fuels

    DOEpatents

    Gutierrez, R.L.; Herbst, R.J.; Johnson, K.W.R.

    Thorium-uranium carbide and thorium-plutonium carbide fuel pellets have been fabricated by the carbothermic reduction process. Temperatures of 1750/sup 0/C and 2000/sup 0/C were used during the reduction cycle. Sintering temperatures of 1800/sup 0/C and 2000/sup 0/C were used to prepare fuel pellet densities of 87% and > 94% of theoretical, respectively. The process allows the fabrication of kilogram quantities of fuel with good reproductibility of chemical and phase composition.

  15. 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.

  16. Natural thorium resources and recovery: Options and impacts

    USGS Publications Warehouse

    Ault, Timothy; Van Gosen, Bradley S.; Krahn, Steven; Croff, Allen

    2016-01-01

    This paper reviews the front end of the thorium fuel cycle, including the extent and variety of thorium deposits, the potential sources of thorium production, and the physical and chemical technologies required to isolate and purify thorium. Thorium is frequently found within rare earth element–bearing minerals that exist in diverse types of mineral deposits, often in conjunction with other minerals mined for their commercial value. It may be possible to recover substantial quantities of thorium as a by-product from active titanium, uranium, tin, iron, and rare earth mines. Incremental physical and chemical processing is required to obtain a purified thorium product from thorium minerals, but documented experience with these processes is extensive, and incorporating thorium recovery should not be overly challenging. The anticipated environmental impacts of by-product thorium recovery are small relative to those of uranium recovery since existing mining infrastructure utilization avoids the opening and operation of new mines and thorium recovery removes radionuclides from the mining tailings.

  17. METHOD OF RECOVERING URANIUM COMPOUNDS

    DOEpatents

    Poirier, R.H.

    1957-10-29

    S>The recovery of uranium compounds which have been adsorbed on anion exchange resins is discussed. The uranium and thorium-containing residues from monazite processed by alkali hydroxide are separated from solution, and leached with an alkali metal carbonate solution, whereby the uranium and thorium hydrorides are dissolved. The carbonate solution is then passed over an anion exchange resin causing the uranium to be adsorbed while the thorium remains in solution. The uranium may be recovered by contacting the uranium-holding resin with an aqueous ammonium carbonate solution whereby the uranium values are eluted from the resin and then heating the eluate whereby carbon dioxide and ammonia are given off, the pH value of the solution is lowered, and the uranium is precipitated.

  18. Lanthanide(III)/actinide(III) differentiation in coordination of azine molecules to tris(cyclopentadienyl) complexes of cerium and uranium.

    PubMed

    Mehdoui, Thouraya; Berthet, Jean-Claude; Thuéry, Pierre; Ephritikhine, Michel

    2004-02-21

    Reaction of azine molecules L with the trivalent metallocenes [M(C5H4R)3](M = Ce, U; R = But, SiMe3) in toluene gave the Lewis base adducts [M(C5H4R)3(L)](L = pyridine, 3-picoline, 3,5-lutidine, 3-chloropyridine, pyridazine, pyrimidine, pyrazine, 3,5-dimethylpyrazine and s-triazine), except in the cases of M = U and L = 3-chloropyridine, pyridazine, pyrazine and s-triazine where oxidation of U(III) was found to occur. In the pairs of analogous compounds of Ce(III) and U(III), i.e.[M(C5H4But)3(L)](L = pyridine, picoline) and [M(C5H4SiMe3)3(L)](L = pyridine, lutidine, pyrimidine and dimethylpyrazine), the M-N and average M-C distances are longer for M = Ce than for M = U; however, within a series of azine adducts of the same metallocene, no significant variation is noted in the M-N and average M-C distances. The equilibria between [M(C5H4R)3], L and [M(C5H4R)3(L)] were studied by 1H NMR spectroscopy. The stability constants of the uranium complexes, KUL, are greater than those of the cerium counterparts, KCeL. The values of KML are much greater for R = SiMe3 than for R = But and a linear correlation is found between the logarithms of KML and the hydrogen-bond basicity pKHB scale of the azines. Thermodynamic parameters indicate that the enthalpy-entropy compensation effect holds for these complexation reactions. Competition reactions of [Ce(C5H4R)3] and [U(C5H4R)3] with L show that the selectivity of L in favour of U(III) increases with the [small pi] donor character of the metallocene and is proportional to the pi accepting ability of the azine molecule, measured by its reduction potential.

  19. Uranium*

    NASA Astrophysics Data System (ADS)

    Grenthe, Ingmar; Drożdżyński, Janusz; Fujino, Takeo; Buck, Edgar C.; Albrecht-Schmitt, Thomas E.; Wolf, Stephen F.

    Uranium compounds have been used as colorants since Roman times (Caley, 1948). Uranium was discovered as a chemical element in a pitchblende specimen by Martin Heinrich Klaproth, who published the results of his work in 1789. Pitchblende is an impure uranium oxide, consisting partly of the most reduced oxide uraninite (UO2) and partly of U3O8. Earlier mineralogists had considered this mineral to be a complex oxide of iron and tungsten or of iron and zinc, but Klaproth showed by dissolving it partially in strong acid that the solutions yielded precipitates that were different from those of known elements. Therefore he concluded that it contained a new element (Mellor, 1932); he named it after the planet Uranus, which had been discovered in 1781 by William Herschel, who named it after the ancient Greek deity of the Heavens.

  20. Development of solid thorium-232 reference materials

    NASA Astrophysics Data System (ADS)

    Engelder, P. R.; Donivan, S.; Chessmore, R. B.

    1985-05-01

    Thorium-232 reference materials with a matrix similar to soil and uranium-mill tailings are necessary for ensuring uniform standardization among measurements performed by remedial-action contractors. Some 200 pounds each of three different concentrations of Th-232 reference material were prepared by diluting a thorium ore with soil. Target values for Th-232 content were 70, 30, and 10 pCi/q. The recommended thorium-232 concentrations for the three reference materials are 71.2 + or - 2.0 pCi/g, 30.5 + or - 0.6 pCi/g, and 10.2 + or - 0.3 pCi/g.

  1. 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.

  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. Uranium and thorium in achondrites.

    NASA Technical Reports Server (NTRS)

    Morgan, J. W.; Lovering, J. F.

    1973-01-01

    The abundances of U and Th in 19 achondrites and two pallasite olivines have been measured by radiochemical neutron activation analysis. Brecciated eucrites are enriched relative to chondrites in both elements by factors between 10 and 20, perhaps as a result of a magmatic differentiation process. Two unbrecciated eucrites are far less enriched, possibly due to their origin as igneous cumulates. The diogenites Johnstown and Shalka contain approximately chondritic levels of U and Th, but Ellemeet is 10 times lower. The abundances in three howardites are in good agreement with those expected from major element data for a mixing model with eucrite and diogenite end members. The high O-18 basaltic achondrites Nakhla, Shergotty and Angra dos Reis have a range of U and Th abundances similar to the brecciated eucrites and howardites, but have systematically higher Th/U ratios.

  4. Thorium-uranium fission radiography

    NASA Technical Reports Server (NTRS)

    Haines, E. L.; Weiss, J. R.; Burnett, D. S.; Woolum, D. S.

    1976-01-01

    Results are described for studies designed to develop routine methods for in-situ measurement of the abundance of Th and U on a microscale in heterogeneous samples, especially rocks, using the secondary high-energy neutron flux developed when the 650 MeV proton beam of an accelerator is stopped in a 42 x 42 cm diam Cu cylinder. Irradiations were performed at three different locations in a rabbit tube in the beam stop area, and thick metal foils of Bi, Th, and natural U as well as polished silicate glasses of known U and Th contents were used as targets and were placed in contact with mica which served as a fission track detector. In many cases both bare and Cd-covered detectors were exposed. The exposed mica samples were etched in 48% HF and the fission tracks counted by conventional transmitted light microscopy. Relative fission cross sections are examined, along with absolute Th track production rates, interaction tracks, and a comparison of measured and calculated fission rates. The practicality of fast neutron radiography revealed by experiments to data is discussed primarily for Th/U measurements, and mixtures of other fissionable nuclei are briefly considered.

  5. 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

  6. Safety and Regulatory Issues of the Thorium Fuel Cycle

    SciTech Connect

    Ade, Brian; Worrall, Andrew; Powers, Jeffrey; Bowman, Steve; Flanagan, George; Gehin, Jess

    2014-02-01

    Thorium has been widely considered an alternative to uranium fuel because of its relatively large natural abundance and its ability to breed fissile fuel (233U) from natural thorium (232Th). Possible scenarios for using thorium in the nuclear fuel cycle include use in different nuclear reactor types (light water, high temperature gas cooled, fast spectrum sodium, molten salt, etc.), advanced accelerator-driven systems, or even fission-fusion hybrid systems. The most likely near-term application of thorium in the United States is in currently operating light water reactors (LWRs). This use is primarily based on concepts that mix thorium with uranium (UO2 + ThO2), add fertile thorium (ThO2) fuel pins to LWR fuel assemblies, or use mixed plutonium and thorium (PuO2 + ThO2) fuel assemblies. The addition of thorium to currently operating LWRs would result in a number of different phenomenological impacts on the nuclear fuel. Thorium and its irradiation products have nuclear characteristics that are different from those of uranium. In addition, ThO2, alone or mixed with UO2 fuel, leads to different chemical and physical properties of the fuel. These aspects are key to reactor safety-related issues. The primary objectives of this report are to summarize historical, current, and proposed uses of thorium in nuclear reactors; provide some important properties of thorium fuel; perform qualitative and quantitative evaluations of both in-reactor and out-of-reactor safety issues and requirements specific to a thorium-based fuel cycle for current LWR reactor designs; and identify key knowledge gaps and technical issues that need to be addressed for the licensing of thorium LWR fuel in the United States.

  7. 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.

  8. The inverse-trans-influence in tetravalent lanthanide and actinide bis(carbene) complexes

    NASA Astrophysics Data System (ADS)

    Gregson, Matthew; Lu, Erli; Mills, David P.; Tuna, Floriana; McInnes, Eric J. L.; Hennig, Christoph; Scheinost, Andreas C.; McMaster, Jonathan; Lewis, William; Blake, Alexander J.; Kerridge, Andrew; Liddle, Stephen T.

    2017-02-01

    Across the periodic table the trans-influence operates, whereby tightly bonded ligands selectively lengthen mutually trans metal-ligand bonds. Conversely, in high oxidation state actinide complexes the inverse-trans-influence operates, where normally cis strongly donating ligands instead reside trans and actually reinforce each other. However, because the inverse-trans-influence is restricted to high-valent actinyls and a few uranium(V/VI) complexes, it has had limited scope in an area with few unifying rules. Here we report tetravalent cerium, uranium and thorium bis(carbene) complexes with trans C=M=C cores where experimental and theoretical data suggest the presence of an inverse-trans-influence. Studies of hypothetical praseodymium(IV) and terbium(IV) analogues suggest the inverse-trans-influence may extend to these ions but it also diminishes significantly as the 4f orbitals are populated. This work suggests that the inverse-trans-influence may occur beyond high oxidation state 5f metals and hence could encompass mid-range oxidation state actinides and lanthanides. Thus, the inverse-trans-influence might be a more general f-block principle.

  9. The inverse-trans-influence in tetravalent lanthanide and actinide bis(carbene) complexes

    PubMed Central

    Gregson, Matthew; Lu, Erli; Mills, David P.; Tuna, Floriana; McInnes, Eric J. L.; Hennig, Christoph; Scheinost, Andreas C.; McMaster, Jonathan; Lewis, William; Blake, Alexander J.; Kerridge, Andrew; Liddle, Stephen T.

    2017-01-01

    Across the periodic table the trans-influence operates, whereby tightly bonded ligands selectively lengthen mutually trans metal–ligand bonds. Conversely, in high oxidation state actinide complexes the inverse-trans-influence operates, where normally cis strongly donating ligands instead reside trans and actually reinforce each other. However, because the inverse-trans-influence is restricted to high-valent actinyls and a few uranium(V/VI) complexes, it has had limited scope in an area with few unifying rules. Here we report tetravalent cerium, uranium and thorium bis(carbene) complexes with trans C=M=C cores where experimental and theoretical data suggest the presence of an inverse-trans-influence. Studies of hypothetical praseodymium(IV) and terbium(IV) analogues suggest the inverse-trans-influence may extend to these ions but it also diminishes significantly as the 4f orbitals are populated. This work suggests that the inverse-trans-influence may occur beyond high oxidation state 5f metals and hence could encompass mid-range oxidation state actinides and lanthanides. Thus, the inverse-trans-influence might be a more general f-block principle. PMID:28155857

  10. URANIUM SEPARATION PROCESS

    DOEpatents

    Lyon, W.L.

    1962-04-17

    A method of separating uranium oxides from PuO/sub 2/, ThO/sub 2/, and other actinide oxides is described. The oxide mixture is suspended in a fused salt melt and a chlorinating agent such as chlorine gas or phosgene is sparged through the suspension. Uranium oxides are selectively chlorinated and dissolve in the melt, which may then be filtered to remove the unchlorinated oxides of the other actinides. (AEC)

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

    DOEpatents

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

    2004-12-14

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

  12. IUPAC-NIST Solubility Data Series. 84. Solubility of Inorganic Actinide Compounds

    NASA Astrophysics Data System (ADS)

    Hála, Jiri

    2007-12-01

    This volume presents the solubility of inorganic compounds of actinides except for carbonates, which are included in Volume 74 of this series, and nitrates, which are covered in Volume 55. Also included are solubility data of compounds such as organosulfates, phosphates, and arsenates, which are not covered in Volume 74. The predominant part of this volume covers solubility data of thorium, uranium, neptunium, and plutonium compounds. Fewer data have been published for americium compounds and very few for compounds of actinium, protactinium, and transamericium elements. The literature has been covered up to the end of 2004. Documents which remained unavailable to the editor, and could not be included in the volume are listed in the Appendix. For some compounds it was not possible to show the Chemical Abstracts registry numbers since these have not been assigned.

  13. Separation of uranium from (Th,U)O.sub.2 solid solutions

    DOEpatents

    Chiotti, Premo; Jha, Mahesh Chandra

    1976-09-28

    Uranium is separated from mixed oxides of thorium and uranium by a pyrometallurgical process in which the oxides are mixed with a molten chloride salt containing thorium tetrachloride and thorium metal which reduces the uranium oxide to uranium metal which can then be recovered from the molten salt. The process is particularly useful for the recovery of uranium from generally insoluble high-density sol-gel thoria-urania nuclear reactor fuel pellets.

  14. The Use of Thorium within the Nuclear Power Industry - 13472

    SciTech Connect

    Miller, Keith

    2013-07-01

    Thorium is 3 to 4 times more abundant than uranium and is widely distributed in nature as an easily exploitable resource in many countries. Unlike natural uranium, which contains ∼0.7% fissile {sup 235}U isotope, natural thorium does not contain any fissile material and is made up of the fertile {sup 232}Th isotope only. Therefore thorium and thorium-based fuel as metal, oxide or carbide, has been utilized in combination with fissile {sup 235}U or {sup 239}Pu in nuclear research and power reactors for conversion to fissile {sup 233}U, thereby enlarging fissile material resources. During the pioneering years of nuclear energy, from the mid 1950's to mid 1970's, there was considerable interest worldwide to develop thorium fuels and fuel cycles in order to supplement uranium reserves. Thorium fuels and fuel cycles are particularly relevant to countries having large thorium deposits but very limited uranium reserves for their long term nuclear power programme. The feasibility of thorium utilization in high temperature gas cooled reactors (HTGR), light water reactors (LWR), pressurized heavy water reactors (PHWRs), liquid metal cooled fast breeder reactors (LMFBR) and molten salt breeder reactors (MSBR) were demonstrated. The initial enthusiasm for thorium fuels and fuel cycles was not sustained among the developing countries later, due to new discovery of uranium deposits and their improved availability. However, in recent times, the need for proliferation-resistance, longer fuel cycles, higher burnup, and improved waste form characteristics, reduction of plutonium inventories and in situ use of bred-in fissile material has led to renewed interest in thorium-based fuels and fuel cycles. (authors)

  15. 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.

  16. 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.

  17. Accelerator-driven thorium-cycle fission power

    NASA Astrophysics Data System (ADS)

    Sattarov, Akhdiyor

    2009-10-01

    A flux-coupled stack of superconducting isochronous cyclotrons could be used to drive thorium-cycle fission power. The 800 MeV proton beams produce fast neutrons through spallation, then the fast neutrons transmute the thorium into uranium and drive fission. The thorium reactor would provide GW electric power, eat its own long-lived waste, run for 7 years between core accesses, operate below criticality, and be stable against melt-down. Reserves of thorium are sufficient to provide the world's energy needs for a thousand years.

  18. 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.

  19. Nuclear and materials aspects of the thorium fuel cycle

    NASA Astrophysics Data System (ADS)

    Rodriguez, P.; Sundaram, C. V.

    1981-09-01

    This paper is an attempt to assess and review the materials aspects of the thorium fuel cycle. It starts with an examination of the nuclear aspects of the thorium fuel cycle, meant as an introduction for materials scientists and engineers who may not normally be familiar with the concepts and terms involved. After defining and describing the thorium and uranium fuel cycles, the reasons for the resurgence of interest in the thorium fuel cycle and the technical and economic considerations that support its early adoption are examined. The reactor physics and fissile economics aspects of the thorium and uranium cycles are then compared. The specific reactor types suitable for the adoption of the thorium cycle are briefly examined and described. Subsequent sections of the paper are devoted to a detailed discussion of the materials aspects of the thorium fuel cycle. Available information on fabrication, refabrication and irradiation performance of thorium-based fuels for light water reactors, heavy water reactors, high temperature gas-cooled reactors, molten salt breeder reactors and fast breeder reactors is critically reviewed and analysed. Materials problems related to cladding and structural materials are also discussed whenever these are unique to the thorium cycle.

  20. Thorium: An energy source for the world of tomorrow

    NASA Astrophysics Data System (ADS)

    Revol, J.-P.

    2015-08-01

    To meet the tremendous world energy needs, systematic R&D has to be pursued to replace fossil fuels. Nuclear energy, which produces no green house gases and no air pollution, should be a leading candidate. How nuclear energy, based on thorium rather than uranium, could be an acceptable solution is discussed. Thorium can be used both to produce energy and to destroy nuclear waste. The thorium conference, organized by iThEC at CERN in October 2013, has shown that thorium is seriously considered by some major developing countries as a key element of their energy strategy. However, developed countries do not seem to move fast enough in that direction, while global cooperation is highly desirable in this domain. Thorium is not fissile. Various possible ways of using thorium will be reviewed. However, an elegant option is to drive an "Accelerator Driven System (ADS)" with a proton accelerator, as suggested by Nobel Prize laureate Carlo Rubbia .

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

    PubMed

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

    2016-04-01

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

  2. Involvement of 5f-orbitals in the bonding and reactivity of organoactinide compounds: thorium(IV) and uranium(IV) bis (hydrazonato) complexes

    SciTech Connect

    Cantat, Thibault; Graves, Christopher R; Morris, David E; Kiplinger, Jaqueline L

    2008-01-01

    Migratory insertion of diphenyldiazomethane into both metal-carbon bonds of the bis(alkyl) and bis(aryl) complexes (C5Me5)2AnR2 yields the first f-element bis(hydrazonato) complexes (C5Me5)2An[2-(N,N')-R-N-NCPh2]2 [An = Th, R = CH3 (18), PhCH2 (15), Ph (16); An = U, R = CH3 (17), PhCH2 (14)], which have been characterized by a combination of spectroscopy, electrochemistry, and X-ray crystallography. The two hydrazonato ligands adopt an 2-coordination mode leading to 20-electron (for Th) and 22-electron (for U) complexes that have no transition-metal analogues. In fact, reaction of (C5H5)2Zr(CH3)2 or (C5Me5)2Hf(CH3)2 with diphenyldiazomethane is limited to the formation of the corresponding mono(hydrazonato) complex (C5R5)2M[2-(N,N')-CH3-N-NCPh2](CH3) (M = Zr, R = H or M = Hf, R = CH3). The difference in the reactivities of the group 4 metal complexes and the actinides was used as a unique platform for investigating in depth the role of 5f orbitals on the reactivity and bonding in actinide organometallic complexes. The electronic structure of the (C5H5)2M[2-(N,N')-CH3-N-NCH2]2 (M = Zr, Th, U) model complexes was studied using density functional theory (DFT) calculations and compared to experimental structural, electrochemical, and spectroscopic results. Whereas transition-metal bis(cyclopentadienyl) complexes are known to stabilize three ligands in the metallocene girdle to form saturated (C5H5)2ML3 species, in a bis(hydrazonato) system, a fourth ligand is coordinated to the metal center to give (C5H5)2ML4. DFT calculations have shown that 5f orbitals in the actinide complexes play a crucial role in stabilizing this fourth ligand by stabilizing both the s and p electrons of the two 2-coordinated hydrazonato ligands. In contrast, the stabilization of the hydrazonato ligands was found to be significantly less effective for the putative bis(hydrazonato) zirconium(IV) complex, yielding a higher energy structure. However, the difference in the reactivities of the group 4

  3. Safeguards Considerations for Thorium Fuel Cycles

    DOE PAGES

    Worrall, Louise G.; Worrall, Andrew; Flanagan, George F.; ...

    2016-04-21

    We report that by around 2025, thorium-based fuel cycles are likely to be deployed internationally. States such as China and India are pursuing research, development, and deployment pathways toward a number of commercial-scale thorium fuel cycles, and they are already building test reactors and the associated fuel cycle infrastructure. In the future, the potential exists for these emerging programs to sell, export, and deploy thorium fuel cycle technology in other states. Without technically adequate international safeguards protocols and measures in place, any future potential clandestine misuse of these fuel cycles could go undetected, compromising the deterrent value of these protocolsmore » and measures. The development of safeguards approaches for thorium-based fuel cycles is therefore a matter of some urgency. Yet, the focus of the international safeguards community remains mainly on safeguarding conventional 235U- and 239Pu-based fuel cycles while the safeguards challenges of thorium-uranium fuel cycles remain largely uninvestigated. This raises the following question: Is the International Atomic Energy Agency and international safeguards system ready for thorium fuel cycles? Furthermore, is the safeguards technology of today sufficiently mature to meet the verification challenges posed by thorium-based fuel cycles? In defining these and other related research questions, the objectives of this paper are to identify key safeguards considerations for thorium-based fuel cycles and to call for an early dialogue between the international safeguards and the nuclear fuel cycle communities to prepare for the potential safeguards challenges associated with these fuel cycles. In this paper, it is concluded that directed research and development programs are required to meet the identified safeguards challenges and to take timely action in preparation for the international deployment of thorium fuel cycles.« less

  4. Safeguards Considerations for Thorium Fuel Cycles

    SciTech Connect

    Worrall, Louise G.; Worrall, Andrew; Flanagan, George F.; Croft, Steven

    2016-04-21

    We report that by around 2025, thorium-based fuel cycles are likely to be deployed internationally. States such as China and India are pursuing research, development, and deployment pathways toward a number of commercial-scale thorium fuel cycles, and they are already building test reactors and the associated fuel cycle infrastructure. In the future, the potential exists for these emerging programs to sell, export, and deploy thorium fuel cycle technology in other states. Without technically adequate international safeguards protocols and measures in place, any future potential clandestine misuse of these fuel cycles could go undetected, compromising the deterrent value of these protocols and measures. The development of safeguards approaches for thorium-based fuel cycles is therefore a matter of some urgency. Yet, the focus of the international safeguards community remains mainly on safeguarding conventional 235U- and 239Pu-based fuel cycles while the safeguards challenges of thorium-uranium fuel cycles remain largely uninvestigated. This raises the following question: Is the International Atomic Energy Agency and international safeguards system ready for thorium fuel cycles? Furthermore, is the safeguards technology of today sufficiently mature to meet the verification challenges posed by thorium-based fuel cycles? In defining these and other related research questions, the objectives of this paper are to identify key safeguards considerations for thorium-based fuel cycles and to call for an early dialogue between the international safeguards and the nuclear fuel cycle communities to prepare for the potential safeguards challenges associated with these fuel cycles. In this paper, it is concluded that directed research and development programs are required to meet the identified safeguards challenges and to take timely action in preparation for the international deployment of thorium fuel cycles.

  5. 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.

  6. 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.

  7. 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.

  8. Catalysis vs. oxophilicity: Breaking the myth of inactive actinide-oxo complexes

    NASA Astrophysics Data System (ADS)

    Andrea, Tamer; Barnea, Eyal; Wang, Jiaxi; Eisen, Moris S.

    2010-03-01

    For many decades, compounds containing oxygen atoms were excluded from the actinide-catalysis field because of the high oxophilic nature of these complexes. Pursuing the conceptual question about the potential activity of actinide-oxo bonds we were surprised to find that the coupling of aromatic aldehydes catalyzed by Cp*2ThMe2 and Th(NEtMe)4 via thorium-alkoxide intermediates take place in high yields to produce the corresponding esters. Here we present our breakthrough results including comprehensive mechanistic, deuterium labeling, kinetic and thermodynamic studies. In addition, the tetrachloride salt of uranium reacts with one equivalent of Li2[(C5Me4)2SiMe2] in DME to form the complex {[η5-(C5Me4)2SiMe2]UCl2·2LiCl·2DME (13), which reacts with equimolar amounts of water in DME yielding the coordinative unsaturated bridged mono oxide and mono chloride uranium lithium salt complex {[η5-(C5Me4)2SiMe2]UCl}2((μ-O)((μ-Cl)•Li(DME)3•DME (14). The alkylation of complexes 14 with BuLi gives the mono bridged dibutyl complex {[η5-(C5Me4)2SiMe2]UBu}2(μ-O) (16). Complex 16 is an active catalyst for the disproportionation metathesis of TMSC≡CH and the cross-metathesis of TMSC≡CH or TMSC≡CTMS with various terminal alkynes. PhSiH3 reacts with complex 16 producing Ph2SiH2 and SiH4 (caution) indicating the cleavage of the trimethylsilyl group from the phenyl moiety and the formation of uranium-silyl intermediate.

  9. Distribution of uranium, thorium and some stable trace and toxic elements in human hair and nails in Niška Banja Town, a high natural background radiation area of Serbia (Balkan Region, South-East Europe).

    PubMed

    Sahoo, S K; Žunić, Z S; Kritsananuwat, R; Zagrodzki, P; Bossew, P; Veselinovic, N; Mishra, S; Yonehara, H; Tokonami, S

    2015-07-01

    Human hair and nails can be considered as bio-indicators of the public exposure to certain natural radionuclides and other toxic metals over a long period of months or even years. The level of elements in hair and nails usually reflect their levels in other tissues of body. Niška Banja, a spa town located in southern Serbia, with locally high natural background radiation was selected for the study. To assess public exposure to the trace elements, hair and nail samples were collected and analyzed. The concentrations of uranium, thorium and some trace and toxic elements (Mn, Ni, Cu, Sr, Cd, and Cs) were determined using inductively coupled plasma mass spectrometry (ICP-MS). U and Th concentrations in hair varied from 0.0002 to 0.0771 μg/g and from 0.0002 to 0.0276 μg/g, respectively. The concentrations in nails varied from 0.0025 to 0.0447 μg/g and from 0.0023 to 0.0564 μg/g for U and Th, respectively. We found significant correlations between some elements in hair and nails. Also indications of spatial clustering of high values could be found. However, this phenomenon as well as the large variations in concentrations of heavy metals in hair and nail could not be explained. As hypotheses, we propose possible exposure pathways which may explain the findings, but the current data does not allow testing them.

  10. Utilization of non-weapons-grade plutonium and highly enriched uranium with breeding of the {sup 233}U isotope in the VVER reactors using thorium and heavy water

    SciTech Connect

    Marshalkin, V. E. Povyshev, V. M.

    2015-12-15

    A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium–uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D{sub 2}O, H{sub 2}O) is proposed. The method is characterized by efficient breeding of the {sup 233}U isotope and safe reactor operation and is comparatively simple to implement.

  11. Thorium, uranium and rare earth elements content in lanthanide concentrate (LC) and water leach purification (WLP) residue of Lynas advanced materials plant (LAMP)

    SciTech Connect

    AL-Areqi, Wadeeah M. Majid, Amran Ab. Sarmani, Sukiman

    2014-02-12

    Lynas Advanced Materials Plant (LAMP) has been licensed to produce the rare earths elements since early 2013 in Malaysia. LAMP processes lanthanide concentrate (LC) to extract rare earth elements and subsequently produce large volumes of water leach purification (WLP) residue containing naturally occurring radioactive material (NORM). This residue has been rising up the environmental issue because it was suspected to accumulate thorium with significant activity concentration and has been classified as radioactive residue. The aim of this study is to determine Th-232, U-238 and rare earth elements in lanthanide concentrate (LC) and water leach purification (WLP) residue collected from LAMP and to evaluate the potential radiological impacts of the WLP residue on the environment. Instrumental Neutron Activation Analysis and γ-spectrometry were used for determination of Th, U and rare earth elements concentrations. The results of this study found that the concentration of Th in LC was 1289.7 ± 129 ppm (5274.9 ± 527.6Bq/kg) whereas the Th and U concentrations in WLP were determined to be 1952.9±17.6 ppm (7987.4 ± 71.9 Bq/kg) and 17.2 ± 2.4 ppm respectively. The concentrations of Th and U in LC and WLP samples determined by γ- spectrometry were 1156 ppm (4728 ± 22 Bq/kg) and 18.8 ppm and 1763.2 ppm (7211.4 Bq/kg) and 29.97 ppm respectively. This study showed that thorium concentrations were higher in WLP compare to LC. This study also indicate that WLP residue has high radioactivity of {sup 232}Th compared to Malaysian soil natural background (63 - 110 Bq/kg) and come under preview of Act 304 and regulations. In LC, the Ce and Nd concentrations determined by INAA were 13.2 ± 0.6% and 4.7 ± 0.1% respectively whereas the concentrations of La, Ce, Nd and Sm in WLP were 0.36 ± 0.04%, 1.6%, 0.22% and 0.06% respectively. This result showed that some amount of rare earth had not been extracted and remained in the WLP and may be considered to be reextracted.

  12. Thorium, uranium and rare earth elements content in lanthanide concentrate (LC) and water leach purification (WLP) residue of Lynas advanced materials plant (LAMP)

    NASA Astrophysics Data System (ADS)

    AL-Areqi, Wadeeah M.; Majid, Amran Ab.; Sarmani, Sukiman

    2014-02-01

    Lynas Advanced Materials Plant (LAMP) has been licensed to produce the rare earths elements since early 2013 in Malaysia. LAMP processes lanthanide concentrate (LC) to extract rare earth elements and subsequently produce large volumes of water leach purification (WLP) residue containing naturally occurring radioactive material (NORM). This residue has been rising up the environmental issue because it was suspected to accumulate thorium with significant activity concentration and has been classified as radioactive residue. The aim of this study is to determine Th-232, U-238 and rare earth elements in lanthanide concentrate (LC) and water leach purification (WLP) residue collected from LAMP and to evaluate the potential radiological impacts of the WLP residue on the environment. Instrumental Neutron Activation Analysis and γ-spectrometry were used for determination of Th, U and rare earth elements concentrations. The results of this study found that the concentration of Th in LC was 1289.7 ± 129 ppm (5274.9 ± 527.6Bq/kg) whereas the Th and U concentrations in WLP were determined to be 1952.9±17.6 ppm (7987.4 ± 71.9 Bq/kg) and 17.2 ± 2.4 ppm respectively. The concentrations of Th and U in LC and WLP samples determined by γ- spectrometry were 1156 ppm (4728 ± 22 Bq/kg) & 18.8 ppm and 1763.2 ppm (7211.4 Bq/kg) &29.97 ppm respectively. This study showed that thorium concentrations were higher in WLP compare to LC. This study also indicate that WLP residue has high radioactivity of 232Th compared to Malaysian soil natural background (63 - 110 Bq/kg) and come under preview of Act 304 and regulations. In LC, the Ce and Nd concentrations determined by INAA were 13.2 ± 0.6% and 4.7 ± 0.1% respectively whereas the concentrations of La, Ce, Nd and Sm in WLP were 0.36 ± 0.04%, 1.6%, 0.22% and 0.06% respectively. This result showed that some amount of rare earth had not been extracted and remained in the WLP and may be considered to be reextracted.

  13. Radionuclide Basics: Thorium

    EPA Pesticide Factsheets

    Thorium is a naturally occurring radioactive metal found at trace levels in soil, rocks, plants and animals. Thorium is used very little in industry, but can be found in heat-resistant alloys and paints and optical lenses.

  14. Transuranic Waste Burning Potential of Thorium Fuel in a Fast Reactor - 12423

    SciTech Connect

    Wenner, Michael; Franceschini, Fausto; Ferroni, Paolo; Sartori, Alberto; Ricotti, Marco

    2012-07-01

    Westinghouse Electric Company (referred to as 'Westinghouse' in the rest of this paper) is proposing a 'back-to-front' approach to overcome the stalemate on nuclear waste management in the US. In this approach, requirements to further the societal acceptance of nuclear waste are such that the ultimate health hazard resulting from the waste package is 'as low as reasonably achievable'. Societal acceptability of nuclear waste can be enhanced by reducing the long-term radiotoxicity of the waste, which is currently driven primarily by the protracted radiotoxicity of the transuranic (TRU) isotopes. Therefore, a transition to a more benign radioactive waste can be accomplished by a fuel cycle capable of consuming the stockpile of TRU 'legacy' waste contained in the LWR Used Nuclear Fuel (UNF) while generating waste which is significantly less radio-toxic than that produced by the current open U-based fuel cycle (once through and variations thereof). Investigation of a fast reactor (FR) operating on a thorium-based fuel cycle, as opposed to the traditional uranium-based is performed. Due to a combination between its neutronic properties and its low position in the actinide chain, thorium not only burns the legacy TRU waste, but it does so with a minimal production of 'new' TRUs. The effectiveness of a thorium-based fast reactor to burn legacy TRU and its flexibility to incorporate various fuels and recycle schemes according to the evolving needs of the transmutation scenario have been investigated. Specifically, the potential for a high TRU burning rate, high U-233 generation rate if so desired and low concurrent production of TRU have been used as metrics for the examined cycles. Core physics simulations of a fast reactor core running on thorium-based fuels and burning an external TRU feed supply have been carried out over multiple cycles of irradiation, separation and reprocessing. The TRU burning capability as well as the core isotopic content have been characterized

  15. 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.

  16. PRODUCTION OF THORIUM FLUORIDE

    DOEpatents

    Zachariasen, W.H.

    1959-08-11

    A process is presented for producing anhydrous thorium fluoride comprising the step of contacting a saturated aqueous solution of thorium nitrate with an aqueous solution of hydrofluoric acid having a concentration of about 45 to 50% by weight at a temperature above 70 deg C whereby anhydrous thorium fluoride precipitates.

  17. Uranium-238 and thorium-232 series concentrations in soil, radon-222 indoor and drinking water concentrations and dose assessment in the city of Aldama, Chihuahua, Mexico.

    PubMed

    Colmenero Sujo, L; Montero Cabrera, M E; Villalba, L; Rentería Villalobos, M; Torres Moye, E; García León, M; García-Tenorio, R; Mireles García, F; Herrera Peraza, E F; Sánchez Aroche, D

    2004-01-01

    High-resolution gamma spectrometry was used to determine the concentration of 40K, 238U and 232Th series in soil samples taken from areas surrounding the city of Aldama, in Chihuahua. Results of indoor air short-time sampling, with diffusion barrier charcoal detectors, revealed relatively high indoor radon levels, ranging from 29 to 422 Bq/m3; the radon concentrations detected exceeded 148 Bq/m3 in 76% of the homes tested. Additionally, liquid scintillation counting showed concentrations of radon in drinking water ranging from 4.3 to 42 kBq/m3. The high activity of 238U in soil found in some places may be a result of the uranium milling process performed 20 years ago in the area. High radon concentrations indoor and in water may be explained by assuming the presence of uranium-bearing rocks underneath of the city, similar to a felsic dike located near Aldama. The estimated annual effective dose of gamma radiation from the soil and radon inhalation was 3.83 mSv.

  18. 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

  19. Thorium and uranium redox-active ligand complexes; reversible intramolecular electron transfer in U(dpp-BIAN)2/ U(dpp-BIAN)2(THE)

    SciTech Connect

    Schelter, Eric John; Wu, Ruilian; Scott, Brian L; Thompson, Joe D; Batista, Enrique R; Morris, David E; Kiplinger, Jaqueline L

    2008-01-01

    Actinide complexes of the redox-active ligand dpp-BIAN{sup 2-} (dpp-BIAN = bis(2,6-diisopropylphenyl)acenaphthylene), An(dpp-BIAN){sub 2}(THF){sub n} (An = Th, n = 1; An = U, n = 0, 1) have been prepared. Solid-state magnetic and single-crystal X-ray data for U(dpp-BIAN){sub 2}(THF){sub n} show when n = 0, the complex exists in an f{sup 2}-{pi}*{sup 4} configuration; whereas an intramolecular electron transfer occurs for n = 1, resulting in an f{sup 3}-{pi}*{sup 3} ground configuration. The magnetic data also indicate that interconversion between the two forms of the complex is possible, limited only by the ability of THF vapor to penetrate the solid on cooling of the sample. Spectroscopic data indicate the complex exists solely in the f{sup 2}-{pi}*{sup 4} form in solution, evidenced by the appearance of only small changes in the electronic absorption spectra of the U(dpp-BIAN){sub 2} complex on titration with THF and by measurement of the solution magnetic moment m d{sub 8}-tetrahydrofuran using Evans method. Electrochemistry of the complexes is reported, with small differences observed in wave potentials between metals and in the presence of THF. These data represent the first example of a well-defined, reversible intramolecular electron transfer in an f-element complex and the second example of oxidation state change through dative interaction with a metal ion.

  20. Raman Spectroscopy for Analysis of Thorium Compounds

    SciTech Connect

    Su, Yin-Fong; Johnson, Timothy J.; Olsen, Khris B.

    2016-05-12

    The thorium fuel cycle is an alternative to the uranium fuel cycle in that when 232Th is irradiated with neutrons it is converted to 233U, another fissile isotope. There are several chemical forms of thorium which are used in the Th fuel cycle. Recently, Raman spectroscopy has become a very portable and facile analytical technique useful for many applications, including e.g. determining the chemical composition of different materials such as for thorium compounds. The technique continues to improve with the development of ever-more sensitive instrumentation and better software. Using a laboratory Fourier-transform (FT)-Raman spectrometer with a 785 nm wavelength laser, we were able to obtain Raman spectra from a series of thorium-bearing compounds of unknown origin. These spectra were compared to the spectra of in-stock-laboratory thorium compounds including ThO2, ThF4, Th(CO3)2 and Th(C2O4)2. The unknown spectra showed very good agreement to the known standards, demonstrating the applicability of Raman spectroscopy for detection and identification of these nuclear materials.

  1. Thorium dioxide: properties and nuclear applications

    SciTech Connect

    Belle, J.; Berman, R.M.

    1984-01-01

    This is the sixth book on reactor materials published under sponsorship of the Naval Reactors Office of the United States Department of Energy, formerly the United States Atomic Energy Commission. This book presents a comprehensive compilation of the most significant properties of thorium dioxide, much like the book Uranium Dioxide: Properties and Nuclear Applications presented information on the fuel material used in the Shippingport Pressurized Water Reactor core.

  2. Structure and thermodynamics of uranium-containing iron garnets

    DOE PAGES

    Guo, Xiaofeng; Navrotsky, Alexandra; Kukkadapu, Ravi K.; ...

    2016-09-15

    Use of crystalline garnet as a waste form phase appears to be advantageous for accommodating actinides from nuclear waste. Previous studies show that large amounts of uranium (U) and its analogues such as cerium (Ce) and thorium (Th) can be incorporated into the garnet structure. In this study, we synthesized U loaded garnet phases, Ca3UxZr2–xFe3O12 (x = 0.5–0.7), along with the endmember phase, Ca3(Zr2)SiFe3+2O12, for comparison. The oxidation states of U were determined by X-ray photoelectron and absorption spectroscopies, revealing the presence of mixed pentavalent and hexavalent uranium in the phases with x = 0.6 and 0.7. The oxidation statesmore » and coordination environments of Fe were measured using transmission 57Fe-Mössbauer spectroscopy, which shows that all iron is tetrahedrally coordinated Fe3+. U substitution had a significant effect on local environments, the extent of U substitution within this range had a minimal effect on the structure, and unlike in the x = 0 sample, Fe exists in two different environments in the substituted garnets. The enthalpies of formation of garnet phases from constituent oxides and elements were first time determined by high temperature oxide melt solution calorimetry. The results indicate that these substituted garnets are thermodynamically stable under reducing conditions. Furthermore, our structural and thermodynamic analysis further provides explanation for the formation of natural uranium garnet, elbrusite-(Zr), and supports the potential use of Ca3UxZr2–xFe3O12 as viable waste form phases for U and other actinides.« less

  3. Structure and thermodynamics of uranium-containing iron garnets

    SciTech Connect

    Guo, Xiaofeng; Navrotsky, Alexandra; Kukkadapu, Ravi K.; Engelhard, Mark H.; Lanzirotti, Antonio; Newville, Matthew; Ilton, Eugene S.; Sutton, Stephen R.; Xu, Hongwu

    2016-09-01

    Use of crystalline garnet as a waste form phase appears to be advantageous for accommodating actinides from nuclear waste. Previous studies show that large amounts of uranium (U) and its analogues such as cerium (Ce) and thorium (Th) can be incorporated into the garnet structure. In this study, we synthesized U loaded garnet phases, Ca3UxZr2-xFe3O12 (x = 0.5 - 0.7), along with the endmember phase, Ca3(Zr2)SiFe3+2O12, for comparison. The oxidation states of U were determined by X-ray photoelectron and absorption spectroscopies, revealing the presence of mixed pentavalent and hexavalent uranium in the phases with x = 0.6 and 0.7. The oxidation states and coordination environments of Fe were measured using transmission 57Fe-Mössbauer spectroscopy, which shows that all iron is tetrahedrally coordinated Fe3+ (x = 0 and substituted sample), U substitution had a significant effect on local environments, the extent of U isubstitution within this range had a minimal effect on the structure, and unlike in the x = 0 sample, Fe exists in two different environments in the substituted garnets. The enthalpies of formation of garnet phases from constituent oxides and elements were determined by high temperature oxide melt solution calorimetry. The results indicate that these substituted garnets are thermodynamically stable under reducing conditions. Our structural and thermodynamic analysis further provides explanation for the formation of natural uranium garnet, elbrusite-(Zr), and supports the potential use of Ca3UxZr2-xFe3O12 as viable waste form phases for U and other actinides.

  4. Structure and thermodynamics of uranium-containing iron garnets

    SciTech Connect

    Guo, Xiaofeng; Navrotsky, Alexandra; Kukkadapu, Ravi K.; Engelhard, Mark H.; Lanzirotti, Antonio; Newville, Matthew; Ilton, Eugene S.; Sutton, Stephen R.; Xu, Hongwu

    2016-09-15

    Use of crystalline garnet as a waste form phase appears to be advantageous for accommodating actinides from nuclear waste. Previous studies show that large amounts of uranium (U) and its analogues such as cerium (Ce) and thorium (Th) can be incorporated into the garnet structure. In this study, we synthesized U loaded garnet phases, Ca3UxZr2–xFe3O12 (x = 0.5–0.7), along with the endmember phase, Ca3(Zr2)SiFe3+2O12, for comparison. The oxidation states of U were determined by X-ray photoelectron and absorption spectroscopies, revealing the presence of mixed pentavalent and hexavalent uranium in the phases with x = 0.6 and 0.7. The oxidation states and coordination environments of Fe were measured using transmission 57Fe-Mössbauer spectroscopy, which shows that all iron is tetrahedrally coordinated Fe3+. U substitution had a significant effect on local environments, the extent of U substitution within this range had a minimal effect on the structure, and unlike in the x = 0 sample, Fe exists in two different environments in the substituted garnets. The enthalpies of formation of garnet phases from constituent oxides and elements were first time determined by high temperature oxide melt solution calorimetry. The results indicate that these substituted garnets are thermodynamically stable under reducing conditions. Furthermore, our structural and thermodynamic analysis further provides explanation for the formation of natural uranium garnet, elbrusite-(Zr), and supports the potential use of Ca3UxZr2–xFe3O12 as viable waste form phases for U and other actinides.

  5. Structure and thermodynamics of uranium-containing iron garnets

    NASA Astrophysics Data System (ADS)

    Guo, Xiaofeng; Navrotsky, Alexandra; Kukkadapu, Ravi K.; Engelhard, Mark H.; Lanzirotti, Antonio; Newville, Matthew; Ilton, Eugene S.; Sutton, Stephen R.; Xu, Hongwu

    2016-09-01

    Use of crystalline garnet as a waste form phase appears to be advantageous for accommodating actinides from nuclear waste. Previous studies show that large amounts of uranium (U) and its analogues such as cerium (Ce) and thorium (Th) can be incorporated into the garnet structure. In this study, we synthesized U loaded garnet phases, Ca3UxZr2-xFe3O12 (x = 0.5-0.7), along with the endmember phase, Ca3(Zr2)SiFe3+2O12, for comparison. The oxidation states of U were determined by X-ray photoelectron and absorption spectroscopies, revealing the presence of mixed pentavalent and hexavalent uranium in the phases with x = 0.6 and 0.7. The oxidation states and coordination environments of Fe were measured using transmission 57Fe-Mössbauer spectroscopy, which shows that all iron is tetrahedrally coordinated Fe3+. U substitution had a significant effect on local environments, the extent of U substitution within this range had a minimal effect on the structure, and unlike in the x = 0 sample, Fe exists in two different environments in the substituted garnets. The enthalpies of formation of garnet phases from constituent oxides and elements were first time determined by high temperature oxide melt solution calorimetry. The results indicate that these substituted garnets are thermodynamically stable under reducing conditions. Our structural and thermodynamic analysis further provides explanation for the formation of natural uranium garnet, elbrusite-(Zr), and supports the potential use of Ca3UxZr2-xFe3O12 as viable waste form phases for U and other actinides.

  6. LWR First Recycle of TRU with Thorium Oxide for Transmutation and Cross Sections

    SciTech Connect

    Andrea Alfonsi; Gilles Youinou

    2012-07-01

    Thorium has been considered as an option to uranium-based fuel, based on considerations of resource utilization (thorium is approximately three times more plentiful than uranium) and as a result of concerns about proliferation and waste management (e.g. reduced production of plutonium, etc.). Since the average composition of natural Thorium is dominated (100%) by the fertile isotope Th-232, Thorium is only useful as a resource for breeding new fissile materials, in this case U-233. Consequently a certain amount of fissile material must be present at the start-up of the reactor in order to guarantee its operation. The thorium fuel can be used in both once-through and recycle options, and in both fast and thermal spectrum systems. The present study has been aimed by the necessity of investigating the option of using reprocessed plutonium/TRU, from a once-through reference LEU scenario (50 GWd/ tIHM), mixed with natural thorium and the need of collect data (mass fractions, cross-sections etc.) for this particular fuel cycle scenario. As previously pointed out, the fissile plutonium is needed to guarantee the operation of the reactor. Four different scenarios have been considered: • Thorium – recycled Plutonium; • Thorium – recycled Plutonium/Neptunium; • Thorium – recycled Plutonium/Neptunium/Americium; • Thorium – recycled Transuranic. The calculations have been performed with SCALE6.1-TRITON.

  7. LWR First Recycle of TRU with Thorium Oxide for Transmutation and Cross Sections

    SciTech Connect

    Andrea Alfonsi; Gilles Youinou; Sonat Sen

    2013-02-01

    Thorium has been considered as an option to uranium-based fuel, based on considerations of resource utilization (thorium is approximately three times more plentiful than uranium) and as a result of concerns about proliferation and waste management (e.g. reduced production of plutonium, etc.). Since the average composition of natural Thorium is dominated (100%) by the fertile isotope Th-232, Thorium is only useful as a resource for breeding new fissile materials, in this case U-233. Consequently a certain amount of fissile material must be present at the start-up of the reactor in order to guarantee its operation. The thorium fuel can be used in both once-through and recycle options, and in both fast and thermal spectrum systems. The present study has been aimed by the necessity of investigating the option of using reprocessed plutonium/TRU, from a once-through reference LEU scenario (50 GWd/ tIHM), mixed with natural thorium and the need of collect data (mass fractions, cross-sections etc.) for this particular fuel cycle scenario. As previously pointed out, the fissile plutonium is needed to guarantee the operation of the reactor. Four different scenarios have been considered: • Thorium – recycled Plutonium; • Thorium – recycled Plutonium/Neptunium; • Thorium – recycled Plutonium/Neptunium/Americium; • Thorium – recycled Transuranic. The calculations have been performed with SCALE6.1-TRITON.

  8. RECOVERY OF URANIUM BY SECONDARY XANTHATE COMPLEXING

    DOEpatents

    Neville, O.K.

    1959-09-01

    A method is described for separating and recovering uranium values contained in an acidic aqueous solution together with thorium or protactinium values. In accordance with the invention, the acidic solution containing uranium in the uranyl form is contacted with an organic xanthate. The xanthate forms a urano-xanthate complex but is substantially non-reactive with thorium and protactinium. The urano-xanthate complex is recovered by organic solvent extraction.

  9. Non-Proliferative, Thorium-Based, Core and Fuel Cycle for Pressurized Water Reactors

    SciTech Connect

    Todosow M.; Todosow M.; Raitses, G. Galperin, A.

    2009-07-12

    Two of the major barriers to the expansion of worldwide adoption of nuclear power are related to proliferation potential of the nuclear fuel cycle and issues associated with the final disposal of spent fuel. The Radkowsky Thorium Fuel (RTF) concept proposed by Professor A. Radkowsky offers a partial solution to these problems. The main idea of the concept is the utilization of the seed-blanket unit (SBU) fuel assembly geometry which is a direct replacement for a 'conventional' assembly in either a Russian pressurized water reactor (VVER-1000) or a Western pressurized water reactor (PWR). The seed-blanket fuel assembly consists of a fissile (U) zone, known as seed, and a fertile (Th) zone known as blanket. The separation of fissile and fertile allows separate fuel management schemes for the thorium part of the fuel (a subcritical 'blanket') and the 'driving' part of the core (a supercritical 'seed'). The design objective for the blanket is an efficient generation and in-situ fissioning of the U233 isotope, while the design objective for the seed is to supply neutrons to the blanket in a most economic way, i.e. with minimal investment of natural uranium. The introduction of thorium as a fertile component in the nuclear fuel cycle significantly reduces the quantity of plutonium production and modifies its isotopic composition, reducing the overall proliferation potential of the fuel cycle. Thorium based spent fuel also contains fewer higher actinides, hence reducing the long-term radioactivity of the spent fuel. The analyses show that the RTF core can satisfy the requirements of fuel cycle length, and the safety margins of conventional pressurized water reactors. The coefficients of reactivity are comparable to currently operating VVER's/PWR's. The major feature of the RTF cycle is related to the total amount of spent fuel discharged for each cycle from the reactor core. The fuel management scheme adopted for RTF core designs allows a significant decrease in the

  10. THORIUM DISPERSION IN BISMUTH

    DOEpatents

    Bryner, J.S.

    1961-07-01

    The growth of thorium bismutaide particles, which are formed when thorium is suspended in liquid bismuth, is inhibited when the liquid metal suspension is being flowed through a reactor and through a heat exchanger in sequence. It involves the addition of as little as 1 part by weight of tellurium to 100 parts of thorium. This addition is sufficient to inhibit particle growth and agglomeration.

  11. URANIUM BISMUTHIDE DISPERSION IN MOLTEN METAL

    DOEpatents

    Teitel, R.J.

    1959-10-27

    The formation of intermetallic bismuth compounds of thorium or uranium dispersed in a liquid media containing bismuth and lead is described. A bismuthide of uranium dispersed in a liquid metal medium is formed by dissolving uranium in composition of lead and bismuth containing less than 80% lead and lowering the temperature of the composition to a temperature below the point at which the solubility of uranium is exceeded and above the melting point of the composition.

  12. Thorium Diffusion in Monazite

    NASA Astrophysics Data System (ADS)

    Cherniak, D. J.

    2006-05-01

    Diffusion of thorium has been characterized in synthetic monazite under dry conditions. The synthetic monazites (either pure CePO4, NdPO4, or a mixed LREE phosphate containing Ce, Nd, and Sm) were grown via a Na2CO3-MoO3 flux method. The source of diffusant for the experiments were either synthesized ThSiO4 or CaTh(PO4)2 powders. Experiments were performed by placing source and monazite in Pt capsules and annealing capsules in 1 atm furnaces for times ranging from 10 days to a few hours, at temperatures from 1400 to 1550C. The Th distributions in the monazite were profiled by Rutherford Backscattering Spectrometry (RBS). The following Arrhenius relation was obtained for diffusion in monazite: DSm = 7.2x103 exp(-814 kJ mol-1/RT) m2sec-1 The diffusivity of Th was similar for monazites containing a single REE and the mixed LREE phosphates. Th diffusion was also similar for experiments run using the Th silicate and Ca-Th phosphate sources, suggesting that the substitutional mechanism for Th in monazite, i.e, Th+4 + Si+4 for REE+3 + P+5 with the ThSiO4 source, and Th+4 + Ca+2 for 2REE+3 with the CaTh(PO4)2 source, does not significantly affect Th diffusivities, and that Th is likely the rate-limiting species. Th diffusion in monazite is about 4 orders of magnitude slower than Pb diffusion (Cherniak et al., 2004). This contrasts with findings of Gardes et al. (2005) who determined that Pb, Th and REE diffusivities in monazite are similar. Th diffusion in zircon (Cherniak et al., 1997) is about an order of magnitude slower than in monazite, but with similar activation energy for diffusion. The smaller diffusivities in zircon may be a consequence of the larger disparity in size between Th and the Zr site in zircon as compared with Th and the REE site in monazite. Nonetheless, Th is essentially immobile in monazite with respect to exchange by volume diffusion under most geologic conditions; these findings may have implications for containment of high- level actinide

  13. 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.

  14. 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.

  15. 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.

  16. Geochemical investigations by the U.S. Geological Survey on uranium mining, milling, and environmental restoration

    USGS Publications Warehouse

    Landa, Edward R.; Cravotta, Charles A.; Naftz, David L.; Verplanck, Philip L.; Nordstrom, D. Kirk; Zielinski, Robert A.

    2000-01-01

    Recent research by the U.S. Geological Survey has characterized contaminant sources and identified important geochemical processes that influence transport of radionuclides from uranium mining and milling wastes. 1) Selective extraction studies indicated that alkaline earth sulfates and hydrous ferric oxides are important hosts of 226Ra in uranium mill tailings. The action of sulfate-reducing and ironreducing bacteria on these phases was shown to enhance release of radium, and this adverse result may temper decisions to dispose of uranium mill tailings in anaerobic environments. 2) Field studies have shown that although surface-applied sewage sludge/wood chip amendments aid in revegetating pyritic spoil, the nitrogen in sludge leachate can enhance pyrite oxidation, acidification of groundwater, and the consequent mobilization of metals and radionuclides. 3) In a U.S. Environmental Protection Agencyfunded study, three permeable reactive barriers consisting of phosphate-rich material, zero-valent iron, or amorphous ferric oxyhydroxide have been installed at an abandoned uranium upgrader facility near Fry Canyon, UT. Preliminary results indicate that each of the permeable reactive barriers is removing the majority of the uranium from the groundwater. 4) Studies on the geochemistry of rare earth elements as analogues for actinides such as uranium and thorium in acid mine drainage environments indicate high mobility under acid-weathering conditions but measurable attenuation associated with iron and aluminum colloid formation. Mass balances from field and laboratory studies are being used to quantify the amount of attenuation. 5) A field study in Colorado demonstrated the use of 234U/238U isotopic ratio measurements to evaluate contamination of shallow groundwater with uranium mill effluent.

  17. CATALYTIC RECOMBINATION OF RADIOLYTIC GASES IN THORIUM OXIDE SLURRIES

    DOEpatents

    Morse, L.E.

    1962-08-01

    A method for the coinbination of hydrogen and oxygen in aqueous thorium oxide-uranium oxide slurries is described. A small amount of molybdenum oxide catalyst is provided in the slurry. This catalyst is applicable to the recombination of hydrogen and/or deuterium and oxygen produced by irradiation of the slurries in nuclear reactors. (AEC)

  18. METHOD OF RECOVERING THORIUM

    DOEpatents

    Fisher, R.W.

    1957-12-10

    A method is described for recovering thorium from impurities found in a slag containing thorium and said impurities, comprising leaching a composition containing thorium with water, removing the water solution, treating the residue with hydrochloric acid, separating the solution from the insoluble residue, adjusting its acidity to 1 to 3 normal, adding oxalic acid, and thereafter separating the precipitated thorium oxalate digesting the residue from the hydrochloric acid treatment with a strong solution of sodium hydroxide at an elevated temperature, removing said solution and treating the insoluble residue with hydrochloric acid, separating the solution from the insoluble residue, adjusting the acidity of this solution to 1 to 3 normal, adding nitric acid to oxidize the iron present, adding oxalic acid and thereafter separating the thorium oxalate thus precipitated.

  19. 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.

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

    PubMed

    Veliscek-Carolan, Jessica

    2016-11-15

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

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

    PubMed Central

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

    2013-01-01

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

  2. Thorium-230 dating of carbonates: current technical capabilities and major applications

    NASA Astrophysics Data System (ADS)

    Edwards, R. L.; Cheng, H.; Pythoud, M.; Lu, Y.; Zhang, P.; Nissen, J.; Berry, A.; Cross, M.

    2015-12-01

    Uranium-thorium or Th-230 dating has proven to be an important tool in determining the timing of events in the late Quaternary. Among the major applications are: the timing of sea level change, the timing of continental climate change as preserved in cave archives, the timing of climate change in marine and ice core archives through correlation to Th-230 - dated cave records, and calibration of the radiocarbon timescale. The success of these applications has been driven by continuing technical advances in the measurement of the rare actinide isotopes, U-234 and Th-230. The advances have improved the precision, sensitivity, and accuracy of the measurements. The main factor in measurement improvement has been an increase of about 5 orders of magnitude (over the past 30 years) in the fraction of the sample that can be detected, dramatically improving counting statistics, as well as measurement sensitivity. The 5-order of magnitude improvement, comes largely from the shift to mass spectrometric measurement techniques, but also has resulted from subsequent improvement in ionization plus transmission efficiency. While additional improvement above the 5-order of magnitude figure may be possible, current efforts are focused on improving the accuracy of the measurements, standardizing gravimetric standards among laboratories, and shortening measurement times. These efforts will be discussed along with summary results of some of the major applications.

  3. 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.

  4. 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.

  5. 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.

  6. PLUTONIUM PURIFICATION PROCESS EMPLOYING THORIUM PYROPHOSPHATE CARRIER

    DOEpatents

    King, E.L.

    1959-04-28

    The separation and purification of plutonium from the radioactive elements of lower atomic weight is described. The process of this invention comprises forming a 0.5 to 2 M aqueous acidffc solution containing plutonium fons in the tetravalent state and elements with which it is normally contaminated in neutron irradiated uranium, treating the solution with a double thorium compound and a soluble pyrophosphate compound (Na/sub 4/P/sub 2/O/sub 7/) whereby a carrier precipitate of thorium A method is presented of reducing neptunium and - trite is advantageous since it destroys any hydrazine f so that they can be removed from solutions in which they are contained is described. In the carrier precipitation process for the separation of plutonium from uranium and fission products including zirconium and columbium, the precipitated blsmuth phosphate carries some zirconium, columbium, and uranium impurities. According to the invention such impurities can be complexed and removed by dissolving the contaminated carrier precipitate in 10M nitric acid, followed by addition of fluosilicic acid to about 1M, diluting the solution to about 1M in nitric acid, and then adding phosphoric acid to re-precipitate bismuth phosphate carrying plutonium.

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

    NASA Astrophysics Data System (ADS)

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

    2016-07-01

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

  8. METHOD OF SEPARATING URANIUM FROM ALLOYS

    DOEpatents

    Chiotti, P.; Shoemaker, H.E.

    1960-06-28

    Uranium can be recovered from metallic uraniumthorium mixtures containing uranium in comparatively small amounts. The method of recovery comprises adding a quantity of magnesium to a mass to obtain a content of from 48 to 85% by weight; melting and forming a magnesium-thorium alloy at a temperature of between 585 and 800 deg C; agitating the mixture, allowing the mixture to settle whereby two phases, a thorium-containing magnesium-rich liquid phase and a solid uranium-rich phase, are formed; and separating the two phases.

  9. Synthesis, structure and bonding of actinide disulphide dications in the gas phase.

    PubMed

    Lucena, Ana F; Bandeira, Nuno A G; Pereira, Cláudia C L; Gibson, John K; Marçalo, Joaquim

    2017-04-11

    Actinide disulphide dications, AnS2(2+), were produced in the gas phase for An = Th and Np by reaction of An(2+) cations with the sulfur-atom donor COS, in a sequential abstraction process of two sulfur atoms, as examined by FTICR mass spectrometry. For An = Pu and Am, An(2+) ions were unreactive with COS and did not yield any sulphide species. High level multiconfigurational (CASPT2) calculations were performed to assess the structures and bonding of the new AnS2(2+) species obtained for An = Th, Np, as well as for An = Pu to examine trends along the An series, and for An = U to compare with a previous experimental study and DFT computational scrutiny of US2(2+). The CASPT2 results showed that, like in the case of uranium, the new AnS2(2+) ions have ground states with triangular geometries, corresponding to the presence of a persulphide in the case of thorium that formally leads to a stable Th(IV)S2(2+) species, while a supersulphide appears to be present in the case of U, Np and Pu, formally leading to a An(III)S2(2+) species. The computations also revealed that linear thioactinyl structures are higher in energy, with a difference that increases fourfold upon moving from U to Pu, apparently indicating that it will be even more pronounced for Am.

  10. Minerals yearbook, 1988: Thorium

    SciTech Connect

    Hedrick, J.B.

    1988-01-01

    Mine production of monazite, the principal source of thorium, decreased slightly in 1988. Associated Minerals (USA) Inc. was the only domestic monazite producer. Monazite produced in the United States was exported, and the thorium products used domestically were derived from imported materials, existing company stocks, and thorium nitrate released from the National Defense Stockpile. Major nonenergy uses were in refractory applications, ceramics, and mantles for incandescent lanterns. The only energy use of thorium in the United States was in the high-temperature gas-cooled (HTGC) nuclear reactor at Fort St. Vrain, CO. Topics discussed in the report include domestic data coverage, legislation and government programs, domestic production, consumption and uses, stocks, prices, foreign trade, world capacity, and world review--(Australia, Brazil, Madagascar, Mozambique).

  11. Uranium-thorium-protactinium dating systematics

    SciTech Connect

    Cheng, H.; Edwards, R.L.; Murrell, M.T.; Benjamin, T.M.

    1998-11-01

    With precise {sup 234}U, {sup 230}Th, and {sup 231}Pa data available, {sup 230}Th and {sup 231}Pa ages can now be tested rigorously for concordancy. If the material is not concordant, the isotope characteristics of this material may be examined in some detail. Here, models similar to those used to describe the U-Pb system are evaluated for use in U-Th-Pa studies, for the case in which initial {sup 230}Th and {sup 231}Pa concentrations are effectively zero. The systematics of concordia plots in relation to models of variation in {delta}{sup 234}U, episodic U or loss or gain, continuous U loss or gain, and continuous {sup 234}U, {sup 230}Th and {sup 231}Pa gain or loss are considered for the case in which initial U concentration is significant (for example, in many carbonate deposits). The authors also examine linear U uptake models for the case in which initial U concentration is effectively zero (for example, in teeth and bones). Such models should prove useful in interpreting data from materials that have behaved as open-systems. In particular, these models may help constrain the nature of diagenetic processes, and in some situations it may be possible to determine or constrain true ages with materials that have behaved as open-systems.

  12. Preliminary summary review of thorium-bearing mineral occurrences in Alaska

    USGS Publications Warehouse

    Bates, Robert G.; Wedow, Helmuth

    1952-01-01

    Thorium-bearing minerals are known at 47 localities in Alaska. At these localities the thorium occurs as a major constituent or in minor amounts as an impurity in one or more of the following 12 minerals: allanite, columbite, ellsworthite, eschynite, gummite, monazite, orangite, parisite, thorianite, thorite, xenotime, and zircon. In addition other minerals, such as biotite and sphene, are radioactive and may contain thorium. Several unidentified columbate minerals with uranium or thorium and uranium as major constituents have been recognized at some localities. The distribution, by type of deposit, of the 57 thorium occurrences is as follows: lode - 3, lode and placer - 1, granitic rock - 3, granitic rock and related placer - 14, and placer - 26. Of the four lode occurrences only the radioactive veins at Salmon Bay in southeastern Alaska and the contact metamorphic deposit in the Nixon Fork area of central Alaska warrant further consideration, although insufficient data are available to determine whether these two deposits have commercial possibilities. The remaining occurrences of thorium-bearing minerals in Alaska are limited to placer deposits and disseminations of accessory minerals in granitic rocks. In most of these occurrences the thorium-bearing minerals occur in only trace amounts and consequently warrent little further consideration. More data are needed to determine the possibilities of byproduct recovery of thorium-bearing minerals from several of the gold and tin placers.

  13. Inhalation radiotoxicity of irradiated thorium as a heavy water reactor fuel

    SciTech Connect

    Edwards, G.W.R.; Priest, N.D.; Richardson, R.B.

    2013-07-01

    The online refueling capability of Heavy Water Reactors (HWRs), and their good neutron economy, allows a relatively high amount of neutron absorption in breeding materials to occur during normal fuel irradiation. This characteristic makes HWRs uniquely suited to the extraction of energy from thorium. In Canada, the toxicity and radiological protection methods dealing with personnel exposure to natural uranium (NU) spent fuel (SF) are well-established, but the corresponding methods for irradiated thorium fuel are not well known. This study uses software to compare the activity and toxicity of irradiated thorium fuel ('thorium SF') against those of NU. Thorium elements, contained in the inner eight elements of a heterogeneous high-burnup bundle having LEU (Low-enriched uranium) in the outer 35 elements, achieve a similar burnup to NU SF during its residence in a reactor, and the radiotoxicity due to fission products was found to be similar. However, due to the creation of such inhalation hazards as U-232 and Th-228, the radiotoxicity of thorium SF was almost double that of NU SF after sufficient time has passed for the decay of shorter-lived fission products. Current radio-protection methods for NU SF exposure are likely inadequate to estimate the internal dose to personnel to thorium SF, and an analysis of thorium in fecal samples is recommended to assess the internal dose from exposure to this fuel. (authors)

  14. 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.

  15. Evaluation of in vitro dissolution rates of throum in uranium mill tailings

    SciTech Connect

    Reif, R.G.

    1996-06-01

    Dissolution rates of thorium from the uranium mill tailings piles at two Department of Energy Uranium Mill Tailings Remedial Action Project (UMTRAP) sites have been evaluated. The thorium dissolution rates were evaluated in vitro using simulated lung fluid. The former uranium mills at the UMTRAP sites employed different chemical processes (acid leach and alkaline pressure leach) to extract the uranium from the ore, and the thorium dissolution rates at these sites were found to be markedly different. A site specific annual limit on intake (ALI) value for {sup 230}Th was calculated for the UMTRAP Site that was associated with a multiple component dissolution curve.

  16. METHOD OF SEPARATING URANIUM VALUES, PLUTONIUM VALUES AND FISSION PRODUCTS BY CHLORINATION

    DOEpatents

    Brown, H.S.; Seaborg, G.T.

    1959-02-24

    The separation of plutonium and uranium from each other and from other substances is described. In general, the method comprises the steps of contacting the uranium with chlorine in the presence of a holdback material selected from the group consisting of lanthanum oxide and thorium oxide to form a uranium chloride higher than uranium tetrachloride, and thereafter heating the uranium chloride thus formed to a temperature at which the uranium chloride is volatilized off but below the volatilizalion temperature of plutonium chloride.

  17. 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)

  18. The role of chemical interactions between thorium, cerium, and lanthanum in lymphocyte toxicity.

    PubMed

    Oliveira, Monica S; Duarte, Isabelle M; Paiva, Amanda V; Yunes, Samira N; Almeida, Carlos E; Mattos, Rita C; Sarcinelli, Paula N

    2014-01-01

    Thorium, cerium, and lanthanum are metals present in several types of minerals, the most common of which is monazite. Cerium and lanthanum are elements in the lanthanides series. Thorium, an actinide metal, is a hazardous element due to its radioactive characteristics. There is a lack of information describing the possible chemical interactions among these elements and the effects they may have on humans. Toxicological analyses were performed using cell viability, cell death, and DNA damage assays. Chemical interactions were evaluated based on the Loewe additivity model. The results indicate that thorium and cerium individually have no toxic effects on lymphocytes. However, thorium associated with lanthanum increases the toxicity of this element, thereby reducing the viability of lymphocytes at low concentrations of metals in the mixture.

  19. 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.

  20. THORIUM OXALATE-URANYL ACETATE COUPLED PROCEDURE FOR THE SEPARATION OF RADIOACTIVE MATERIALS

    DOEpatents

    Gofman, J.W.

    1959-08-11

    The recovery of fission products from neutronirradiated uranium is described. The neutron-irradiated uranium is dissolved in acid and thorium oxalate is precipitated in ihe solution formed, whereby the fission products are carried on the thorium oxalate. The separated thorium oxalate precipitate is then dissolved in an aqueous oxalate solution and the solution formed is acidified, limiting ihe excess acidity to a maximum of 2 N, whereby thorium oxalate precipitates and carries lanthanum-rareearth- and alkaline-earth-metal fission products while the zirconium-fission-product remains in solution. This precipitate, too, is dissolved in an aqaeous oxalate solution at elevated temperature, and lanthanum-rare-earth ions are added to the solution whereby lanthanum-rare-earth oxalate forms and the lanthanum-rare-earth-type and alkalineearth-metal-type fission products are carried on the oxalate. The precipitate is separated from the solution.

  1. ZIRCONIUM-CLADDING OF THORIUM

    DOEpatents

    Beaver, R.J.

    1961-11-21

    A method of cladding thorium with zirconium is described. The quality of the bond achieved between thorium and zirconium by hot-rolling is improved by inserting and melting a thorium-zirconium alloy foil between the two materials prior to rolling. (AEC)

  2. 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.

  3. 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.

  4. 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.

  5. 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

  6. Thorium in mineral products.

    PubMed

    Collier, D E; Brown, S A; Blagojevic, N; Soldenhoff, K H; Ring, R J

    2001-01-01

    Many ores contain low levels of thorium. When these ores are processed, the associated radioactivity can be found in mineral concentrates, intermediates and final products. There is an incentive for industries to remove radioactivity from mineral products to allow the movement and sale of these materials, both nationally and internationally, without the need for licensing. Control of thorium in various products involves the development and optimisation of process steps to be able to meet product specifications. The Australian Nuclear Science and Technology Organisation (ANSTO) has undertaken a range of R & D programmes targeting the treatment of thorium-bearing minerals. This paper discusses the application of a microprobe technique for siting radioactivity in zircon and ilmenite and the problems experienced in measuring the concentrations in solid rare earth products.

  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. Analysis of key safety metrics of thorium utilization in LWRs

    DOE PAGES

    Ade, Brian J.; Bowman, Stephen M.; Worrall, Andrew; ...

    2016-04-08

    Here, thorium has great potential to stretch nuclear fuel reserves because of its natural abundance and because it is possible to breed the 232Th isotope into a fissile fuel (233U). Various scenarios exist for utilization of thorium in the nuclear fuel cycle, including use in different nuclear reactor types (e.g., light water, high-temperature gas-cooled, fast spectrum sodium, and molten salt reactors), along with use in advanced accelerator-driven systems and even in fission-fusion hybrid systems. The most likely near-term application of thorium in the United States is in currently operating light water reactors (LWRs). This use is primarily based on conceptsmore » that mix thorium with uranium (UO2 + ThO2) or that add fertile thorium (ThO2) fuel pins to typical LWR fuel assemblies. Utilization of mixed fuel assemblies (PuO2 + ThO2) is also possible. The addition of thorium to currently operating LWRs would result in a number of different phenomenological impacts to the nuclear fuel. Thorium and its irradiation products have different nuclear characteristics from those of uranium and its irradiation products. ThO2, alone or mixed with UO2 fuel, leads to different chemical and physical properties of the fuel. These key reactor safety–related issues have been studied at Oak Ridge National Laboratory and documented in “Safety and Regulatory Issues of the Thorium Fuel Cycle” (NUREG/CR-7176, U.S. Nuclear Regulatory Commission, 2014). Various reactor analyses were performed using the SCALE code system for comparison of key performance parameters of both ThO2 + UO2 and ThO2 + PuO2 against those of UO2 and typical UO2 + PuO2 mixed oxide fuels, including reactivity coefficients and power sharing between surrounding UO2 assemblies and the assembly of interest. The decay heat and radiological source terms for spent fuel after its discharge from the reactor are also presented. Based on this evaluation, potential impacts on safety requirements and identification of

  9. Analysis of key safety metrics of thorium utilization in LWRs

    SciTech Connect

    Ade, Brian J.; Bowman, Stephen M.; Worrall, Andrew; Powers, Jeffrey

    2016-04-08

    Here, thorium has great potential to stretch nuclear fuel reserves because of its natural abundance and because it is possible to breed the 232Th isotope into a fissile fuel (233U). Various scenarios exist for utilization of thorium in the nuclear fuel cycle, including use in different nuclear reactor types (e.g., light water, high-temperature gas-cooled, fast spectrum sodium, and molten salt reactors), along with use in advanced accelerator-driven systems and even in fission-fusion hybrid systems. The most likely near-term application of thorium in the United States is in currently operating light water reactors (LWRs). This use is primarily based on concepts that mix thorium with uranium (UO2 + ThO2) or that add fertile thorium (ThO2) fuel pins to typical LWR fuel assemblies. Utilization of mixed fuel assemblies (PuO2 + ThO2) is also possible. The addition of thorium to currently operating LWRs would result in a number of different phenomenological impacts to the nuclear fuel. Thorium and its irradiation products have different nuclear characteristics from those of uranium and its irradiation products. ThO2, alone or mixed with UO2 fuel, leads to different chemical and physical properties of the fuel. These key reactor safety–related issues have been studied at Oak Ridge National Laboratory and documented in “Safety and Regulatory Issues of the Thorium Fuel Cycle” (NUREG/CR-7176, U.S. Nuclear Regulatory Commission, 2014). Various reactor analyses were performed using the SCALE code system for comparison of key performance parameters of both ThO2 + UO2 and ThO2 + PuO2 against those of UO2 and typical UO2 + PuO2 mixed oxide fuels, including reactivity coefficients and power sharing between surrounding UO2 assemblies and the assembly of interest. The decay heat and

  10. Gas-phase chemistry of bare and oxo-ligated protactinium ions: a contribution to a systematic understanding of actinide chemistry.

    PubMed

    Gibson, John K; Haire, Richard G

    2002-11-04

    Gas-phase chemistry of bare and oxo-ligated protactinium ions has been studied for the first time. Comparisons were made with thorium, uranium, and neptunium ion chemistry to further the systematic understanding of 5f elements. The rates of oxidation of Pa(+) and PaO(+) by ethylene oxide compared with those of the homologous uranium ions indicate that the first and second bond dissociation energies, BDE[Pa(+)-O] and BDE[OPa(+)-O], are approximately 800 kJ mol(-1). The relatively facile fluorination of Pa(+) to PaF(4)(+) by SF(6) is consistent with the high stability of the pentavalent oxidation state of Pa. Reactions with ethene, propene, 1-butene, and iso-butene revealed that Pa(+) is a very reactive metal ion. In analogy with U(+) chemistry, ethene was trimerized by Pa(+) to give PaC(6)H(6)(+). Reactions of Pa(+) with larger alkenes resulted in secondary and tertiary products not observed for U(+) or Np(+). The bare protactinium ion is significantly more reactive with organic substrates than are heavier actinide ions. The greatest difference between Pa and heavier actinide congeners was the exceptional dehydrogenation activity of PaO(+) with alkenes; UO(+) and NpO(+) were comparatively inert. The striking reactivity of PaO(+) is attributed to the distinctive electronic structure at the metal center in this oxide, which is considered to reflect the greater availability of the 5f electrons for participation in bonding, either directly or by promotion/hybridization with higher-energy valence orbitals.

  11. 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)

  12. Unique advantages of organometallic supporting ligands for uranium complexes

    SciTech Connect

    Diaconescu, Paula L.; Garcia, Evan

    2014-05-31

    The objective of our research project was to study the reactivity of uranium complexes supported by ferrocene-based ligands. In addition, this research provides training of graduate students as the next generation of actinide scientists.

  13. PLUTONIUM-THORIUM ALLOYS

    DOEpatents

    Schonfeld, F.W.

    1959-09-15

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

  14. 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.

  15. Determination of trace amounts of thorium by electroanalytical techniques.

    PubMed

    Mazzocchin, G A; Daniele, S; Moretto, L M

    1990-03-01

    Trace amounts of thorium have been determined in the presence of uranyl nitrate and ammonium diuranate (as interferents) by cyclic voltammetry, differential-pulse polarography, differential-pulse voltammetry, square-wave voltammetry and anodic-stripping voltammetry. The determination is based on the substitution of thorium for copper, lead and cadmium in their EDTA complexes and voltammetric measurement of the displaced metal ion. The detection limits ranged between 2 x 10(-7) and 1 x 10(-6)M (r.s.d. 2-7%) for solutions free from the uranium compounds, and between 8 x 10(-7) and 5 x 10(-6)M (r.s.d. 3-5%) in the presence of the uranium compounds at concentrations up to about 1000 times that of thorium. The detection limits depend on both the particular technique and the EDTA complex employed. Anodic-stripping voltammetry gave detection limits of 8 x 10(-8) and 10(-7)M in the absence and presence of uranium respectively.

  16. Verification study of thorium cross section in MVP calculation of thorium based fuel core using experimental data

    SciTech Connect

    Mai, V. T.; Fujii, T.; Wada, K.; Kitada, T.; Takaki, N.; Yamaguchi, A.; Watanabe, H.; Unesaki, H.

    2012-07-01

    Considering the importance of thorium data and concerning about the accuracy of Th-232 cross section library, a series of experiments of thorium critical core carried out at KUCA facility of Kyoto Univ. Research Reactor Inst. have been analyzed. The core was composed of pure thorium plates and 93% enriched uranium plates, solid polyethylene moderator with hydro to U-235 ratio of 140 and Th-232 to U-235 ratio of 15.2. Calculations of the effective multiplication factor, control rod worth, reactivity worth of Th plates have been conducted by MVP code using JENDL-4.0 library [1]. At the experiment site, after achieving the critical state with 51 fuel rods inserted inside the reactor, the measurements of the reactivity worth of control rod and thorium sample are carried out. By comparing with the experimental data, the calculation overestimates the effective multiplication factor about 0.90%. Reactivity worth of the control rods evaluation using MVP is acceptable with the maximum discrepancy about the statistical error of the measured data. The calculated results agree to the measurement ones within the difference range of 3.1% for the reactivity worth of one Th plate. From this investigation, further experiments and research on Th-232 cross section library need to be conducted to provide more reliable data for thorium based fuel core design and safety calculation. (authors)

  17. Establishing bounding internal dose estimates for thorium activities at Rocky Flats.

    PubMed

    Ulsh, Brant A; Rich, Bryce L; Chew, Melton H; Morris, Robert L; Sharfi, Mutty; Rolfes, Mark R

    2008-07-01

    As part of an evaluation of a Special Exposure Cohort petition filed on behalf of workers at the Rocky Flats Plant, the National Institute for Occupational Safety and Health (NIOSH) was required to demonstrate that bounding values could be established for radiation doses due to the potential intake of all radionuclides present at the facility. The main radioactive elements of interest at Rocky Flats were plutonium and uranium, but much smaller quantities of several other elements, including thorium, were occasionally handled at the site. Bounding potential doses from thorium has proven challenging at other sites due to the early historical difficulty in detecting this element through urinalysis methods and the relatively high internal dose delivered per unit intake. This paper reports the results of NIOSH's investigation of the uses of thorium at Rocky Flats and provides bounding dose reconstructions for these operations. During this investigation, NIOSH reviewed unclassified reports, unclassified extracts of classified materials, material balance and inventory ledgers, monthly progress reports from various groups, and health physics field logbooks, and conducted interviews with former Rocky Flats workers. Thorium operations included: (1) an experimental metal forming project with 240 kg of thorium in 1960; (2) the use of pre-formed parts in weapons mockups; (3) the removal of Th from U; (4) numerous analytical procedures involving trace quantities of thorium; and (5) the possible experimental use of thorium as a mold coating compound. The thorium handling operations at Rocky Flats were limited in scope, well-monitored and documented, and potential doses can be bounded.

  18. 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

  19. 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.

  20. Improvement of the thermal margins in the Swedish Ringhals-3 PWR by introducing new fuel assemblies with thorium

    SciTech Connect

    Lau, C. W.; Demaziere, C.; Nylen, H.; Sandberg, U.

    2012-07-01

    Thorium is a fertile material and most of the past research has focused on breeding thorium to fissile material. In this paper, the focus is on using thorium to improve the thermal margins by homogeneously distributing thorium in the fuel pellets. A proposed uranium-thorium-based fuel assembly is simulated for the Swedish Ringhals-3 PWR core in a realistic demonstration. All the key safety parameters, such as isothermal temperature coefficient of reactivity, Doppler temperature of reactivity, boron worth, shutdown margins and fraction of delayed neutrons are studied in this paper, and are within safety limits for the new core design using the uranium-thorium-based fuel assemblies. The calculations were performed by the two-dimensional transport code CASMO-4E and the two group steady-state three dimensional nodal code SIMULATE-3 from Studsvik Scandpower. The results showed that the uranium-thorium-based fuel assembly improves the thermal margins, both in the pin peak power and the local power (Fq). The improved thermal margins would allow more flexible core designs with less neutron leakage or could be used in power uprates to offer efficient safety margins. (authors)

  1. 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)

  2. 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.

  3. 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.

  4. 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).

  5. Annual report of the United States transuranium and uranium registries, October 1, 1988--September 30, 1989

    SciTech Connect

    Kathren, R.L.; Swint, M.J.; Dietert, S.E.

    1990-04-01

    This report summarizes the primary scientific activities of the United States Transuranium and Uranium Registries for the period October 1, 1988 through September 30, 1989. The Registries are parallel human tissue research programs devoted to the study of the actinide elements in man. The emphasis of the Transuranium Registry was directed toward evaluation of six whole body donations. In the five cases whose exposure was through inhalation, approximately half of the total body content of Pu-239 + 240 and a third of the Am-241 was found in the respiratory tract, suggesting that these nuclides are more avidly retained than predicted by the current model of the International Commission on Radiological Protection. A significant fraction of these nuclides is found in soft tissues other than liver, and an uptake fraction of 0.2 is proposed for muscle, with a residence half-time of 10 years. Studies of these and routine autopsy cases indicate that more than 90% of the total respiratory tract plutonium or americium is in the lungs, with the remainder in the lymph nodes, and that a greater fraction is found in the lungs of smokers relative to the lymph nodes. Primary activities of the Uranium Registry centered around the acquisition of a whole body donation from a woman who had received an injection of colloidal thorium dioxide some 38 years prior to death.

  6. 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

  7. 76 FR 63330 - Policy Regarding Submittal of Amendments for Processing of Equivalent Feed at Licensed Uranium...

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-10-12

    ... of Amendments for Processing of Equivalent Feed at Licensed Uranium Recovery Facilities AGENCY... amendment, of equivalent feed at an NRC and Agreement State-licensed uranium recovery site. This action is... Licensing of Uranium and Thorium Recovery Facilities--Proposed New 10 CFR Part 41,'' available at...

  8. Influence of hydrofluoric acid on extraction of thorium using a commercially available extraction chromatographic resin.

    PubMed

    Shimada-Fujiwara, Asako; Hoshi, Akiko; Kameo, Yutaka; Nakashima, Mikio

    2009-05-01

    The dependence of Th recovery on hydrofluoric acid (HF) concentration in nitric acid (HNO(3)) solutions (1-5 mol/dm(3)) containing 1x10(-6) mol/dm(3) of Th and various concentrations of HF and the elution behavior were studied using a commercially available UTEVA (for uranium and tetravalent actinide) resin column. Thorium recovery decreased with an increase in HF concentration in the sample solutions. The concentration of HF at which Th recovery started to decrease was approximately 1x10(-4) mol/dm(3) in 1 mol/dm(3) HNO(3) solution, approximately 1x10(-3) mol/dm(3) in 3 mol/dm(3) HNO(3) solution, and approximately 1x10(-2) mol/dm(3) in 5 mol/dm(3) HNO(3) solution. When Al(NO(3))(3) (0.2 mol/dm(3)) or Fe(NO(3))(3) (0.6 mol/dm(3)) was added as a masking agent for F(-) to the Th solution containing 1x10(-1) mol/dm(3) HF and 1 mol/dm(3) HNO(3), Th recovery improved from 1.4+/-0.3% to 95+/-5% or 93+/-3%. Effective extraction of Th using UTEVA resin was achieved by selecting the concentration of HNO(3) and/or adding masking agents such as Al(NO(3))(3) according to the concentration of HF in the sample solution.

  9. 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)

  10. Accelerator Driven Nuclear Energy: The Thorium Option

    ScienceCinema

    Raja, Rajendran

    2016-07-12

    Conventional nuclear reactors use enriched Uranium as fuel and produce nuclear waste which needs to be stored away for over 10,000 years.   At the current rate of use, existing sources of Uranium will last for 50-100 years.  We describe a solution to the problem that uses particle accelerators to produce fast neutrons that can be used to burn existing nuclear waste and produce energy.  Such systems, initially proposed by Carlo Rubbia and collaborators in the 1990's, are being seriously considered by many countries as a possible solution to the green energy problem.  Accelerator driven reactors operate in a sub-critical regime and, thus, are safer and can obtain energy from plentiful elements such as Thorium-232 and Uranium-238. What is missing is the high intensity (10MW) accelerator that produces 1 GeV protons. We will describe scenarios which if implemented will make such systems a reality.  

  11. The extraction of actinides from nitric acid solutions with diamides of dipicolinic acid

    NASA Astrophysics Data System (ADS)

    Lapka, Joseph L.; Paulenova, Alena; Alyapyshev, Mikhail Yu; Babain, Vasiliy A.; Law, Jack D.; Herbst, R. Scott

    2010-03-01

    Diamides of dipicolinic acid (N,N'-diethyl-N,N'-ditolyl-dipicolinamide, EtTDPA) were synthesized and evaluated for their extraction capability for actinides. In this work the extractions of neptunium(V), protactinium(V), and thorium(IV) with EtTDPA in a polar fluorinated diluent from nitric acid were investigated. EtTDPA shows a high affinity for Th(IV) even at millimolar concentrations. Np(V) and Pa(V) are both reasonably extractable with EtTDPA; however, near saturated solutions are required to achieve appreciable distribution ratios. A comparison with previously published actinide extraction data is given.

  12. RECOVERY OF URANIUM BY CYCLOALKYLDITHIO-CARBAMATE COMPLEXING

    DOEpatents

    Neville, O.K.

    1959-06-30

    The separation of uranium-233 from an aqueous nitric acid solution of neutron irradiated thorium by selectively complexing the uranium is described. The separation is carried out by contacting the thorium solution with a non- aromatic organic dithiocarbamate selected from the group which consists of alkali and alkaline earth cycloalkyldithiocarbamates and recovering the resulting uranyl cycloalkyldithiocarbamate complex by organic solvent extraction such as with methyl ethyl ketone. The complexed uranium may be stripped from the separated organic phase by scrubbing with one normal nitric acid solution.

  13. 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.

  14. Geological and geochemical aspects of uranium deposits. A selected, annotated bibliography

    SciTech Connect

    Garland, P.A.; Thomas, J.M.; Brock, M.L.; Daniel, E.W.

    1980-06-01

    A bibliography of 479 references encompassing the fields of uranium and thorium geochemistry and mineralogy, geology of uranium deposits, uranium mining, and uranium exploration techniques has been compiled by the Ecological Sciences Information Center of Oak Ridge National Laboratory. The bibliography was produced for the National Uranium Resource Evaluation Program, which is funded by the Grand Junction Office of the Department of Energy. The references contained in the bibliography have been divided into the following eight subject categories: (1) geology of deposits, (2) geochemistry, (3) genesis O deposits, (4) exploration, (5) mineralogy, (6) uranium industry, (7) reserves and resources, and (8) geology of potential uranium-bearing areas. All categories specifically refer to uranium and thorium; the last category contains basic geologic information concerning areas which the Grand Junction Office feels are particularly favorable for uranium deposition. The references are indexed by author, geographic location, quadrangle name, geoformational feature, taxonomic name, and keyword.

  15. High resolution analysis of uranium and thorium concentration as well as U-series isotope distributions in a Neanderthal tooth from Payre (Ardèche, France) using laser ablation ICP-MS

    NASA Astrophysics Data System (ADS)

    Grün, Rainer; Aubert, Maxime; Joannes-Boyau, Renaud; Moncel, Marie-Hélène

    2008-11-01

    We have mapped U ( 238U) and Th ( 232Th) elemental concentrations as well as U-series isotope distributions in a Neanderthal tooth from the Middle Palaeolithic site of Payre using laser ablation ICP-MS. The U-concentrations in an enamel section varied between 1 and 1500 ppb. The U-concentration maps show that U-migration through the external enamel surface is minute, the bulk of the uranium having migrated internally via the dentine into the enamel. The uranium migration and uptake is critically dependent on the mineralogical structure of the enamel. Increased U-concentrations are observed along lineaments, some of which are associated with cracks, and others may be related to intra-prismatic zones or structural weaknesses reaching from the dentine into the enamel. The uranium concentrations in the dentine vary between about 25,000 and 45,000 ppb. Our systematic mapping of U-concentration and U-series isotopes provides insight into the time domain of U-accumulation. Most of the uranium was accumulated in an early stage of burial, with some much later overprints. None of the uranium concentration and U-series profiles across the root of the tooth complied with a single stage diffusion-adsorption (D-A) model that is used for quality control in U-series dating of bones and teeth. Nevertheless, in the domains that yielded the oldest apparent U-series age estimates, U-leaching could be excluded. This means that the oldest apparent U-series ages of around 200 ka represent a minimum age for this Neanderthal specimen. This is in good agreement with independent age assessments (200-230 ka) for the archaeological layer, in which it was found. The Th elemental concentrations in the dental tissues were generally low (between about 1 and 20 ppb), and show little relationship with the nature of the tissue.

  16. Structures of dimeric hydrolysis products of thorium.

    PubMed

    Wilson, Richard E; Skanthakumar, S; Sigmon, Ginger; Burns, Peter C; Soderholm, L

    2007-04-02

    Three unique thorium dimeric compounds have been crystallized from either direct hydrolysis of Th4+(aq)/HCl or titration of Th(OH)4(am) with Th(NO3)4(aq) and their structures determined using single-crystal X-ray diffraction. The compound [Th2(micro2-OH)2(NO3)6(H2O)6]H2O (1) is identical to that identified previously by Johansson. Two additional unreported compounds have been identified, [Th2(micro2-OH)2(NO3)4(H2O)8](NO3)2 (2) and [Th2(micro2-OH)2Cl2(H2O)12]Cl4.2H2O (3). 1 crystallizes in the monoclinic space group P21/c, with a = 6.792(2) A, b = 11.710(4) A, c = 13.778(5) A, and beta = 102.714(5) degrees and 2 crystallizes in the monoclinic space group P21/n, with a = 6.926(5) A, b = 7.207(1) A, c = 21.502(1) A, and beta = 96.380(1) degrees . The chloride-containing dimer, 3, crystallizes in triclinic P, with a = 8.080(2) A, b = 8.880(2) A, c = 9.013(2) A, alpha = 97.41(3) degrees , beta = 91.00(3), and gamma = 116.54(3) degrees . We also present high-energy X-ray scattering data demonstrating the presence of the hydroxo-bridged moiety in solution and discuss our findings in the context of known solid-state structures. The three structures demonstrate 11-, 10-, and 9-coordinate thorium, respectively, and coupled with the scattering experiments provide additional structural and chemical insight into tetravalent actinide hydrolysis.

  17. Recovery of protactinium-231 and thorium-230 from cotter concentrate: pilot plant operatins and process development

    SciTech Connect

    Hertz, M.R.; Figgins, P.E.; Deal, W.R.

    1983-02-10

    The equipment and methods used to recover and purify 339 g of thorium-230 and 890 mg of protactinium-231 from 22 of the 1251 drums of Cotter Concentrate are described. The process developed was (1) dissolution at 100/sup 0/C in concentrated nitric acid and dilution to 2 to 3 molar acid, (2) filtration to remove undissolved solids (mostly silica filter aid), (3) extraction of uranium with di-sec-butyl-phenyl phophonate (DSBPP) in carbon tetrachloride, (4) extraction of both thorium and protactinium with tri-n-octylphosphine oxide (TOPO) in carbon tetrachloride followed by selective stripping of the thorium with dilute of sulfuric acid, (5) thorium purification using oxalic acid, (6) stripping protactinium from the TOPO with oxalic acid, and (7) protactinium purification through a sequence of steps. The development of the separation procedures, the design of the pilot plant, and the operating procedures are described in detail. Analytical procedures are given in an appendix. 8 figures, 4 tables.

  18. 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.

  19. The separation of lanthanides and actinides in supercritical fluid carbon dioxide

    SciTech Connect

    Mincher, Bruce J.; Wai, Chien M.; Fox, Robert V.; Baek, Donna L.; Yen, Clive; Case, Mary E.

    2015-10-28

    Supercritical fluid carbon dioxide presents an attractive alternative to conventional solvents for recovery of the actinides and lanthanides. Carbon dioxide is a good solvent for fluorine and phosphate-containing ligands, including the traditional tributylphosphate ligand used in process-scale uranium separations. Actinide and lanthanide oxides may even be directly dissolved in carbon dioxide containing the complexes formed between these ligands and mineral acids, obviating the need for large volumes of acids for leaching and dissolution, and the corresponding organic liquid–liquid solvent extraction solutions. As a result, examples of the application of this novel technology for actinide and lanthanide separations are presented.

  20. Establishment of a room temperature molten salt capability to measure fundamental thermodynamic properties of actinide elements

    SciTech Connect

    Smith, W.H.; Costa, D.A.

    1998-12-31

    This is the final report of a six-month, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory (LANL). The goal of this work was to establish a capability for the measurement of fundamental thermodynamic properties of actinide elements in room temperature molten salts. This capability will be used to study in detail the actinide chloro- and oxo-coordination chemistries that dominate in the chloride-based molten salt media. Uranium will be the first actinide element under investigation.

  1. Design study of long-life PWR using thorium cycle

    SciTech Connect

    Subkhi, Moh. Nurul; Su'ud, Zaki; Waris, Abdul

    2012-06-06

    Design study of long-life Pressurized Water Reactor (PWR) using thorium cycle has been performed. Thorium cycle in general has higher conversion ratio in the thermal spectrum domain than uranium cycle. Cell calculation, Burn-up and multigroup diffusion calculation was performed by PIJ-CITATION-SRAC code using libraries based on JENDL 3.2. The neutronic analysis result of infinite cell calculation shows that {sup 231}Pa better than {sup 237}Np as burnable poisons in thorium fuel system. Thorium oxide system with 8%{sup 233}U enrichment and 7.6{approx} 8%{sup 231}Pa is the most suitable fuel for small-long life PWR core because it gives reactivity swing less than 1%{Delta}k/k and longer burn up period (more than 20 year). By using this result, small long-life PWR core can be designed for long time operation with reduced excess reactivity as low as 0.53%{Delta}k/k and reduced power peaking during its operation.

  2. PRETREATING THORIUM FOR ELECTROPLATING

    DOEpatents

    Beach, J.G.; Schaer, G.R.

    1959-07-28

    A method is presented for pretreating a thorium surface prior to electroplating the surface. The pretreatment steps of the invention comprise cleaning by vapor blasting the surface, anodically pickling in a 5 to 15% by volume aqueous hydrochloric acid bath with a current of 125 to 250 amp/sq ft for 3 to 5 min at room temperature, chemically pickling the surface in a 5 to 15% by volume of aqueous sulfuric acid for 3 to 5 min at room temperature, and rinsing the surface with water.

  3. Role of Minor Actinides for Long-Life Reactor Cores

    SciTech Connect

    Saito, M.; Artisyuk, V.; Shmelev, A.; Nikitin, K.; Peryoga, Y

    2002-07-01

    The paper addresses the study on advanced fuel cycles for LWR oriented to high burnup values that exceed 100 GWd/tHM, thus giving the chance to establish the long-life reactor cores without fuel reloading on site. The key element of this approach is a broad involvement of Minor Actinides whose admixture to 20% enriched uranium fuel provides safe release of initial reactivity excess and improved proliferation resistance properties. (authors)

  4. Determination of actinides in urine and fecal samples

    SciTech Connect

    McKibbin, T.T.

    1992-12-31

    A method of determining the radioactivity of specific actinides that are carried in urine or fecal sample material is disclosed. The samples are ashed in a muffle furnace, dissolved in an acid, and then treated in a series of steps of reduction, oxidation, dissolution, and precipitation, including a unique step of passing a solution through a chloride form anion exchange resin for separation of uranium and plutonium from americium.

  5. Determination of actinides in urine and fecal samples

    DOEpatents

    McKibbin, T.T.

    1993-03-02

    A method of determining the radioactivity of specific actinides that are carried in urine or fecal sample material is disclosed. The samples are ashed in a muffle furnace, dissolved in an acid, and then treated in a series of steps of reduction, oxidation, dissolution, and precipitation, including a unique step of passing a solution through a chloride form anion exchange resin for separation of uranium and plutonium from americium.

  6. Determination of actinides in urine and fecal samples

    DOEpatents

    McKibbin, Terry T.

    1993-01-01

    A method of determining the radioactivity of specific actinides that are carried in urine or fecal sample material is disclosed. The samples are ashed in a muffle furnace, dissolved in an acid, and then treated in a series of steps of reduction, oxidation, dissolution, and precipitation, including a unique step of passing a solution through a chloride form anion exchange resin for separation of uranium and plutonium from americium.

  7. Production of medical isotopes from a thorium target irradiated by light charged particles up to 70 MeV

    NASA Astrophysics Data System (ADS)

    Duchemin, C.; Guertin, A.; Haddad, F.; Michel, N.; Métivier, V.

    2015-02-01

    The irradiation of a thorium target by light charged particles (protons and deuterons) leads to the production of several isotopes of medical interest. Direct nuclear reaction allows the production of Protactinium-230 which decays to Uranium-230 the mother nucleus of Thorium-226, a promising isotope for alpha radionuclide therapy. The fission of Thorium-232 produces fragments of interest like Molybdenum-99, Iodine-131 and Cadmium-115g. We focus our study on the production of these isotopes, performing new cross section measurements and calculating production yields. Our new sets of data are compared with the literature and the last version of the TALYS code.

  8. Production of medical isotopes from a thorium target irradiated by light charged particles up to 70 MeV.

    PubMed

    Duchemin, C; Guertin, A; Haddad, F; Michel, N; Métivier, V

    2015-02-07

    The irradiation of a thorium target by light charged particles (protons and deuterons) leads to the production of several isotopes of medical interest. Direct nuclear reaction allows the production of Protactinium-230 which decays to Uranium-230 the mother nucleus of Thorium-226, a promising isotope for alpha radionuclide therapy. The fission of Thorium-232 produces fragments of interest like Molybdenum-99, Iodine-131 and Cadmium-115g. We focus our study on the production of these isotopes, performing new cross section measurements and calculating production yields. Our new sets of data are compared with the literature and the last version of the TALYS code.

  9. Correlation consistent basis sets for actinides. I. The Th and U atoms.

    PubMed

    Peterson, Kirk A

    2015-02-21

    New correlation consistent basis sets based on both pseudopotential (PP) and all-electron Douglas-Kroll-Hess (DKH) Hamiltonians have been developed from double- to quadruple-zeta quality for the actinide atoms thorium and uranium. Sets for valence electron correlation (5f6s6p6d), cc - pV nZ - PP and cc - pV nZ - DK3, as well as outer-core correlation (valence + 5s5p5d), cc - pwCV nZ - PP and cc - pwCV nZ - DK3, are reported (n = D, T, Q). The -PP sets are constructed in conjunction with small-core, 60-electron PPs, while the -DK3 sets utilized the 3rd-order Douglas-Kroll-Hess scalar relativistic Hamiltonian. Both series of basis sets show systematic convergence towards the complete basis set limit, both at the Hartree-Fock and correlated levels of theory, making them amenable to standard basis set extrapolation techniques. To assess the utility of the new basis sets, extensive coupled cluster composite thermochemistry calculations of ThFn (n = 2 - 4), ThO2, and UFn (n = 4 - 6) have been carried out. After accurately accounting for valence and outer-core correlation, spin-orbit coupling, and even Lamb shift effects, the final 298 K atomization enthalpies of ThF4, ThF3, ThF2, and ThO2 are all within their experimental uncertainties. Bond dissociation energies of ThF4 and ThF3, as well as UF6 and UF5, were similarly accurate. The derived enthalpies of formation for these species also showed a very satisfactory agreement with experiment, demonstrating that the new basis sets allow for the use of accurate composite schemes just as in molecular systems composed only of lighter atoms. The differences between the PP and DK3 approaches were found to increase with the change in formal oxidation state on the actinide atom, approaching 5-6 kcal/mol for the atomization enthalpies of ThF4 and ThO2. The DKH3 atomization energy of ThO2 was calculated to be smaller than the DKH2 value by ∼1 kcal/mol.

  10. Correlation consistent basis sets for actinides. I. The Th and U atoms

    SciTech Connect

    Peterson, Kirk A.

    2015-02-21

    New correlation consistent basis sets based on both pseudopotential (PP) and all-electron Douglas-Kroll-Hess (DKH) Hamiltonians have been developed from double- to quadruple-zeta quality for the actinide atoms thorium and uranium. Sets for valence electron correlation (5f6s6p6d), cc − pV nZ − PP and cc − pV nZ − DK3, as well as outer-core correlation (valence + 5s5p5d), cc − pwCV nZ − PP and cc − pwCV nZ − DK3, are reported (n = D, T, Q). The -PP sets are constructed in conjunction with small-core, 60-electron PPs, while the -DK3 sets utilized the 3rd-order Douglas-Kroll-Hess scalar relativistic Hamiltonian. Both series of basis sets show systematic convergence towards the complete basis set limit, both at the Hartree-Fock and correlated levels of theory, making them amenable to standard basis set extrapolation techniques. To assess the utility of the new basis sets, extensive coupled cluster composite thermochemistry calculations of ThF{sub n} (n = 2 − 4), ThO{sub 2}, and UF{sub n} (n = 4 − 6) have been carried out. After accurately accounting for valence and outer-core correlation, spin-orbit coupling, and even Lamb shift effects, the final 298 K atomization enthalpies of ThF{sub 4}, ThF{sub 3}, ThF{sub 2}, and ThO{sub 2} are all within their experimental uncertainties. Bond dissociation energies of ThF{sub 4} and ThF{sub 3}, as well as UF{sub 6} and UF{sub 5}, were similarly accurate. The derived enthalpies of formation for these species also showed a very satisfactory agreement with experiment, demonstrating that the new basis sets allow for the use of accurate composite schemes just as in molecular systems composed only of lighter atoms. The differences between the PP and DK3 approaches were found to increase with the change in formal oxidation state on the actinide atom, approaching 5-6 kcal/mol for the atomization enthalpies of ThF{sub 4} and ThO{sub 2}. The DKH3 atomization energy of ThO{sub 2} was calculated to be smaller than the DKH2

  11. CRYSTAL AND MOLECULAR STRUCTURE OF HYDRIDOTIS (BIS(TRIMETHYLSILYL)AMIDO]URANIUM(IV)

    SciTech Connect

    Andersen, Richard A.; Zalkin, Allen; Templeton, David H.

    1980-05-01

    New hydride derivatives of thorium (IV) and uranium (IV), HM[N(SiMe{sub 3}){sub 2}]{sub 3}, have recently been prepared. This paper describes the crystal structure of the uranium species, though the hydride-ion was not located, and shows that the thorium analogue is isostructural. The reaction chemistry and spectroscopy leave no doubt that these derivatives are authentic examples of four-coordinate, monomeric hydride, compounds.

  12. 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.

  13. National Uranium Resource Evaluation, Klamath Falls Quadrangle, Oregon and California

    SciTech Connect

    Castor, S.B.; Berry, M.R.; Robins, J.W.

    1982-07-01

    The Klamath Falls Quadrangle, Oregon, was evaluated to identify and delineate areas favorable for uranium deposits according to criteria developed for the National Uranium Resource Evaluation. Surface radiometric reconnaissance and geochemical sampling were used for overall evaluation of the quadrangle. Detailed rock sampling, geologic mapping, and examinations of uranium mines and occurrences were performed in suspected favorable areas. Results of the work indicate good potential for shallow hydrothermal volcanogenic uranium deposits in the Lakeview favorable area, which comprises a northwest-trending belt of rhyolite intrusions in the eastern half of the quadrangle. The young age, peraluminous chemistry, and low thorium-to-uranium ratios of the rhyolite intrusions, as well as low uranium content of groundwater samples, indicate that uranium has not been leached from the intrusions by ground water. Therefore, supergene uranium deposits are not likely in the area. Scattered occurrences of ash-flow tuff in the east half of the quadrangle that contain high uranium and (or) thorium contents, and four occurrences of secondary uranium minerals in ash-flow tuff, indicate possible uranium deposits in ash flows in a poorly defined area that is partially coextensive with the Lakeview favorable area. Small granitic plutons with associated quartz-tourmaline breccia veins and base-metal occurrences may also be favorable for uranium deposits but were not examined during this study.

  14. The role of transferrin in actinide(IV) uptake: comparison with iron(III).

    PubMed

    Jeanson, Aurélie; Ferrand, M; Funke, Harald; Hennig, Christoph; Moisy, Philippe; Solari, Pier Lorenzo; Vidaud, Claude; Den Auwer, Christophe

    2010-01-25

    The impact of actinides on living organisms has been the subject of numerous studies since the 1950s. From a general point of view, these studies show that actinides are chemical poisons as well as radiological hazards. Actinides in plasma are assumed to be mainly complexed to transferrin, the iron carrier protein. This paper casts light on the uptake of actinides(IV) (thorium, neptunium, plutonium) by transferrin, focusing on the pH dependence of the interaction and on a molecular description of the cation binding site in the protein. Their behavior is compared with that of iron(III), the endogenous transferrin cation, from a structural point of view. Complementary spectroscopic techniques (UV/Vis spectrophotometry, microfiltration coupled with gamma spectrometry, and X-ray absorption fine structure) have been combined in order to propose a structural model for the actinide-binding site in transferrin. Comparison of our results with data available on holotransferrin suggests some similarities between the behavior of Fe(III) and Np(IV)/Pu(IV)/ Np(IV) is not complexed at pH <7, whereas at pH approximately 7.4 complexation can be regarded as quantitative. This pH effect is consistent with the in vivo transferrin "cycle". Pu(IV) also appears to be quantitatively bound by apotransferrin at around pH approximately 7.5, whereas Th(IV) was never complexed under our experimental conditions. EXAFS data at the actinide edge have allowed a structural model of the actinide binding site to be elaborated: at least one tyrosine residue could participate in the actinide coordination sphere (two for iron), forming a mixed hydroxo-transferrin complex in which actinides are bound with transferrin both through An-tyrosine and through An--OH bonds. A description of interatomic distances is provided.

  15. Contributions to the geology of uranium and thorium by the United States Geological Survey and Atomic Energy Commission for the United Nations International Conference on Peaceful Uses of Atomic Energy, Geneva, Switzerland, 1955

    USGS Publications Warehouse

    Page, Lincoln R.; Stocking, Hobart E.; Smith, Harriet B.

    1956-01-01

    Within the boundaries of the United States abnormal amounts of uranium have been found in rocks of nearly all geologic ages and lithologic types. Distribution of ore is more restricted. On the Colorado Plateau, the Morrison formation of Jurassic age yields 61.4 percent of the ore produced in the United States, and the Chinle conglomerate and Shinarump formation of Triassic age contribute 26.0 and 5.8 percent, respectively. Clastic, carbonaceous, and carbonate sedimentary rocks of Tertiary, Mesozoic, and Paleozoic ages and veins of Tertiary age are the source of the remaining 6.8 percent.

  16. Analytical microscopy observations of rat enterocytes after oral administration of soluble salts of lanthanides, actinides and elements of group III-A of the periodic chart.

    PubMed

    Floren, C; Tekaya, L; Escaig, F; Labejof, L; Mouthon, G; Galle, P

    2001-05-01

    The behavior in the intestinal barrier of nine elements (three of the group III-A, four lanthanides and two actinides), absorbed as soluble salts, has been studied by two microanalytical methods: electron probe X-ray micro analysis (EPMA) and secondary ion mass spectrometry (SIMS). It has been shown that the three elements of group III-A, aluminium, gallium and indium; and the four lanthanides, lanthanum, cerium, europium and thulium, are selectively concentrated and precipitated as non-soluble form in enterocytes of proximal part of the intestinal tract. SIMS microscopy has shown that these elements are concentrated as a number of submicroscopic precipitates, most of them localized in the apical part of the duodenum enterocytes, where they are observed from one hour to 48 hr after a single intragastric administration. No precipitate is observed after three days. It is suggested that this mechanism of local concentration limits the diffusion of these elements through the digestive barrier, some of them being toxic and none of them having a recognized physiological role. Additionally, the precipitation in duodenal enterocytes, the life time of which is on the order of 2-3 days, allows the elements absorbed as soluble form to be eliminated as a non-soluble form in the digestive lumen along with the desquamation of the apoptotic enterocytes. The intracytoplasmic localization of the precipitates are supposed to be the lysosomes although no direct evidence could be given here due to the very small sizes of the lysosomes of enterocytes. The same results were not observed with the two studied actinides. After administration of thorium, only some very sparse microprecipitates could be observed in intestinal mucosa and, after administration of uranium, no precipitates were observed with the exception of some in the conjunctive part of the duodenal villi.

  17. METHOD FOR PRODUCING THORIUM TETRACHLORIDE

    DOEpatents

    Mason, E.A.; Cobb, C.M.

    1960-03-15

    A process for producing thorium tetrachloride from thorium concentrate comprises reacting thorium concentrates with a carbonaceous reducing agent in excess of 0.05 part by weight per part of thoriferous concentrate at a temperature in excess of 1300 deg C, cooling and comminuting the mass, chlorinating the resulting comminuting mass by suspending in a gaseous chlorinating agent in a fluidized reactor at a temperatare maintained between about l85 deg C and 770 deg C, and removing the resulting solid ThCl/sub 4/ from the reaction zone.

  18. Preparation and structure of uranium-incorporated Gd2Zr2O7 compounds and their thermodynamic stabilities under oxidizing and reducing conditions.

    PubMed

    Jafar, Mohsin; Phapale, Suhas B; Mandal, Balaji P; Mishra, Ratikant; Tyagi, Avesh K

    2015-10-05

    Gd2Zr2O7 is being contemplated as a futuristic matrix for the incorporation of high-level radioactive nuclear waste. This compound has the unique ability to incorporate several fission products and heavy metal ions like uranium and thorium into its lattice sites without undergoing structural changes. X-ray diffraction analyses of Gd2-xUxZr2O7+δ samples indicate that the parent compound can incorporate a substantial amount of uranium, both under oxidizing and reducing conditions. The oxidation state of these samples was investigated by X-ray photoelectron spectroscopy. The thermodynamic stability of uranium-substituted Gd2Zr2O7 is an important parameter that will govern the long-term storage of uranium and minor actinides in this matrix. High-temperature calorimetry has been used to investigate the stability of the Gd2-xUxZr2O7+δ (0.00 ≤ x ≤ 0.15) compositions. The standard molar free energy of the formation of Gd2-xUxZr2O7+δ (0.00 ≤ x ≤ 0.15) compositions has been estimated. From the free energy of formation data, the sample corresponding to x = 0.15 was found to be most stable in the Gd2-xUxZr2O7+δ (0.00 ≤ x ≤ 0.15) series. The relative stabilities of U(4+) and U(6+) substituted gadolinium zirconate have been discussed on the basis of the charge on the uranium ion and the incorporation of corresponding extra oxygen atoms into the lattice for charge compensation.

  19. Simulation on reactor TRIGA Puspati core kinetics fueled with thorium (Th) based fuel element

    SciTech Connect

    Mohammed, Abdul Aziz Rahman, Shaik Mohmmed Haikhal Abdul; Pauzi, Anas Muhamad Zin, Muhamad Rawi Muhammad; Jamro, Rafhayudi; Idris, Faridah Mohamad

    2016-01-22

    In confronting global energy requirement and the search for better technologies, there is a real case for widening the range of potential variations in the design of nuclear power plants. Smaller and simpler reactors are attractive, provided they can meet safety and security standards and non-proliferation issues. On fuel cycle aspect, thorium fuel cycles produce much less plutonium and other radioactive transuranic elements than uranium fuel cycles. Although not fissile itself, Th-232 will absorb slow neutrons to produce uranium-233 ({sup 233}U), which is fissile. By introducing Thorium, the numbers of highly enriched uranium fuel element can be reduced while maintaining the core neutronic performance. This paper describes the core kinetic of a small research reactor core like TRIGA fueled with a Th filled fuel element matrix using a general purpose Monte Carlo N-Particle (MCNP) code.

  20. Simulation on reactor TRIGA Puspati core kinetics fueled with thorium (Th) based fuel element

    NASA Astrophysics Data System (ADS)

    Mohammed, Abdul Aziz; Pauzi, Anas Muhamad; Rahman, Shaik Mohmmed Haikhal Abdul; Zin, Muhamad Rawi Muhammad; Jamro, Rafhayudi; Idris, Faridah Mohamad

    2016-01-01

    In confronting global energy requirement and the search for better technologies, there is a real case for widening the range of potential variations in the design of nuclear power plants. Smaller and simpler reactors are attractive, provided they can meet safety and security standards and non-proliferation issues. On fuel cycle aspect, thorium fuel cycles produce much less plutonium and other radioactive transuranic elements than uranium fuel cycles. Although not fissile itself, Th-232 will absorb slow neutrons to produce uranium-233 (233U), which is fissile. By introducing Thorium, the numbers of highly enriched uranium fuel element can be reduced while maintaining the core neutronic performance. This paper describes the core kinetic of a small research reactor core like TRIGA fueled with a Th filled fuel element matrix using a general purpose Monte Carlo N-Particle (MCNP) code.

  1. Microwave dissolution of plant tissue and the subsequent determination of trace lanthanide and actinide elements by inductively coupled plasma-mass spectrometry

    SciTech Connect

    Alvarado, J.S.; Neal, T.J.; Smith, L.L.; Erickson, M.D.

    1997-08-01

    Recently there has been much concern with the ability of plants to uptake heavy metals from their surroundings. With the development of instrumental techniques with low detection limits such as inductively coupled plasma-mass spectrometry (ICP-MS), attention is shifting toward achieving faster and more elegant ways of oxidizing the organic material inherent in environmental samples. Closed-vessel microwave dissolution was compared with conventional methods for the determination of concentrations of cerium, samarium, europium, terbium, uranium and thorium in a series of samples from the National Institute of Standards and Technology and from fields in Idaho. The ICP-MS technique exhibited detection limits in parts-per-trillion and linear calibration plots over three orders of magnitude for the elements under study. The results obtained by using nitric acid and hydrogen peroxide in a microwave digestion system for the analysis of reference materials showed close agreement with the accepted values. These values were compared with results obtained from dry- and wet-ashing procedures. The findings from an experiment comparing radiometric techniques for the determination of actinide elements to ICP-MS are reported.

  2. Actinide Oxidation State and O/M Ratio in Hypostoichiometric Uranium-Plutonium-Americium U0.750Pu0.246Am0.004O2-x Mixed Oxides.

    PubMed

    Vauchy, Romain; Belin, Renaud C; Robisson, Anne-Charlotte; Lebreton, Florent; Aufore, Laurence; Scheinost, Andreas C; Martin, Philippe M

    2016-03-07

    Innovative americium-bearing uranium-plutonium mixed oxides U1-yPuyO2-x are envisioned as nuclear fuel for sodium-cooled fast neutron reactors (SFRs). The oxygen-to-metal (O/M) ratio, directly related to the oxidation state of cations, affects many of the fuel properties. Thus, a thorough knowledge of its variation with the sintering conditions is essential. The aim of this work is to follow the oxidation state of uranium, plutonium, and americium, and so the O/M ratio, in U0.750Pu0.246Am0.004O2-x samples sintered for 4 h at 2023 K in various Ar + 5% H2 + z vpm H2O (z = ∼ 15, ∼ 90, and ∼ 200) gas mixtures. The O/M ratios were determined by gravimetry, XAS, and XRD and evidenced a partial oxidation of the samples at room temperature. Finally, by comparing XANES and EXAFS results to that of a previous study, we demonstrate that the presence of uranium does not influence the interactions between americium and plutonium and that the differences in the O/M ratio between the investigated conditions is controlled by the reduction of plutonium. We also discuss the role of the homogeneity of cation distribution, as determined by EPMA, on the mechanisms involved in the reduction process.

  3. Immobilization of actinides in stable mineral type and ceramic materials (high temperature synthesis)

    SciTech Connect

    Starkov, O.; Konovalov, E.

    1996-05-01

    Alternative vitrification technologies are being developed in the world for the immobilization of high radioactive waste in materials with improved thermodynamic stability, as well as improved chemical and thermal stability and stability to radiation. Oxides, synthesized in the form of analogs to rock-forming minerals and ceramics, are among those materials that have highly stable properties and are compatible with the environment. In choosing the appropriate material, we need to be guided by its geometric stability, the minimal number of cations in the structure of the material and the presence of structural elements in the mineral that are isomorphs of uranium and thorium, actinoids found in nature. Rare earth elements, yttrium, zirconium and calcium are therefore suitable. The minerals listed in the table (with the exception of the zircon) are pegatites by origin, i.e. they are formed towards the end of the magma crystallization of silicates form the residual melt, enriched with Ta, Nb, Ti, Zr, Ce, Y, U and Th. Uranium and thorium in the form of isomorphic admixtures form part of the lattice of the mineral. These minerals, which are rather simple in composition and structure and are formed under high temperatures, may be viewed as natural physio-chemical systems that are stable and long-lived in natural environments. The similarity of the properties of actinoids and lanthanoids plays an important role in the geochemistry of uranium and thorium; however, uranium (IV) is closer to the {open_quotes}heavy{close_quotes} group of lanthanoids (the yttrium group) while thorium (IV) is closer to the {open_quotes}light{close_quotes} group (the cerium group). That is why rare earth minerals contain uranium and thorium in the form of isomorphic admixtures.

  4. Uranium mineralization in southern Victoria Land, Antarctica

    SciTech Connect

    Dreschhoff, G.A.M.; Zeller, E.J.

    1986-01-01

    For the past 10 antarctic field seasons, an airborne gamma-ray spectrometric survey has been conducted over widely separated parts of the continent. Localized accumulations of both primary and secondary uranium minerals have been discovered at several localities scattered along the Transantarctic Mountains from the Scott Glacier to northern Victoria Land. A number of highly significant radiation anomalies have been discovered in the area between the Koettlitz Glacier and the Pyramid Trough. The occurrences consist of pegmatite vein complexes which contain an association of primary uranium and thorium minerals. Of still greater significance is the fact that abundant secondary uranium minerals were found in association with the primary deposits, and they indicate clearly that uranium is geochemically mobile under the conditions imposed by the arid polar climate that now exists in southern Victoria Land. Preliminary results of a uranium analysis performed by neutron activation indicate a concentration of 0.12% uranium in a composite sample from the two veins. Even higher levels of thorium are present. The nature of the primary uranium mineralization is currently under investigation. Preliminary results are discussed.

  5. 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.

  6. Redox response of actinide materials to highly ionizing radiation

    NASA Astrophysics Data System (ADS)

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

    2015-01-01

    Energetic radiation can cause dramatic changes in the physical and chemical properties of actinide materials, degrading their performance in fission-based energy systems. As advanced nuclear fuels and wasteforms are developed, fundamental understanding of the processes controlling radiation damage accumulation is necessary. Here we report oxidation state reduction of actinide and analogue elements caused by high-energy, heavy ion irradiation and demonstrate coupling of this redox behaviour with structural modifications. ThO2, in which thorium is stable only in a tetravalent state, exhibits damage accumulation processes distinct from those of multivalent cation compounds CeO2 (Ce3+ and Ce4+) and UO3 (U4+, U5+ and U6+). The radiation tolerance of these materials depends on the efficiency of this redox reaction, such that damage can be inhibited by altering grain size and cation valence variability. Thus, the redox behaviour of actinide materials is important for the design of nuclear fuels and the prediction of their performance.

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

    PubMed

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

    2015-01-27

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

  8. Principal thorium resources in the United States

    USGS Publications Warehouse

    Staatz, Mortimer Hay; Armbrustmacher, T.J.; Olson, J.C.; Brownfield, I.K.; Brock, M.R.; Lemons, J.F.; Coppa, L.V.; Clingan, B.V.

    1979-01-01

    Lemhi Pass and Wet Mountains Districts. The first district has reserves of 68,000 tons of ThO2 and probable potential resources of 124,000 tons that can be produced at less than $15 per pound; the second district has 54,000 tons of reserves and 141,000 tons of probable potential resources producible at less than $15 per pound. Rare earths are a common byproduct, and in many veins they are from one-half to several times as abundant as thorium. Massive carbonatite bodies are large-tonnage low-grade deposits. Thorium in these deposits would be a byproduct either of rare earth or of niobium mining. The Iron Hill carbonatite body in the Powderhorn district, Colorado, and the Sulfide Queen carbonatite body in the Mountain Pass district, California, were evaluated. These two deposits contain 40,800 tons of ThO2 in reserves and 125,000 tons of ThO2 in probable potential resources. More than 80 percent of this total is in the Iron Hill carbonatite. This thorium is entirely a byproduct and is producible at less than $15 per pound of ThO2. The Sulphide Queen massive carbonatite deposit was being mined in 1977 for rare earths, and thorium could be recovered by adding an extra circuit to the existing mill. Stream placers in North and South Carolina occur both in the Piedmont and just east of the Fall Line. The reserves of these deposits total 5,270 tons of ThO2, and the probable potential resources are 36,800 tons of ThO2. The Piedmont placers are all too small to produce ThO2 at a cost of less than $50 per pound. One placer on Hollow Creek, S.C., just east of the Fall Line had reserves of 2,040 tons of ThO2 that is producible at between $15 and $30 per pound. Thorium occurs in monazite in these placers. Other heavy minerals that would be recovered with the monazite include rutile, zircon, and ilmenite. In addition to thorium, monazite contains large amounts of rare earths and small amounts of uranium; both can be recovered during the process that separates thorium fr

  9. Closed fuel cycle with increased fuel burn-up and economy applying of thorium resources

    NASA Astrophysics Data System (ADS)

    Kulikov, G. G.; Apse, V. A.

    2017-01-01

    The possible role of existing thorium reserves in the Russian Federation on engaging thorium in being currently closed (U-Pu)-fuel cycle of nuclear power of the country is considered. The application efficiency of thermonuclear neutron sources with thorium blanket for the economical use of existing thorium reserves is demonstrated. The aim of the work is to find solutions of such major tasks as the reduction of both front-end and back-end of nuclear fuel cycle and an enhancing its protection against the uncontrolled proliferation of fissile materials by means of the smallest changes in the fuel cycle. During implementation of the work we analyzed the results obtained earlier by the authors, brought new information on the number of thorium available in the Russian Federation and made further assessments. On the basis of proposal on the inclusion of hybrid reactors with Th-blanket into the future nuclear power for the production of light uranium fraction 232+233+234U, and 231Pa, we obtained the following results: 1. The fuel cycle will shift from fissile 235U to 233U which is more attractive for thermal power reactors. 2. The light uranium fraction is the most "protected" in the uranium component of fuel and mixed with regenerated uranium will in addition become a low enriched uranium fuel, that will weaken the problem of uncontrolled proliferation of fissile materials. 3. 231Pa doping into the fuel stabilizes its multiplying properties that will allow us to implement long-term fuel residence time and eventually to increase the export potential of all nuclear power technologies. 4. The thorium reserves being near city Krasnoufimsk (Russia) are large enough for operation of large-scale nuclear power of the Russian Federation of 70 GWe capacity during more than a quarter century under assumption that thorium is loaded into blankets of hybrid TNS only. The general conclusion: the inclusion of a small number of hybrid reactors with Th-blanket into the future nuclear

  10. COORDINATION COMPOUND-SOLVENT EXTRACTION PROCESS FOR URANIUM RECOVERY

    DOEpatents

    Reas, W.H.

    1959-03-10

    A method is presented for the separation of uranium from aqueous solutions containing a uranyl salt and thorium. Thc separation is effected by adding to such solutions an organic complexing agent, and then contacting the solution with an organic solvent in which the organic complexing agent is soluble. By use of the proper complexing agent in the proper concentrations uranium will be complexed and subsequently removed in the organic solvent phase, while the thorium remains in the aqueous phase. Mentioned as suitable organic complexing agents are antipyrine, bromoantipyrine, and pyramidon.

  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. A Tetrapositive Metal Ion in the Gas Phase: Thorium(IV) Coordinated by Neutral Tridentate Ligands

    SciTech Connect

    Gong, Yu; Hu, Han-Shi; Tian, Guoxin; Rao, Linfeng; Li, Jun; Gibson, John K.

    2013-07-01

    ESI of 1:1 mixtures of Th(ClO₄)₄ and ligand TMOGA in acetonitrile resulted in the observation of the TMOGA supported tetracation, Th(L)₃⁴⁺, in the gas phase. Three TMOGA ligands are necessary to stabilize the tetrapositive thorium ion; no Th(L)₂⁴⁺ or Th(L)₄⁴⁺ was observed. Theoretical calculations reveal that the Th(L)₃⁴⁺ complex possesses C₃ symmetry with the thorium center coordinated by nine oxygen atoms from three ligands, which forms a twisted TPP geometry. Actinide compounds with such a geometry feature a nine-coordinate chiral actinide center. The Th-L binding energy and bond orders of Th(L)n⁴⁺ decrease as the coordination number increases, consistent with the trend of concurrently increasing Th-O distances. The Th-O bonding is mainly electrostatic in nature, but the covalent interactions are not negligible. CID of the Th(L)₃⁴⁺ complex mainly resulted in charge reduction to form Th(L)₂(L-86)³⁺oss of neutral TMOGA was not observed. The protic ligand methanol stabilized only tri- and dications of ligated thorium. The intensity of the Th(L)₃⁴⁺ peak was reduced as the percentage of water increased in the Th(ClO₄)₄/TMOGA solution.

  13. Stability of a new cubic monoxide of Thorium under pressure

    PubMed Central

    Sun, Weiwei; Luo, Wei; Ahuja, Rajeev

    2015-01-01

    Density functional theory has been applied to elucidate the stability of thorium monoxide (ThO). It is found out that the pressure can stabilize the rocksalt phase of ThO, and the transition pressure is estimated between 14 and 22 GPa. The stability of ThO can be attributed due to the gradually filling 5f orbitals at the expense of 7s and 6d electrons in Th metal. For ThO, the pressure induces stronger Th-O bond reflected by the newly established 6d-2p hybridization which is the dominant cause of its stability. The phonon dispersion curves of the rocksalt phase show the positive frequencies which indicates its dynamical stability. Our successful prediction of the stabilization of the metallic ThO has proposed a route to synthesize novel actinide monoxides. PMID:26337015

  14. 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.

  15. THE ATTRACTIVENESS OF MATERIAS ASSOCIATED WITH THORIUM-BASED NUCLEAR FUEL CYCLES FOR PHWRS

    SciTech Connect

    Prichard, Andrew W.; Niehus, Mark T.; Collins, Brian A.; Bathke, Charles G.; Ebbinghaus, Bartley B.; Hase, Kevin R.; Sleaford, Brad W.; Robel, Martin; Smith, Brian W.

    2011-07-17

    This paper reports the continued evaluation of the attractiveness of materials mixtures containing special nuclear materials (SNM) associated with thorium based nuclear fuel cycles. Specifically, this paper examines a thorium fuel cycle in which a pressurized heavy water reactor (PHWR) is fueled with mixtures of natural uranium/233U/thorium. This paper uses a PHWR fueled with natural uranium as a base fuel cycle, and then compares material attractiveness of fuel cycles that use 233U/thorium salted with natural uranium. The results include the material attractiveness of fuel at beginning of life (BoL), end of life (EoL), and the number of fuel assemblies required to collect a bare critical mass of plutonium or uranium. This study indicates what is required to render the uranium as having low utility for use in nuclear weapons; in addition, this study estimates the increased number of assemblies required to accumulate a bare critical mass of plutonium that has a higher utility for use in nuclear weapons. This approach identifies that some fuel cycles may be easier to implement the International Atomic Energy Agency (IAEA) safeguards approach and have a more effective safeguards by design outcome. For this study, approximately one year of fuel is required to be reprocessed to obtain one bare critical mass of plutonium. Nevertheless, the result of this paper suggests that all spent fuel needs to be rigorously safeguarded and provided with high levels of physical protection. This study was performed at the request of the United States Department of Energy /National Nuclear Security Administration (DOE/NNSA). The methodology and key findings will be presented.

  16. 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)

  17. National Uranium Resource Evaluation. Volume 1. Summary of the geology and uranium potential of Precambrian conglomerates in southeastern Wyoming

    SciTech Connect

    Karlstrom, K.E.; Houston, R.S.; Flurkey, A.J.; Coolidge, C.M.; Kratochvil, A.L.; Sever, C.K.

    1981-02-01

    A series of uranium-, thorium-, and gold-bearing conglomerates in Late Archean and Early Proterozoic metasedimentary rocks have been discovered in southern Wyoming. The mineral deposits were found by applying the time and strata bound model for the origin of uranium-bearing quartz-pebble conglomerates to favorable rock types within a geologic terrane known from prior regional mapping. No mineral deposits have been discovered that are of current (1981) economic interest, but preliminary resource estimates indicate that over 3418 tons of uranium and over 1996 tons of thorium are present in the Medicine Bow Mountains and that over 440 tons of uranium and 6350 tons of thorium are present in Sierra Madre. Sampling has been inadequate to determine gold resources. High grade uranium deposits have not been detected by work to date but local beds of uranium-bearing conglomerate contain as much as 1380 ppM uranium over a thickness of 0.65 meters. This project has involved geologic mapping at scales from 1/6000 to 1/50,000 detailed sampling, and the evaluation of 48 diamond drill holes, but the area is too large to fully establish the economic potential with the present information. This first volume summarizes the geologic setting and geologic and geochemical characteristics of the uranium-bearing conglomerates. Volume 2 contains supporting geochemical data, lithologic logs from 48 drill holes in Precambrian rocks, and drill site geologic maps and cross-sections from most of the holes. Volume 3 is a geostatistical resource estimate of uranium and thorium in quartz-pebble conglomerates.

  18. Mineral resource of the month: thorium

    USGS Publications Warehouse

    ,

    2009-01-01

    This article provides information on thorium. Thorium is a natural radioactive element that can be found with other minerals. It can be used to generate power, produce light and transmit energy. Thorium has a potential to be used as a nuclear fuel. This element was discovered by Swedish chemist and mineralogist Jóns Jakob Berzelius in 1828.

  19. 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.

  20. Radiotoxicity Characterization of Multi-Recycled Thorium Fuel - 12394

    SciTech Connect

    Franceschini, F.; Wenner, M.; Fiorina, C.; Huang, M.; Petrovic, B.; Krepel, J.

    2012-07-01

    As described in companion papers, Westinghouse is proposing the implementation of a thorium based fuel cycle to burn the transuranic (TRU) contained in the used nuclear fuel. The potential of thorium as a TRU burner is described in another paper presented at this conference. This paper analyzes the long-term impact of thorium on the front-end and backend of the fuel cycle. This is accomplished by an assessment of the isotopic make-up of Th in a closed cycle and its impact on representative metrics, such as radiotoxicity, decay heat and gamma heat. The behavior in both thermal and fast neutron energy ranges has been investigated. Irradiation in a Th fuel PWR has been assumed as representative of the thermal range, while a Th fuel fast reactor (FR) has been employed to characterize the behavior in the high-energy range. A comparison with a U-fuel closed-cycle FR has been undertaken in an attempt of a more comprehensive evaluation of each cycle's long-term potential. As the Th fuel undergoes multiple cycles of irradiation, the isotopic composition of the recycled fuel changes. Minor Th isotopes are produced; U-232 and Pa-231 build up; the U vector gradually shifts towards increasing amounts of U-234, U-235 etc., eventually leading to the production of non negligible amounts of TRU isotopes, especially Pu-238. The impact of the recycled fuel isotopic makeup on the in-core behavior is mild, and for some aspects beneficial, i.e. the reactivity swing during irradiation is reduced as the fertile characteristics of the fuel increase. On the other hand, the front and the back-end of the fuel cycle are negatively affected due to the presence of Th-228 and U-232 and the build-up of higher actinides (Pu-238 etc.). The presence of U-232 can also be seen as advantageous as it represents an obstacle to potential proliferators. Notwithstanding the increase in the short-term radiotoxicity and decay heat in the multi-recycled fuel, the Th closed cycle has some potentially substantial

  1. Conceptual design study of small long-life PWR based on thorium cycle fuel

    SciTech Connect

    Subkhi, M. Nurul; Su'ud, Zaki; Waris, Abdul; Permana, Sidik

    2014-09-30

    A neutronic performance of small long-life Pressurized Water Reactor (PWR) using thorium cycle based fuel has been investigated. Thorium cycle which has higher conversion ratio in thermal region compared to uranium cycle produce some significant of {sup 233}U during burn up time. The cell-burn up calculations were performed by PIJ SRAC code using nuclear data library based on JENDL 3.3, while the multi-energy-group diffusion calculations were optimized in whole core cylindrical two-dimension R-Z geometry by SRAC-CITATION. this study would be introduced thorium nitride fuel system which ZIRLO is the cladding material. The optimization of 350 MWt small long life PWR result small excess reactivity and reduced power peaking during its operation.

  2. Conceptual design study of small long-life PWR based on thorium cycle fuel

    NASA Astrophysics Data System (ADS)

    Subkhi, M. Nurul; Su'ud, Zaki; Waris, Abdul; Permana, Sidik

    2014-09-01

    A neutronic performance of small long-life Pressurized Water Reactor (PWR) using thorium cycle based fuel has been investigated. Thorium cycle which has higer conversion ratio in thermal region compared to uranium cycle produce some significant of 233U during burn up time. The cell-burn up calculations were performed by PIJ SRAC code using nuclear data library based on JENDL 3.3, while the multi-energy-group diffusion calculations were optimized in whole core cylindrical two-dimension R-Z geometry by SRAC-CITATION. this study would be introduced thorium nitride fuel system which ZIRLO is the cladding material. The optimization of 350 MWt small long life PWR result small excess reactivity and reduced power peaking during its operation.

  3. Thorium Chemistry in Oxo-Tellurium System under Extreme Conditions.

    PubMed

    Xiao, Bin; Kegler, Philip; Bosbach, Dirk; Alekseev, Evgeny V

    2017-03-06

    Through the use of a high-temperature/high-pressure synthesis method, four thorium oxo-tellurium compounds with different tellurium valence states were isolated. The novel inorganic phases illustrate the intrinsic complexity of the actinide tellurium chemistry under extreme conditions of pressure and temperature. Th2Te3O11 is the first instance of a mixed-valent oxo-tellurium compound, and at the same time, Te exhibits three different coordination environments (Te(IV)O3, Te(IV)O4, and Te(VI)O6) within a single structure. These three types of Te polyhedra are further fused together, resulting in a [Te3O11](8-) fragment. Na4Th2(Te(VI)3O15) and K2Th(Te(VI)O4)3 are the first alkaline thorium tellurates described in the literature. Both compounds are constructed from ThO9 tricapped trigonal prisms and Te(VI)O6 octahedra. Na4Th2(Te(VI)3O15) is a three-dimensional framework based on Th2O15 and Te2O10 dimers, while K2Th(Te(VI)O4)3 contains tungsten oxide bronze like Te layers linked by ThO9 polyhedra. The structure of β-Th(Te(IV)O3)(SO4) is built from infinite thorium chains cross-linked by Te(IV)O3(2-) and SO4(2-) anions. Close structural analysis suggests that β-Th(Te(IV)O3)(SO4) is highly related to the structure of α-Th(SeO4)2. Additionally, the Raman spectra are recorded and the characteristic peaks are assigned based on a comparison of reported tellurites or tellurates.

  4. Fast Thorium Molten Salt Reactors Started with Plutonium

    SciTech Connect

    Merle-Lucotte, E.; Heuer, D.; Le Brun, C.; Brissot, R.; Liatard, E.; Meplan, O.; Nuttin, A.

    2006-07-01

    One of the pending questions concerning Molten Salt Reactors based on the {sup 232}Th/{sup 233}U fuel cycle is the supply of the fissile matter, and as a consequence the deployment possibilities of a fleet of Molten Salt Reactors, since {sup 233}U does not exist on earth and is not yet produced in the current operating reactors. A solution may consist in producing {sup 233}U in special devices containing Thorium, in Pressurized Water or Fast Neutrons Reactors. Two alternatives to produce {sup 233}U are examined here: directly in standard Molten Salt Reactors started with Plutonium as fissile matter and then operated in the Th/{sup 233}U cycle; or in dedicated Molten Salt Reactors started and fed with Plutonium as fissile matter and Thorium as fertile matter. The idea is to design a critical reactor able to burn the Plutonium and the minor actinides presently produced in PWRs, and consequently to convert this Plutonium into {sup 233}U. A particular reactor configuration is used, called 'unique channel' configuration in which there is no moderator in the core, leading to a quasi fast neutron spectrum, allowing Plutonium to be used as fissile matter. The conversion capacities of such Molten Salt Reactors are excellent. For Molten Salt Reactors only started with Plutonium, the assets of the Thorium fuel cycle turn out to be quickly recovered and the reactor's characteristics turn out to be equivalent to Molten Salt Reactors operated with {sup 233}U only. Using a combination of Molten Salt Reactors started or operated with Plutonium and of Molten Salt Reactors started with {sup 233}U, the deployment capabilities of these reactors fully satisfy the condition of sustainability. (authors)

  5. Malleability of uranium: Manipulating the charge-density wave in epitaxial films

    NASA Astrophysics Data System (ADS)

    Springell, R.; Ward, R. C. C.; Bouchet, J.; Chivall, J.; Wermeille, D.; Normile, P. S.; Langridge, S.; Zochowski, S. W.; Lander, G. H.

    2014-06-01

    We report x-ray synchrotron experiments on epitaxial films of uranium, deposited on niobium and tungsten seed layers. Despite similar lattice parameters for these refractory metals, the uranium epitaxial arrangements are different and the strains propagated along the orthorhombic a axis of the uranium layers are of opposite sign. At low temperatures these changes in epitaxy result in dramatic modifications to the behavior of the charge-density wave in uranium. The differences are explained with the current theory for the electron-phonon coupling in the uranium lattice. Our results emphasize the intriguing possibilities of producing epitaxial films of elements that have complex structures like the light actinides uranium to plutonium.

  6. Uranium assessment for the Precambrian pebble conglomerates in southeastern Wyoming

    SciTech Connect

    Borgman, L.E.; Sever, C.; Quimby, W.F.; Andrew, M.E.; Karlstrom, K.E.; Houston, R.S.

    1981-03-01

    This volume is a geostatistical resource estimate of uranium and thorium in quartz-pebble conglomerates, and is a companion to Volume 1: The Geology and Uranium Potential to Precambrian Conglomerates in the Medicine Bow Mountains and Sierra Madre of Southeastern Wyoming; and to Volume 2: Drill-Hole Data, Drill-Site Geology, and Geochemical Data from the Study of Precambrian Uraniferous Conglomerates of the Medicine Bow Mountains and the Sierra Madre of Southeastern Wyoming.

  7. 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.

  8. 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.

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

    SciTech Connect

    Wilkerson, Marianne Perry

    2010-01-01

    We are interested in applying our understanding of actinide chemical structure and bonding to broaden the suite of analytical tools available for nuclear forensic analyses. Uranium- and plutonium-oxide systems form under a variety of conditions, and these chemical species exhibit some of the most complex behavior of metal oxide systems known. No less intriguing is the ability of AnO{sub 2} (An: U, Pu) to form non-stoichiometric species described as AnO{sub 2+x}. Environmental studies have shown the value of utilizing the chemical signatures of these actinide oxide materials to understand transport following release into the environment. Chemical speciation of actinide-oxide samples may also provide clues as to the age, source, or process history of the material. The scientific challenge is to identify, measure and understand those aspects of speciation of actinide analytes that carry information about material origin and history most relevant to forensics. Here, we will describe our efforts in material synthesis and analytical methods development that we will use to provide the fundamental science to characterize actinide oxide molecular structures for forensic science. Structural properties and initial results to measure structural variability of uranium oxide samples using synchrotron-based X-ray Absorption Fine Structure will be discussed.

  10. SHEATHING URANIUM

    DOEpatents

    Colbeck, E.W.

    1959-02-01

    A method is deseribed for forming a conveniently handled corrosion resistant U articlc comprising pouring molten U into an open-ended corrosion resistant metal eontainer such as Cu and its alloys, Al, or austenitic Ni stainless steel. The exposed surface of the cast U is covered with a metallic packing material such as a brazing flux consisting of Al-Si alloy. The container is sealed iii contact with substantially the entire exposed surface of the packing material. The article is then worked mechanically to reduce the cross section. l3651 A thorium--carbon alloy containing 0.1 to 0.5% by weight carbon, whieh is more resistant to water corrosion than pure thorium metal is presented. The alloy is prepared by fusing thorium metal with the desired amount of carbon at a temperature of about 1850 C. It is found that the carbon is present in the alloy as thorium monocarbide

  11. Phosphonate-functionalized large pore 3-D cubic mesoporous (KIT-6) hybrid as highly efficient actinide extracting agent.

    PubMed

    Lebed, Pablo J; de Souza, Kellen; Bilodeau, François; Larivière, Dominic; Kleitz, Freddy

    2011-11-07

    A new type of radionuclide extraction material is reported based on phosphonate functionalities covalently anchored on the mesopore surface of 3-D cubic mesoporous silica (KIT-6). The easily prepared nanoporous hybrid shows largely superior performance in selective sorption of uranium and thorium as compared to the U/TEVA commercial resin and 2-D hexagonal SBA-15 equivalent.

  12. Spectrophotometric study of the thorium-morin mixed-color system

    USGS Publications Warehouse

    Fletcher, M.H.; Milkey, R.G.

    1956-01-01

    A spectrophotometric study was made of the thoriummorin reaction to evaluate the suitability of morin as a reagent for the determination of trace amounts of thorium. At pH 2, the equilibrium constant for the reaction is 1 ?? 106, and a single complex having a thorium-morin ratio of 1 to 2 is formed. The complex shows maximum absorbance at a wave length of 410 m??, and its absorbance obeys Beer's law. The absorbance readings are highly reproducible, and the sensitivity is relatively high, an absorbance difference of 0.001 being equivalent to 0.007 ?? of ThO2 per sq. cm. The effects of acid, alcohol, and morin concentration, time, temperature, and age of the morin reagent as well as the behavior of morin with zirconium(IV), iron(III), aluminum(III), ytterbium(III), yttrium(III), uranium(VI), praseodymium(III), lead(II), lanthanum(III), and calcium(II) ions are discussed. A method is presented for the determination of thorium in pure solutions. Appropriate separations for the isolation of thorium may extend the usefulness of the method and permit the determination of trace amounts of thorium in complex materials.

  13. Thorium in occupationally exposed men.

    SciTech Connect

    Stehney, A. F.

    1999-02-24

    Higher than environmental levels of {sup 232}Th have been found in autopsy samples of lungs and other organs from four former employees of a thorium refinery. Working periods of the subjects ranged from 3 to 24 years, and times from end of work to death ranged from 6 to 31 years. Examination of the distribution of thorium among the organs revealed poor agreement with the distribution calculated from the dosimetric models in Publication 30 of the International Commission on Radioprotection (ICRP). Concentrations in the lungs relative to pulmonary lymph nodes, bone or liver were much higher than calculated from the model for class Y thorium and the exposure histories of the workers. Much better agreement was found with more recently proposed models in Publications 68 and 69 of the ICRP. Radiation doses estimated from the amounts of thorium in the autopsy samples were compatible with health studies that found no significant difference in mortality from that of the general population of men in the US.

  14. Activation energetics of actinide diffusion in UO2 from first-principles calculations

    NASA Astrophysics Data System (ADS)

    Wang, Jianwei; Becker, Udo

    2013-02-01

    Diffusion of actinides in uranium dioxide plays an important role in determining thermodynamic and mechanic properties of the material. Activation energies of Th, U, Np, and Pu diffusion in uranium dioxide were systematically studied using first-principles calculations. The generalized gradient approximation and projector-augmented wave methods with on-site Coulomb repulsive interaction were applied within Density Functional Theory and Plane Wave framework. Two diffusion paths, one along the lattice <1 1 0> direction and the other along the lattice <1 0 0> direction, were examined in the face-centered cubic UO2 structure. The results show that the <1 1 0> path has lower migration energy than the <1 0 0> path. Under the assumption of a vacancy-assisted jump diffusion mechanism, the major contribution to the activation energy is the migration energy, followed by the vacancy formation energy and vacancy binding energy, where the last has the lowest contribution. However, differences in the activation energies among different actinides stem from both the migration and vacancy binding energies, both of which decrease with atomic number. While discrepancies between the absolute values of the calculated and experimentally observed activation energies remain, this study shows a correlation between activation energy and atomic number and an asymptotic relation between activation energy and ionic radius of the actinides. The present study suggests that the migration of the actinides through the uranium dioxide lattice is closely correlated to the number of 5f electrons and the size of the diffusing atoms.

  15. Actinides recovery from molten salt/liquid metal system by electrochemical methods

    NASA Astrophysics Data System (ADS)

    Iizuka, Masatoshi; Koyama, Tadafumi; Kondo, Naruhito; Fujita, Reiko; Tanaka, Hiroshi

    1997-08-01

    Electrochemical methods were examined for the recovery of actinides from the electrorefiner which is used in pyrometallurgical reprocessing of spent metal fuel for fast reactors. Uranium was successfully collected at the solid steel cathode from both liquid cadmium and molten salt solvents. In electrotransport from liquid cadmium, the behavior of uranium and rare earths was as expected by a computer simulation code based on the diffusion layer model at the interface between the electrolyte and the electrodes. In electroreduction from the molten salt electrolyte, a considerable amount of uranium was reduced at the CdLi anode by direct chemical reduction with lithium, especially at a lower anodic current density. The decrease in collection efficiency of uranium due to the direct chemical reduction would be avoided by maintaining the anode potential higher than the deposition potential of uranium.

  16. Matrix Infrared Spectroscopic and Computational Investigations of Novel Small Uranium Containing Molecules - Final Technical Report

    SciTech Connect

    Andrews, Lester

    2014-10-17

    Direct reactions of f-element uranium, thorium and lanthanide metal atoms were investigated with small molecules. These metal atoms were generated by laser ablation and mixed with the reagent molecules then condensed with noble gases at 4K. The products were analyzed by absorption of infrared light to measure vibrational frequencies which were confirmed by quantum chemical calculations. We have learned more about the reactivity of uranium atoms with common molecules, which will aid in the develolpment of further applications of uranium.

  17. 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)

  18. 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.

  19. Thorium: Issues and prospects in Malaysia

    SciTech Connect

    AL-Areqi, Wadeeah M.; Majid, Amran Ab.; Sarmani, Sukiman; Bahri, Che Nor Aniza Che Zainul

    2015-04-29

    In Malaysia, thorium exists in minerals and rare earth elements production residue. The average range of thorium content in Malaysian monazite and xenotime minerals was found about 70,000 and 15,000 ppm respectively. About 2,636 tonnes of Malaysian monazite was produced for a period of 5 years (2006-2010) and based on the above data, it can be estimated that Malaysian monazite contains about 184.5 tonnes of thorium. Although thorium can become a major radiological problem to our environment, but with the significant deposit of thorium in Malaysian monazite, it has a prospect as a future alternative fuel in nuclear technology. This paper will discuss the thorium issues in Malaysia especially its long term radiological risks to public health and environment at storage and disposal stages, the prospect of exploring and producing high purity thorium from our rare earth elements minerals for future thorium based reactor. This paper also highlights the holistic approach in thorium recovery from Malaysian rare earth element production residue to reduce its radioactivity and extraction of thorium and rare earth elements from the minerals with minimum radiological impact to health and environment.

  20. 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.

  1. 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.

  2. Selective chelation and extraction of lanthanides and actinides with supercritical fluids

    SciTech Connect

    Brauer, R.D.; Carleson, T.E.; Harrington, J.D.; Jean, F.; Jiang, H.; Lin, Y.; Wai, C.M.

    1994-01-01

    This report is made up of three independent papers: (1) Supercritical Fluid Extraction of Thorium and Uranium with Fluorinated Beta-Diketones and Tributyl Phosphate, (2) Supercritical Fluid Extraction of Lanthanides with Beta-Diketones and Mixed Ligands, and (3) A Group Contribution Method for Predicting the Solubility of Solid Organic Compounds in Supercritical Carbon Dioxide. Experimental data are presented demonstrating the successful extraction of thorium and uranium using fluorinated beta-diketones to form stable complexes that are extracted with supercritical carbon dioxide. The conditions for extracting the lanthanide ions from liquid and solid materials using supercritical carbon dioxide are presented. In addition, the Peng-Robison equation of state and thermodynamic equilibrium are used to predict the solubilities of organic solids in supercritical carbon dioxide from the sublimation pressure, critical properties, and a centric factor of the solid of interest.

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

    SciTech Connect

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

    2006-02-02

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

  4. 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.

  5. Quantum Mechanical Studies of the Early Actinide Compounds

    NASA Astrophysics Data System (ADS)

    Obodo, Kingsley Onyebuchi

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

  6. URANIUM RECOVERY

    DOEpatents

    Fitch, F.T.; Cruikshank, A.J.

    1958-10-28

    A process for recovering uranium from a solution of a diethyl dithiocarbaruate of uranium in an orgakic solvent substantially immiscible with water is presented. The process comprises brlnging the organic solutlon into intimate contact wlth an aqueous solution of ammonium carbonate, whereby the uranium passes to the aqueous carbonate solution as a soluble uranyl carbonate.

  7. Thorium: Determination by CDTN, Brazil

    NASA Astrophysics Data System (ADS)

    Menezes, M. A. B. C.; Sabino, C. V. S.

    1999-01-01

    One of the tasks of the Radiochemical Sector, CDTN/CNEN, Brazil, is to meet the clients' analytical needs. The Sector has been facing the challenges of determining several elements in diversified matrixes from all over the country since the sixties. It has been giving analytical support to universities, industries, environmental monitoring programs, research institutes. Due to the growing need to determine thorium isotopes through the years it was necessary to work out a routine procedures. Nowadays the determination of thorium consists of a well established routine whose procedures are applied to grouped samples according to their kind, physical state, matrix interference, detection limits and number of samples. This paper describes the methods used by CDTN to determine232Th by neutron activation analysis and230Th and228Th by radiochemical separations and alpha spectrometry in several matrixes.

  8. Hydration and hydrolysis of thorium(IV) in aqueous solution and the structures of two crystalline thorium(IV) hydrates.

    PubMed

    Torapava, Natallia; Persson, Ingmar; Eriksson, Lars; Lundberg, Daniel

    2009-12-21

    Solid octaaqua(kappa(2)O-perchlorato)thorium(IV) perchlorate hydrate, [Th(H(2)O)(8)(ClO(4))](ClO(4))(3).H(2)O, 1, and aquaoxonium hexaaquatris(kappaO-trifluoromethanesulfonato)thorium(IV) trisaquahexakis(kappaO-trifluoromethanesulfonato)thorinate(IV), H(5)O(2)[Th(H(2)O)(6)(OSO(2)CF(3))(3)][Th(H(2)O)(3)(OSO(2)CF(3))(6)], 2, were crystallized from concentrated perchloric and trifluoromethanesulfonic acid solutions, respectively. 1 adopts a severely distorted tricapped trigonal prismatic configuration with an additional oxygen from the perchlorate ion at a longer distance. 2 consists of individual hexaaquatris(kappaO-trifluoromethanesulfonato)thorium(IV) and trisaquahexakis(kappaO-trifluoromethanesulfonato)thorinate(IV) ions and an aquaoxonium ion bridging these two ions through hydrogen bonding. The hydrated thorium(IV) ion is nine-coordinated in aqueous solution as determined by extended X-ray absorption fine structure (EXAFS) and large angle X-ray scattering (LAXS). The LAXS studies also showed a second hydration sphere of about 18 water molecules, and traces of a 3rd hydration sphere. Structural studies in aqueous solution of the hydrolysis products of thorium(IV) have identified three different types of hydrolysis species: a mu(2)O-hydroxo dimer, [Th(2)(OH)(2)(H(2)O)(12)](6+), a mu(2)O-hydroxo tetramer, [Th(4)(OH)(8)(H(2)O)(16)](8+), and a mu(3)O-oxo hexamer, [Th(6)O(8)(H(2)O)(n)](8+). Detailed structures of these three hydrolysis species are given. A compilation of reported solid state structures of actinoid(IV) compounds with oxygen donor ligands show a strong correlation between the An-O bond distance and the coordination number. The earlier reported U-O bond distance in the hydrated uranium(IV) ion in aqueous solution, confirmed in this study, is related to nine-coordination. The hydrated tri- and tetravalent actinoid ions in aqueous solution all seem to be nine-coordinated. The trivalent ions show a significant difference in bond distance to prismatic and

  9. Thorium isotopes in colloidal fraction of water from San Marcos Dam, Chihuahua, Mexico

    NASA Astrophysics Data System (ADS)

    Cabral-Lares, M.; Melgoza, A.; Montero-Cabrera, M. E.; Renteria-Villalobos, M.

    2013-07-01

    The main interest of this stiidy is to assess the contents and distribution of Th-series isotopes in colloidal fraction of surface water from San Marcos dam, because the suspended particulate matter serves as transport medium for several pollutants. The aim of this work was to assess the distribution of thorium isotopes (232Th and 230Th) contained in suspended matter. Samples were taken from three surface points along the San Marcos dam: water input, midpoint, and near to dam wall. In this last point, a depth sampling was also carried out. Here, three depth points were taken at 0.4, 8 and 15 meters. To evaluate the thorium behavior in surface water, from every water sample the colloidal fraction was separated, between 1 and 0.1 μm. Thorium isotopes concentraron in samples were obtained by alpha spectrometry. Activity concentrations obtained of 232Th and 230Th in surface points ranged from 0.3 to 0.5 Bq ṡ L-1, whereas in depth points ranged from 0.4 to 3.2 Bq ṡ L-1, respectively. The results show that 230Th is in higher concentration than 232Th in colloidal fraction. This can be attributed to a preference of these colloids to adsorb uranium. Thus, the activity ratio 230Th/232Th in colloidal fraction showed values from 2.3 to 10.2. In surface points along the dam, 230Th activity concentration decreases while 232Th concentration remains constant. On the other hand, activity concentrations of both isotopes showed a pointed out enhancement with depth. The results have shown a possible lixiviation of uranium from geological substrate into the surface water and an important fractionation of thorium isotopes, which suggest that thorium is non-homogeneously distributed along San Marcos dam.

  10. Depletion Analysis of Modular High Temperature Gas-cooled Reactor Loaded with LEU/Thorium Fuel

    SciTech Connect

    Sonat Sen; Gilles Youinou

    2013-02-01

    Thorium based fuel has been considered as an option to uranium-based fuel, based on considerations of resource utilization (Thorium is more widely available when compared to Uranium). The fertile isotope of Thorium (Th-232) can be converted to fissile isotope U-233 by neutron capture during the operation of a suitable nuclear reactor such as High Temperature Gas-cooled Reactor (HTGR). However, the fertile Thorium needs a fissile supporter to start and maintain the conversion process such as U-235 or Pu-239. This report presents the results of a study that analyzed the thorium utilization in a prismatic HTGR, namely Modular High Temperature Gas-Cooled Reactor (MHTGR) that was designed by General Atomics (GA). The collected for the modeling of this design come from Chapter 4 of MHTGR Preliminary Safety Information Document that GA sent to Department of Energy (DOE) on 1995. Both full core and unit cell models were used to perform this analysis using SCALE 6.1 and Serpent 1.1.18. Because of the long mean free paths (and migration lengths) of neutrons in HTRs, using a unit cell to represent a whole core can be non-trivial. The sizes of these cells were set to match the spectral index between unit cell and full core domains. It was found that for the purposes of this study an adjusted unit cell model is adequate. Discharge isotopics and one-group cross-sections were delivered to the transmutation analysis team. This report provides documentation for these calculations

  11. 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.

  12. Computational Modeling of Actinide Ions in Aqueous Solution

    NASA Astrophysics Data System (ADS)

    Atta-Fynn, Raymond

    2014-03-01

    Unraveling the chemical behavior of actinide species is difficult owing to the complex electronic structure of these species, the fact that many of these species can occur in multiple oxidation states, and the difficulties encountered in their experimental studies. First principles dynamical modeling, although computationally costly, allows us to gain rich insights into the behavior of actinide species. In this talk, we present results of the hydration shell structure and x-ray absorption spectra of aqueous actinides in different oxidation states including U(VI), U(V), U(IV), and Cm(III) using relativistic ab initiomolecular dynamics at 300 K. We also probed the thermodynamics of hydrolysis by calculating the first acidity constant for uranium in all three oxidation states (IV, V, and VI). We predicted, for the first time, that UO2+ is a weak acid in solution with a pKa value of 8.5. This result is particularly important since no thermodynamic data are available for hydrolyzed species of U(V). In our most recent work on concentrated Cm(III) solutions, we showed that counter-ions can strengthen or weaken the solvent structure itself rather than just the water coordination number. These new results are better explained in terms of the hydrogen bond lifetimes of the solvents.

  13. Electrostatic Radionuclide Separation: A New Version of Rutherford's "Thorium Cow".

    ERIC Educational Resources Information Center

    Eiswirth, Marcus; And Others

    1982-01-01

    Describes three experiments (also useful as demonstrations) using a "thorium cow," a device which concentrates the daughter products from thorium compounds by precipitation on a charged electrode. (JN)

  14. 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.

  15. 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.

  16. Application of diode lasers to the isotopically selective determination of uranium in oxides by optogalvanic spectroscopy

    SciTech Connect

    Young, J.P.; Barshick, C.M.; Shaw, R.W.; Ramsey, J.M.

    1994-09-01

    We have observed isotopically selective diode laser-excited optogalvanic effects in uranium at 778.42 and 776.19 nm. The samples were natural abundance uranium oxide, as well as depleted (0.3% {sup 235}U), natural (0.7% {sup 235}U) and enriched (9.75% {sup 235}U) uranium metal or powders. The measurements were carried out in a demountable-cathode glow discharge cell. Preliminary evaluations of precision for uranium isotopic ratios measured using this technique suggest that it should have broad analytical applications for uranium and other amenable actinides or lanthanides.

  17. United States Transuranium and Uranium Registries

    SciTech Connect

    Kathren, R.

    1993-02-28

    The United States Transuranium and Uranium Registries are unique human tissue research programs studying the distribution, dose, and possible biological effects of the actinide elements in man, with the primary goal of assuring the adequacy of radiation protection standards for these radionuclides. The Registries research is based on radiochemical analysis of tissues collected at autopsy from voluntary donors who have documented occupational exposure to the actinides. To date, tissues, or in some cases radioanalytical results only, have been obtained from approximately 300 individuals; another 464 living individuals have volunteered to participate in the Registries research programs and have signed premortem informed consent and autopsy permissions. The Registries originated at the National Plutonium Registry which was started in 1968 as a then Atomic Energy Commission project under the aegis of a prime contractor at the Hanford site. In 1970, the name was changed to the United States Transuranium Registry to reflect a broader involvement with the higher actinides. In 1978, an administratively separate parallel registry, the United States Uranium Registry, was formed to carry out similar studies among uranium fuel cycle workers.

  18. On the valence fluctuation in the early actinide metals

    SciTech Connect

    Soderlind, P.; Landa, A.; Tobin, J. G.; Allen, P.; Medling, S.; Booth, C. H.; Bauer, E. D.; Cooley, J. C.; Sokaras, D.; Weng, T. -C.; Nordlund, D.

    2015-12-15

    In this study, recent X-ray measurements suggest a degree of valence fluctuation in plutonium and uranium intermetallics. We are applying a novel scheme, in conjunction with density functional theory, to predict 5f configuration fractions of states with valence fluctuations for the early actinide metals. For this purpose we perform constrained integer f-occupation calculations for the α phases of uranium, neptunium, and plutonium metals. For plutonium we also investigate the δ phase. The model predicts uranium and neptunium to be dominated by the f3 and f4 configurations, respectively, with only minor contributions from other configurations. For plutonium (both α and δ phase) the scenario is dramatically different. Here, the calculations predict a relatively even distribution between three valence configurations. The δ phase has a greater configuration fraction of f6 compared to that of the α phase. The theory is consistent with the interpretations of modern X-ray experiments and we present resonant X-ray emission spectroscopy results for α-uranium.

  19. On the valence fluctuation in the early actinide metals

    DOE PAGES

    Soderlind, P.; Landa, A.; Tobin, J. G.; ...

    2015-12-15

    In this study, recent X-ray measurements suggest a degree of valence fluctuation in plutonium and uranium intermetallics. We are applying a novel scheme, in conjunction with density functional theory, to predict 5f configuration fractions of states with valence fluctuations for the early actinide metals. For this purpose we perform constrained integer f-occupation calculations for the α phases of uranium, neptunium, and plutonium metals. For plutonium we also investigate the δ phase. The model predicts uranium and neptunium to be dominated by the f3 and f4 configurations, respectively, with only minor contributions from other configurations. For plutonium (both α and δmore » phase) the scenario is dramatically different. Here, the calculations predict a relatively even distribution between three valence configurations. The δ phase has a greater configuration fraction of f6 compared to that of the α phase. The theory is consistent with the interpretations of modern X-ray experiments and we present resonant X-ray emission spectroscopy results for α-uranium.« less

  20. A glossary of uranium- and thorium-bearing minerals

    USGS Publications Warehouse

    Frondel, Judith Weiss; Fleischer, Michael

    1950-01-01

    During 1980, an estimated 121 million gallons of water per day was pumped in a 26-county area in east-central Georgia from sand aquifers of Paleocene and Late Cretaceous age. Maximum withdrawals were at the kaolin mining and processing centers in Twiggs, Wilkinson, and Washington Counties, where water levels have declined as much as 50 ft since 1944-50. In the southern two-thirds of the study area, water levels have shown little, if any, change. Declining water levels and increasing competition for groundwater have caused concern over the adequacy of groundwater supplies. This report defines the areal extent and describes the geohydrology of the Paleocene-Upper Cretaceous aquifers of east-central Georgia, and evaluates the effects of man on the groundwater flow system. Geohydrologic data from four test wells indicate that the aquifers consist of alternating layers of sand and clay that are largely of deltaic origin. In the northern third of the study area, the confining unit between the Dublin and Midville aquifer systems is absent and the aquifer systems combine to form the Dublin-Midville aquifer system. The aquifer systems range in thickness from 80 to 645 ft and their transmissivities range from 800 to 39,000 sq ft/day. The hydraulic conductivity ranges from 15 to 530 ft/day. Wells yield as much as 3,400 gpm (gallons per minute). Chemical analyses of water from 49 wells indicate that water from both aquifer systems is of good quality except in the central part of the study area, where iron concentrations are as high as 6,700 micrograms/L and exceed the 300 micrograms/L recommended limit for drinking water. The principal recharge to the aquifer systems is from precipitation that occurs within and adjacent to the outcrop areas. The principal discharge is to streams in the outcrop area. (Author 's abstract)