WorldWideScience

Sample records for 237np 231pa ionizatsionnykh

  1. Criticality of a {sup 237}Np Sphere

    Energy Technology Data Exchange (ETDEWEB)

    Sanchez, Rene G.; Hayes, David K.; Cappiello, Charlene C.; Myers, William L.; Jaegers, Peter J.; Clement, Steven D.

    2003-07-22

    A critical mass experiment using a 6-kg {sup 237}Np sphere has been performed. The purpose of the experiment is to get a better estimate of the critical mass of {sup 237}Np. To attain criticality, the {sup 237}Np sphere was surrounded with 93 wt % {sup 235}U shells. A 1/M as a function of uranium mass was performed. An MCNP neutron transport code was used to model the experiment. The MCNP code yielded a k{sub eff} of 0.99089 {+-} 0.0003 compared with a k{sub eff} 1.0026 for the experiment. Based on these results, it is estimated that the critical mass of {sup 237}Np ranges from kilogram weights in the high fifties to low sixties.

  2. Measurements of {sup 237}Np secondary neutron spectra

    Energy Technology Data Exchange (ETDEWEB)

    Kornilov, N.V.

    1997-03-01

    The activities carried out during the first year of the project are summarized. The main problems for Np spectra measurements arise from high intrinsic gamma-ray activity of the sample and admixture of the oxygen and iron nuclei. The inelastically scattered neutrons and the fission neutrons spectra for {sup 237}Np were measured by time-of-flight spectrometer of the IPPE at incident neutron energies {approx_equal}1.5 MeV, and {approx_equal}0.5 MeV. A solid tritium target and a Li-metallic target were used as neutron sources. The neutron scattering on C sample (C(n,n) standard reaction) was measured to normalize the Np data. The experimental data should be simulated by Monte Carlo method to correct the experimental data for oxygen and iron admixture as well as for multiple scattering of the neutrons in the sample. Therefore the response function of the spectrometer, and the neutron energy distribution from the source were investigated in detail. (author)

  3. Measurements of {sup 237}Np secondary neutron spectra

    Energy Technology Data Exchange (ETDEWEB)

    Kornilov, N.V.

    1997-03-01

    The activities carried out during the first year of the project are summarized. The main problems for Np spectra measurements arise from high intrinsic gamma-ray activity of the sample and admixture of the oxygen and iron nuclei. The inelastically scattered neutrons and the fission neutrons spectra for {sup 237}Np were measured by time-of-flight spectrometer of the IPPE at incident neutron energies {approx_equal}1.5 MeV, and {approx_equal}0.5 MeV. A solid tritium target and a Li-metallic target were used as neutron sources. The neutron scattering on C sample (C(n,n) standard reaction) was measured to normalize the Np data. The experimental data should be simulated by Monte Carlo method to correct the experimental data for oxygen and iron admixture as well as for multiple scattering of the neutrons in the sample. Therefore the response function of the spectrometer, and the neutron energy distribution from the source were investigated in detail. (author)

  4. 231Pa systematics in postglacial volcanic rocks from Iceland

    Science.gov (United States)

    Turner, Simon; Kokfelt, Thomas; Hoernle, Kaj; Lundstrom, Craig; Hauff, Folkmar

    2016-07-01

    Several recent studies have highlighted the potential of combined 238U-230Th and 235U-231Pa systematics to constrain upwelling rates and the role of recycled mafic lithologies in mantle plume-derived basalts. Accordingly, we present measurements of the 231Pa concentrations from 26 mafic volcanic rocks from Iceland, including off-axis basalts from the Snaefellsnes Peninsula, to complement previously published 238U-230Th-226Ra data. 231Pa concentrations vary from 27 to 624 fg/g and (231Pa/235U) ratios from 1.12 to 2.11 with the exception of one anomalous sample from the Southeast Rift which has a 231Pa deficit with (231Pa/235U) = 0.86. An important new result is that basalts from the Southeast Rift and the Snaefellsnes Peninsula define a trend at relatively low (231Pa/235U) for a given (230Th/238U) ratio. Many of the remaining samples fall in or around the global field for ocean island basalts but those from the Mid-Iceland Belt and the Southwest Rift/Reykjanes Peninsula extend to higher (231Pa/235U) ratios at a given (230Th/238U), similar to mid-ocean ridge basalts. In principle, these lavas could result from melting of peridotite at lower pressures. However, there is no reason to suspect that the Mid-Iceland Belt and the Southwest Rift lavas reflect shallower melting than elsewhere in Iceland. In our preferred model, these lavas reflect melting of garnet peridotite whereas those from the Southeast Rift and the Snaefellsnes Peninsula contain a significant contribution (up to 20%) of melt from garnet pyroxenite. This is consistent with incompatible trace element and radiogenic isotope evidence for recycled oceanic crust in these lavas. There is increasing agreement that the displacement of ocean island basalts to lower (231Pa/235U) ratios at a given (230Th/238U), compared to mid-ocean ridge basalts, reflects the role of recycled mafic lithologies such as garnet pyroxenite as well as higher average pressures of melting. It now seems likely that this interpretation may

  5. 237 Np analytical method using 239 Np tracers and application to a contaminated nuclear disposal facility

    Energy Technology Data Exchange (ETDEWEB)

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

    2017-06-01

    Environmental 237Np analyses are challenged by low 237Np concentrations and lack of an available yield tracer; we report a rapid, inexpensive 237Np analytical approach employing the short lived 239Np (t1/2 = 2.3 days) as a chemical yield tracer followed by 237Np quantification using inductively coupled plasma-mass spectrometry. 239Np tracer is obtained via separation from a 243Am stock solution and standardized using gamma spectrometry immediately prior to sample processing. Rapid digestions using a commercial, 900 watt “Walmart” microwave and Parr microwave vessels result in 99.8 ± 0.1% digestion yields, while chromatographic separations enable Np/U separation factors on the order of 106 and total Np yields of 95 ± 4% (2σ). Application of this method to legacy soil samples surrounding a radioactive disposal facility (the Subsurface Disposal Area at Idaho National Laboratory) reveal the presence of low level 237Np contamination within 600 meters of this site, with maximum 237Np concentrations on the order of 103 times greater than nuclear weapons testing fallout levels.

  6. {sup 237}Np and {sup 57}Fe Moessbauer study of NpFeGa{sub 5}

    Energy Technology Data Exchange (ETDEWEB)

    Homma, Y., E-mail: yhomma@imr.tohoku.ac.jp [Tohoku University, Institute for Materials Research (Japan); Nakada, M. [Japan Atomic Energy Research Institute, Nuclear Science and Engineering Directorate (Japan); Nakamura, A. [Japan Atomic Energy Research Institute, Advance Science Research Center (Japan); Nasu, S.; Aoki, D. [Tohoku University, Institute for Materials Research (Japan); Sakai, H.; Ikeda, S.; Yamamoto, E.; Haga, Y.; Onuki, Y. [Japan Atomic Energy Research Institute, Advance Science Research Center (Japan); Shiokawa, Y. [Tohoku University, Institute for Materials Research (Japan)

    2006-02-15

    {sup 57}Fe and {sup 237}Np Moessbauer Omeasurements have been performed for NpFeGa{sub 5}, which is one of the so-called neptunium 1-1-5 compounds. The {sup 57}Fe Moessbauer spectra below T{sub N} = 118 K show the magnetically ordered state. The magnitude of the hyperfine magnetic field at the {sup 57}Fe nucleus is determined to be 1.98 {+-} 0.05 T at 10 K. From the {sup 237}Np Moessbauer spectrum at 10 K, the hyperfine magnetic field at the {sup 237}Np nucleus is 203 T and the hyperfine coupling constant is determined to be 237 T/{mu}{sub B} using the Np atomic magnetic moment of 0.86 {mu}{sub B} determined by the neutron diffraction study.

  7. Delayed gamma studies from photo-fission of {sup 237}Np for nuclear waste characterization

    Energy Technology Data Exchange (ETDEWEB)

    Dighe, P.M. [CEA Saclay, IRFU/SPhN, 91191 Gif-sur-Yvette (France); Berthoumieux, E. [CEA Saclay, IRFU/SPhN, 91191 Gif-sur-Yvette (France)], E-mail: Eric.Berthoumieux@cea.fr; Dore, D. [CEA Saclay, IRFU/SPhN, 91191 Gif-sur-Yvette (France); Laborie, J.M.; Ledoux, X. [CEA, DPTA/SPN, Bruyeres-le-Chatel, 91297 Arpajon (France); Macary, V.; Panebianco, S.; Ridikas, D. [CEA Saclay, IRFU/SPhN, 91191 Gif-sur-Yvette (France)

    2009-04-15

    An active and non-destructive method is being established for detection of {sup 237}Np in nuclear waste barrels. The unique high energy decay gamma signature produced after photo-fission is analysed to deduce decay time parameters. A high purity {sup 237}Np sample was irradiated with bremsstrahlung photons and high energy gamma decay spectra were measured with BGO detectors for various irradiation durations. The analysis of decay spectra resulted in the formation of five decay groups, which can reproduce the experimental decay spectra within 10% accuracy. These parameters together with neutron decay groups are absolutely essential to quantify the nuclear material in waste barrels by photo-fission. The delayed decay gamma groups for {sup 237}Np nucleus are being reported for the first time.

  8. Delayed gamma studies from photo-fission of {sup 237}Np for nuclear waste characterization

    Energy Technology Data Exchange (ETDEWEB)

    Dighe, P.M.; Berthoumieux, E.; Dore, D.; Macary, V.; Panebianco, S.; Ridikas, D. [CEA/DSM Saclay, IRFU/SPhN, 91191 Gif-sur-Yvette (France); Laborie, J.M.; Ledoux, X. [CEA/DAM Ile-de-France, DPTA/SPN, 91680 Bruyeres-le-Chatel (France)

    2008-07-01

    An active and non destructive method is being established for detection of {sup 237}Np in nuclear waste barrels. The unique high-energy decay-gamma signature produced after photo-fission is analysed to deduce decay time parameters. High purity {sup 237}Np sample was irradiated with Bremsstrahlung photons and high energies gamma decay spectra were measured with BGO detectors for various irradiation durations. The analysis of decay spectra resulted in formation of five decay groups, which can reproduce the experimental decay spectra within 10 % accuracy. These parameters together with neutron decay groups are absolutely essential to quantify the nuclear material in waste barrels by photo-fission. The delayed decay gamma groups for {sup 237}Np nucleus are being reported for the first time. (authors)

  9. Reliable determination of 237Np in environmental solid samples using 242Pu as a potential tracer

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per;

    2011-01-01

    onto various AG 1-type anion exchangers; suitability of 242Pu as a tracer for 237Np determination in environmental solid samples; and long-term chemical stability of tetravalent Np. Experimental results revealed that the degree of resin cross-linking has a significant influence on the separation...

  10. (237)Np(n,f) Cross Section: New Data and Present Status

    CERN Document Server

    Paradela, C; Carrapico, C; Eleftheriadis, C; Leeb, H; Calvino, F; Herrera-Martinez, A; Savvidis, I; Vlachoudis, V; Haas, B; Vannini, G; Le Naour, C; Gramegna, F; Wiescher, M; Pigni, M T; Audouin, L; Mengoni, A; Quesada, J; Becvar, F; Plag, R; Cennini, P; Mosconi, M; Duran, I; Rauscher, T; Couture, A; Capote, R; Sarchiapone, L; Vlastou, R; Domingo-Pardo, C; Dillmann, I; Pavlopoulos, P; Karamanis, D; Krticka, M; Jericha, E; Ferrari, A; Martinez, T; Trubert, D; Oberhummer, H; Karadimos, D; Plompen, A; Isaev, S; Terlizzi, R; Kaeppeler, F; Cortes, G; Cox, J; Voss, F; Pretel, C; Colonna, N; Berthoumieux, E; Vaz, P; Heil, M; Lopes, I; Lampoudis, C; Walter, S; Calviani, M; Gonzalez-Romero, E; Embid-Segura, M; Stephan, C; Igashira, M; Papachristodoulou, C; Aerts, G; Tavora, L; Berthier, B; Rudolf, G; Andrzejewski, J; Villamarin, D; Ferreira-Marques, R; Tain, J L; O'Brien, S; Gunsing, F; Reifarth, R; Perrot, L; Lindote, A; Neves, F; Poch, A; Kerveno, M; Rubbia, C; Koehler, P; Dahlfors, M; Wisshak, K; Salgado, J; Dridi, W; Ventura, A; Andriamonje, S; Assimakopoulos, P; Santos, C; Ferrant, L; Lozano, M; Patronis, N; Chiaveri, E; Guerrero, C; Kadi, Y; Vicente, M C; Praena, J; Baumann, P; Oshima, M; Rullhusen, P; Furman, W; David, S; Marrone, S; Tassan-Got, L; Cano-Ott, D; Pavlix, A; Alvarez-Velarde, F; Massimi, C; Mastinu, P; Pancin, J; Papadopoulos, C; Tagliente, G; Haight, R; Chepel, V; Kossionides, E; Badurek, G; Marganiec, J; Lukic, S; Tarrio, D; Alvarez, H

    2011-01-01

    In this document, we present the final result obtained at the n_TOF experiment; for the neutron-induced fission cross section of the (237)Np, from the fission threshold up to 1 GeV. The method applied to get tins result is briefly discussed. n_TOF data are compared to the last experimental measurements using other TOF facilities or the surrogate method, reported experiments performed with monoenergetic sources and the FISCAL systematic, including a discussion about the existing discrepancies.

  11. Nuclear Resonance Fluorescence Measurements on ^237Np for Security and Safeguards Applications

    Science.gov (United States)

    Angell, C. T.; Joshi, T.; Yee, Ryan; Norman, E. B.; Kulp, W. D.; Warren, G. A.; Korbly, S.; Klimenko, A.; Wilson, C.; Copping, R.; Shuh, D. K.

    2009-10-01

    The smuggling of nuclear material and the diversion of fissile material for covert weapon programs both present grave risks to world security. Methods are needed to detect nuclear material smuggled in cargo, and for proper material accountability in civilian fuel re-processing facilities. Nuclear resonance fluorescence (NRF) is a technique that can address both needs. It is a non-destructive active interrogation method that provides isotope-specific information. It works by using a γ-ray beam to resonantly excite levels in a nucleus and observing the γ-rays emitted whose energy and intensity are characteristic of that isotope. ^237Np presents significant safeguard challenges; it is fissile yet currently has fewer safeguard restrictions. NRF measurements on ^237Np will expand the nuclear database and will permit designing interrogation and assay systems. Measurements were made using the bremsstrahlung beam at the HVRL at MIT on a 7 g target of ^237Np with two incident electron energies of 2.8 and 3.1 MeV. Results will be presented with discussion of the relevant nuclear structure necessary to predict levels in other actinides.

  12. RAPID SEPARATION METHOD FOR 237NP AND PU ISOTOPES IN LARGE SOIL SAMPLES

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.; Culligan, B.; Noyes, G.

    2010-07-26

    A new rapid method for the determination of {sup 237}Np and Pu isotopes in soil and sediment samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used for large soil samples. The new soil method utilizes an acid leaching method, iron/titanium hydroxide precipitation, a lanthanum fluoride soil matrix removal step, and a rapid column separation process with TEVA Resin. The large soil matrix is removed easily and rapidly using this two simple precipitations with high chemical recoveries and effective removal of interferences. Vacuum box technology and rapid flow rates are used to reduce analytical time.

  13. 231Pa/230Th records of Arctic/Atlantic interchange in Fram Strait

    Science.gov (United States)

    Hoffmann, S. S.; McDermott, K. J.; McManus, J. F.; Mukasa, S. B.

    2014-12-01

    Fram Strait, the Arctic Ocean's only deep passage for exchange with lower latitude oceans, today serves as a conduit for waters flowing north into the Arctic Ocean and south into the Atlantic. Reconstruction of circulation patterns and strength at depth in the strait can help to clarify the history of Arctic/Atlantic deep water exchange and Arctic contributions to global meridional overturning circulation. We will present new sedimentary measurements of radioisotopes 231Pa and 230Th to provide information on this exchange in the past and its relationship to sedimentation and climatic events. Coretop and downcore 231Pa/230Th ratios from Arctic sediments indicate that 231Pa has been exported from the central Arctic basin throughout the Holocene and deglaciation. Fram Strait represents a possible sink for this "missing" 231Pa. Preliminary results from ODP Holes 908A and 909A, at 1274 m and 2519 m water depths respectively in the central strait, suggest that ratios in this region during the Holocene have varied between ~0.106 (above the 231Pa/230Th production ratio of 0.093 in seawater, indicating net import of 231Pa)and ~0.055 (well below the production ratio, indicating net export of 231Pa). Further measurements in cores from the Greenland and Svalbard continental slopes will give a fuller regional picture of 231Pa deposition and transport across the strait.

  14. Moessbauer Spectroscopic Studies of {sup 237}Np in frozen nitric acid solution

    Energy Technology Data Exchange (ETDEWEB)

    Nakada, M; Wang, J; Kitazawa, T; Takahashi, M; Takeda, M; Masaki, N M; Yamashita, T [Department of Materials Science, Japan Atomic Energy Research Institute (JAERI, present JAEA: Japan Atomic Energy Agency), Tokai, Naka, Ibaraki 319-1195 (Japan); Tsutsui, S, E-mail: wangjh@dicp.ac.c [Advanced Science Research Center, JAERI, Tokai, Naka, Ibaraki 319-1195 (Japan)

    2010-03-01

    We applied Moessbauer spectroscopy to {sup 237}Np in nitric acid solutions to study chemical states. Sample solutions were adjusted to 50 mg/ml of Np(V) and Np(VI) concentration in 0.6 M nitric acid solutions. These solutions were put into original designed containers for samples and mounted to sample holders. The values of isomer shift (IS, relative to NpAl{sub 2}) of Np(V) and Np(VI) in 0.6 M nitric acid were -17.4(1) and -37.2(3) mm/s at about 10 K, respectively. It was found that Np(V) had 7 coordination number and Np(VI) had 8 in nitric acid solutions from values of IS.

  15. Development of ionization technique for measurement of fast neutron induced fission products yields of {sup 237}Np

    Energy Technology Data Exchange (ETDEWEB)

    Goverdovski, A.A.; Khryachkov, V.A.; Ketlerov, V.V.; Mitrofanov, V.F.; Ostapenko, Yu.B.; Semenova, N.N.; Fomichev, A.N.; Rodina, L.F. [Institute of Physics and Power Engineering, Obninsk (Russian Federation)

    1997-03-01

    Twin gridded ionization chamber and corresponding software was designed for measurements of masses, kinetic energies and nuclear charges of fission fragments from fast neutron induced fission of {sup 237}Np. The ionization detector design, electronics, data acquisition and processing system and the test results are presented in this paper. (J.P.N.)

  16. DETERMINATION OF 237NP AND PU ISOTOPES IN LARGE SOIL SAMPLES BY INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.

    2010-07-26

    A new method for the determination of {sup 237}Np and Pu isotopes in large soil samples has been developed that provides enhanced uranium removal to facilitate assay by inductively coupled plasma mass spectrometry (ICP-MS). This method allows rapid preconcentration and separation of plutonium and neptunium in large soil samples for the measurement of {sup 237}Np and Pu isotopes by ICP-MS. {sup 238}U can interfere with {sup 239}Pu measurement by ICP-MS as {sup 238}UH{sup +} mass overlap and {sup 237}Np via {sup 238}U peak tailing. The method provides enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then transferring Pu to DGA resin for additional purification. The decontamination factor for removal of uranium from plutonium for this method is greater than 1 x 10{sup 6}. Alpha spectrometry can also be applied so that the shorter-lived {sup 238}Pu isotope can be measured successfully. {sup 239}Pu, {sup 242}Pu and {sup 237}Np were measured by ICP-MS, while {sup 236}Pu and {sup 238}Pu were measured by alpha spectrometry.

  17. Development of ionization technique for measurement of fast neutron induced fission products yields of {sup 237}Np

    Energy Technology Data Exchange (ETDEWEB)

    Goverdovski, A.A.; Khryachkov, V.A.; Ketlerov, V.V.; Mitrofanov, V.F.; Ostapenko, Yu.B.; Semenova, N.N.; Fomichev, A.N.; Rodina, L.F. [Institute of Physics and Power Engineering, Obninsk (Russian Federation)

    1997-03-01

    Twin gridded ionization chamber and corresponding software was designed for measurements of masses, kinetic energies and nuclear charges of fission fragments from fast neutron induced fission of {sup 237}Np. The ionization detector design, electronics, data acquisition and processing system and the test results are presented in this paper. (J.P.N.)

  18. Determination of traces of 237Np in environmental samples by ICP-MS after separation using TOA extraction chromatography.

    Science.gov (United States)

    Ji, Y Q; Li, J Y; Luo, S G; Wu, T; Liu, J L

    2001-09-01

    A simple, rapid, cost-efficient, and robust method for separation of 237Np with an extraction chromatographic column (TOA: tri-n-octylamine on Teflon powder) is outlined in detail and further improved for direct ICP-MS analysis. The column efficiently retained 237Np in 2 mol L(-1) HNO3 medium and all of the 237Np was easily eluted with 0.02 mol L(-1) oxalic acid in 0.16 mol L(-1) HNO3 at 95 degrees C. The separated solutions were free from most matrix elements and were aspirated into the ICP-MS directly. The decontamination factor for 238U is more than 10(4). The instrumental detection limit for 237Np was 0.46 pg mL(-1), which corresponds to 1.2 x 10(-5) Bq mL(-1). The method is more rapid than traditional radiometric techniques. It is also considered to be more suitable for environmental monitoring than existing methods based on TOA.

  19. Fission mode analysis of the reaction {sup 237}Np(n,f) - possibilities and perspectives

    Energy Technology Data Exchange (ETDEWEB)

    Siegler, P. [Joint Research Centre, Geel (Belgium). Geel Establishment

    1996-03-01

    Fission fragment properties for the reaction {sup 237}Np(n,f) have been measured at the Van de Graaff Laboratory of the IRMM. Using a double gridded ionization chamber the mass, kinetic energy and the angular distribution for both fission fragments could be determined simultaneously for an incident neutron energy range from E{sub n}=0.3 MeV upto E{sub n}=5.5 MeV. Complete datasets have been acquired for 13 different neutron energies covering sub barrier fission as well as fission in the plateau region. A detailed analysis of the fragment distributions and the respective momenta has been carried out, checking the coherence against the excitation energy of the compound nucleus. The consideration of multi-modal fission offers an improved possibility for the description of the fragment distributions backed up by theoretical calculations on the basis of the multi-model random-neck rupture model of Brosa, Grossmann and Mueller. The changes of the fission fragment properties under investigation are completely described and an interpretation of the findings is presented. (author)

  20. Diffusion coefficient test of {sup 237}Np in bentonite backfill materials

    Energy Technology Data Exchange (ETDEWEB)

    Cui Anxi; Fan Zhiwen; Zhang Jinsheng; Gu Cunli [China Inst. for Radiation Protection, Shanxi (China); Mukai, M.; Maeda, T.; Matsumoto, J.; Tanaka, T.; Ogawa, H. [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    2002-03-01

    This paper describes the work on diffusion coefficient test of Np in bentonite backfill materials. Due to its very low permeability, diffusion is the dominant migration mechanics in bentonite. The bentonite comes from Inner Mongolia of China. {sup 237}Np was used as tracer. The special apparatus for diffusion test was setup, the diffusion coefficient of Np in pure bentonite and sand-bentonite mixture were tested. The tracer was introduced between two bentonite columns. After a specific contacting period, the bentonite columns were taken out and cut to very thin slices. The radioactivity in bentonite slices was analyzed to give the nuclide concentration versus distance curves. The diffusion coefficient could be estimated. The diffusion coefficient of pure bentonite at different density was tested. When the density of pure bentonite samples varied from 1.1, 1.3, 1.5 to 1.7 g/ml, their diffusion coefficient were 1.36 x 10{sup -13} m{sup 2}/s 1.16 x 10{sup -13}m{sup 2}/s, 1.07 x 10{sup -13} m{sup 2}/s and 8.26 x 10{sup -14} m{sup 2}/s respectively. The diffusion coefficient of Np in sand-bentonite mixture sample was 4.13 x 10{sup -13} m{sup 2}/s. To estimate the distribution coefficient (K{sub d}) value of Np in mixture sample by diffusion method, the diffusion coefficient of Br was measured./ The concluded K{sub d} value was 77ml/g for the sand-bentonite mixture. The K{sub d} value obtained by batch test methods was 30ml/g. The reason is related with the error of Br diffusion coefficient and solid-liquid ratio. (author)

  1. New experimental determination of the neutronic resonance parameters of {sup 237}Np below 500 eV; Nouvelle determination experimentale des parametres de resonances neutroniques de {sup 237}Np en dessous de 500 eV

    Energy Technology Data Exchange (ETDEWEB)

    Gressier, V

    1999-10-01

    For studies of future nuclear reactors dedicated to nuclear waste transmutation, an improvement of the accuracy of the neutron radiative capture cross section of {sup 237}Np appears necessary. In the framework of a collaboration between the Commissariat a l'Energie atomique (CEA) and Institute for Reference Materials and Measurement (IRMM, Geel, Bergium), a new determination of the resonance parameters of {sup 237}Np has been performed. Two types of experiments are carried out at GELINA, the IRMM pulsed neutron source, using the time of flight method: a transmission experiment which is related to the neutron total cross section and a capture experiment which gives the neutron radiative capture cross section. The resonance parameters presented in this work are extracted from the transmission data between 0 and 500 eV with the least square code REFIT, using the Reich-Moore formalism. In parallel, the Doppler effect is investigated. The commonly used free gas model appears inadequate below 20 eV for neptunium dioxide at room temperature. By the use of the program DOPUSH, which calculates the Doppler broadening with a harmonic crystal model according to Lamb's theory, we are able to produce abetter fit of the experimental data for the resonances of {sup 237}Np in NpO{sub 2} at low energy or temperatures. In addition to the resonance parameters, a study of their mean value and distribution is included in this work. (authors)

  2. RAPID DETERMINATION OF 237 NP AND PU ISOTOPES IN WATER BY INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY AND ALPHA SPECTROMETRY

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.; Jones, V.; Culligan, B.; Nichols, S.; Noyes, G.

    2010-06-23

    A new method that allows rapid preconcentration and separation of plutonium and neptunium in water samples was developed for the measurement of {sup 237}Np and Pu isotopes by inductively-coupled plasma mass spectrometry (ICP-MS) and alpha spectrometry; a hybrid approach. {sup 238}U can interfere with {sup 239}Pu measurement by ICP-MS as {sup 238}UH{sup +} mass overlap and {sup 237}Np via peak tailing. The method provide enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then moving Pu to DGA resin for additional removal of uranium. The decontamination factor for uranium from Pu is almost 100,000 and the decontamination factor for U from Np is greater than 10,000. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration is performed using a streamlined calcium phosphate precipitation method. Purified solutions are split between ICP-MS and alpha spectrometry so that long and short-lived Pu isotopes can be measured successfully. The method allows for simultaneous extraction of 20 samples (including QC samples) in 4 to 6 hours, and can also be used for emergency response. {sup 239}Pu, {sup 242}Pu and {sup 237}Np were measured by ICP-MS, while {sup 236}Pu, {sup 238}Pu, and {sup 239}Pu were measured by alpha spectrometry.

  3. Dispersion amplitudes in the Moessbauer lineshape of /sup 237/Np, /sup 182/W, and /sup 195/Pt

    Energy Technology Data Exchange (ETDEWEB)

    Potzel, W. (Technische Universitaet Muenchen, Garching, Ger.); Wagner, F.E.; Kalvius, G.M.; Asch, L.; Spirlet, J.C.; Mueller, W.

    1977-01-01

    Measurements of the dispersion amplitude for the Moessbauer resonances in /sup 237/Np (60 keV), /sup 182/W (100 keV) and /sup 195/Pt (99 keV) are reported. For the E1 transition in /sup 237/Np a value of xi = -(3.4 + 0.2) x 10/sup -2/ was found. Theoretical estimates of xi for this case are of limited accuracy and the comparison with experimental data is inaccurate because of the considerable line broadening. Computer simulations show the influence of xi on /sup 237/Np hyperfine spectra. For the E2 transition in /sup 182/W the dependence of the effective value of xi on absorber thickness was studied. Extrapolations to zero thickness yield xi = -(1.0 +- 0.1) x 10/sup -2/ in good agreement with theoretical calculations. For /sup 195/Pt we found xi = -(1.1 +- 0.3) x 10/sup -2/ for the dispersion amplitude at zero absorber thickness. This is the first pure M1 transition for which a dispersion term has been observed. For all three resonances the dispersion is large enough to affect the determination of isomer shifts.

  4. 230Thand 231Pa in Seawater Sinking Particles from the North Atlantic GEOTRACES Transect

    Science.gov (United States)

    LU, Y.; Edwards, R. L.; Cheng, H.; Anderson, R. F.; Hayes, C. T.; Fleisher, M. Q.; Lam, P. J.; Huang, K. F.; Robinson, L. F.; Wang, X.

    2016-12-01

    The biological carbon pump in the ocean plays a key role in regulating atmospheric CO2 level via oceanic particle dynamics. Radionuclides with proper half-lives, like 230Th and 231Pa, can provide quantitative estimates of particle cycling on the timescales up to hundred thousand years. However, our understanding of particle dynamics is hindered by the difficulty in precisely determining particulate 230Th and 231Pa, due to the trace amounts of Th and Pa in seawater, especially in large sinking particles. Here, we developed a technique to measure sinking particulate 230Th and 231Pa in a small sample size (tens to hundreds attograms of 231Pa, equivalent to 100 L water pumped through QMA filter), and achieved an average precision in percentage level. We firstly applied leaching processes to the particulate samples. The samples were soaked in 8N HNO3 + 0.5N HF mixed with proportionally determined 229Th and 233Pa spikes, and heated at 100°C for 10 hours. Th and Pa were then pre-concentrated by co-precipitation with Fe. After HNO3-HClO4-HNO3 digestion of the precipitates, Th and Pa were separated and purified using anion exchange chromatography (Spectra/Gel anion resin 1x8). Pa was measured on a MC-ICP-MS instrument (Neptune) right after the chemistry in order to minimize the 233Pa "bleeding effect". Replication tests show a good agreement in 231Pa/230Th within the measurement uncertainties. Applying our method to the profile samples collected from the North Atlantic GEOTRACES Transect, we found that the concentrations of 230Th and 231Pa in sinking particles (>51 μm size fraction; attograms/liter) are about 1/10 of those in suspended ones (1 - 51 μm size fraction). The scavenging of Th and Pa to large particles appears to be a function of particle composition (CaCO3, POM, lithogenic, opal and Fe/Mn oxides). In addition, ratios of the adsorbed 231Pa to 230Th are the same in both types of particles, although the particles have significantly different residence time in

  5. Radiation protection potential of MOX-fuel doped with 231Pa and Cs radioisotopes.

    Science.gov (United States)

    Kryuchkov, E F; Glebov, V B; Apse, V A; Shmelev, A N

    2005-01-01

    The paper addresses the problem of MOX-fuel self-protection during full cycle of MOX-fuel management. Under conditions of the closed LWR cycle the proliferation-resistance levels were evaluated for fresh and spent MOX-fuel with 231Pa and Cs feed. As it follows from the paper results, combination of these two admixtures being doped into MOX-fuel is able to enhance the inherent radiation barrier and to weaken shortcomings of both proliferation deterrents.

  6. Holocene Paleocirculation from 231Pa/230Th in Sediments from the North Atlantic Ocean

    Science.gov (United States)

    McManus, J.; Francois, R.; Major, C.; Gherardi, J.; Hoffman, S.

    2004-12-01

    A new record of bulk sedimentary 231Pa/230Th excesses from core GGC5 on the Bermuda Rise has been produced by ICP-MS. The record reveals several aspects of the strength of the meridional overturning circulation during the last ten thousand years. Measurements of uranium, protactinium and thorium in the Holocene section recovered in GGC5 have been resolved at approximately 200-300 years, similar to the response time of excess 231Pa in the water column, and therefore should capture any large departure from modern values in the 231Pa/230Th indicator of paleocirculation. No dramatic increase in ratio or decrease in circulation is indicated by the data, which suggest vigorous overturning in the western basin of the North Atlantic since the end of the Younger Dryas. Instead of large changes in circulation, a series of oscillations punctuates the middle Holocene, indicating a variability of 10-20 percent in the rate of meridional overturning. Specific attention will be paid to millennial events postulated at 8.2 kyr, ~5 kyr, and in the most recent Holocene.

  7. Persistent export of 231Pa from the deep central Arctic Ocean over the past 35,000 years.

    Science.gov (United States)

    Hoffmann, Sharon S; McManus, Jerry F; Curry, William B; Brown-Leger, L Susan

    2013-05-30

    The Arctic Ocean has an important role in Earth's climate, both through surface processes such as sea-ice formation and transport, and through the production and export of waters at depth that contribute to the global thermohaline circulation. Deciphering the deep Arctic Ocean's palaeo-oceanographic history is a crucial part of understanding its role in climatic change. Here we show that sedimentary ratios of the radionuclides thorium-230 ((230)Th) and protactinium-231 ((231)Pa), which are produced in sea water and removed by particle scavenging on timescales of decades to centuries, respectively, record consistent evidence for the export of (231)Pa from the deep Arctic and may indicate continuous deep-water exchange between the Arctic and Atlantic oceans throughout the past 35,000 years. Seven well-dated box-core records provide a comprehensive overview of (231)Pa and (230)Th burial in Arctic sediments during glacial, deglacial and interglacial conditions. Sedimentary (231)Pa/(230)Th ratios decrease nearly linearly with increasing water depth above the core sites, indicating efficient particle scavenging in the upper water column and greater influence of removal by lateral transport at depth. Although the measured (230)Th burial is in balance with its production in Arctic sea water, integrated depth profiles for all time intervals reveal a deficit in (231)Pa burial that can be balanced only by lateral export in the water column. Because no enhanced sink for (231)Pa has yet been found in the Arctic, our records suggest that deep-water exchange through the Fram strait may export (231)Pa. Such export may have continued for the past 35,000 years, suggesting a century-scale replacement time for deep waters in the Arctic Ocean since the most recent glaciation and a persistent contribution of Arctic waters to the global ocean circulation.

  8. Concurrent determination of 237Np and Pu isotopes using ICP-MS: analysis of NIST environmental matrix standard reference materials 4357, 1646a, and 2702.

    Science.gov (United States)

    Matteson, Brent S; Hanson, Susan K; Miller, Jeffrey L; Oldham, Warren J

    2015-04-01

    An optimized method was developed to analyze environmental soil and sediment samples for (237)Np, (239)Pu, and (240)Pu by ICP-MS using a (242)Pu isotope dilution standard. The high yield, short time frame required for analysis, and the commercial availability of the (242)Pu tracer are significant advantages of the method. Control experiments designed to assess method uncertainty, including variation in inter-element fractionation that occurs during the purification protocol, suggest that the overall precision for measurements of (237)Np is typically on the order of ± 5%. Measurements of the (237)Np concentration in a Peruvian Soil blank (NIST SRM 4355) spiked with a known concentration of (237)Np tracer confirmed the accuracy of the method, agreeing well with the expected value. The method has been used to determine neptunium and plutonium concentrations in several environmental matrix standard reference materials available from NIST: SRM 4357 (Radioactivity Standard), SRM 1646a (Estuarine Sediment) and SRM 2702 (Inorganics in Marine Sediment).

  9. Mass and nuclear charge yields for sup 237 Np(2n sub th ,f) at different fission fragment kinetic energies

    Energy Technology Data Exchange (ETDEWEB)

    Martinez, G.; Barreau, G.; Sicre, A.; Doan, T.P.; Audouard, P.; Leroux, B. (CEA Centre d' Etudes Nucleaires de Bordeaux-Gradignan, 33 - Gradignan (France)); Arafa, W.; Brissot, R.; Bocquet, J.P. (Grenoble-1 Univ., 38 (France). Inst. des Sciences Nucleaires); Faust, H. (Institut Max von Laue - Paul Langevin, 38 - Grenoble (France)); Koczon, P.; Mutterer, M. (Technische Hochschule Darmstadt (Germany, F.R.). Inst. fuer Kernphysik); Goennenwein, F. (Tuebingen Univ. (Germany, F.R.). Physikalisches Inst.); Asghar, M. (Universite des Sciences et de la Technologie Houari Boumediene, Algiers (Algeria). Inst. de Physique); Quade, U.; Rudolph, K. (Muenchen Univ. (Germany, F.R.)); Engelhardt, D. (Karlsruhe Univ. (T.H.) (Germany, F.R.)); Piasecki, E. (Warsaw Univ. (Poland))

    1990-09-03

    The recoil mass separator LOHENGRIN of the Laue-Langevin Institute Grenoble has been used to measure for the first time, the yields of light fission fragments from the fissioning system: {sub 93}{sup 239}Np; this odd-Z nucleus is formed after double thermal neutron capture in a {sub 93}{sup 237}Np target. The mass distributions were measured for different kinetic energies between 92 and 115.5 MeV, but the nuclear charge distributions were determined only up to 112 MeV. These distributions are compared to the distributions obtained for the even-even system {sub 94}{sup 240}Pu. At high kinetic energy, the mass distribution shows a prominent peak around mass number A{sub L}=106. These cold fragmentations are discussed in terms of a calculation based on a scission point model extrapolated to the cold fission case. As expected for an odd-Z fissioning nucleus, the nuclear charge distributions do not reveal any odd-even effect. The global neutron odd-even effect is found to be (8.1{plus minus}1.5)%. A simple model has been used to show that most of the neutron odd-even effect results from prompt neutron evaporation from the fragments. (orig.).

  10. Neutron-induced transmutation reactions in 237Np, 238Pu, and 239Pu at the massive natural uranium spallation target

    Science.gov (United States)

    Zavorka, L.; Adam, J.; Baldin, A. A.; Caloun, P.; Chilap, V. V.; Furman, W. I.; Kadykov, M. G.; Khushvaktov, J.; Pronskikh, V. S.; Solnyshkin, A. A.; Sotnikov, V.; Stegailov, V. I.; Suchopar, M.; Tsoupko-Sitnikov, V. M.; Tyutyunnikov, S. I.; Voronko, V.; Vrzalova, J.

    2015-04-01

    Transmutation reactions in the 237Np, 238Pu, and 239Pu samples were investigated in the neutron field generated inside a massive (m = 512 kg) natural uranium spallation target. The uranium target assembly QUINTA was irradiated with the deuteron beams of kinetic energy 2, 4, and 8 GeV provided by the Nuclotron accelerator at the Joint Institute for Nuclear Research (JINR) in Dubna. The neutron-induced transmutation of the actinide samples was measured off-line by implementing methods of gamma-ray spectrometry with HPGe detectors. Results of measurement are expressed in the form of both the individual reaction rates and average fission transmutation rates. For the purpose of validation of radiation transport programs, the experimental results were compared with simulations of neutron production and distribution performed by the MCNPX 2.7 and MARS15 codes employing the INCL4-ABLA physics models and LAQGSM event generator, respectively. In general, a good agreement between the experimental and calculated reaction rates was found in the whole interval of provided beam energies.

  11. Studies of Long-lived Radionuclides in the Environment - with Emphasis on {sup 99}Tc, {sup 237}Np and Pu Isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Lindahl, Patric

    2003-03-01

    Studies of the long-lived anthropogenic radionuclides 99Tc, 237Np, 239Pu and 240Pu were performed in marine and terrestrial areas contaminated by different accidental and controlled releases of radioactive materials. The three main sources discussed in this thesis are nuclear weapons tests, nuclear reprocessing plants and the Chernobyl accident. Results are mainly based on measurements of environmental samples collected in different parts of Sweden. An analytical method for trace analysis of plutonium and neptunium in environmental samples using ICP-MS (Inductively Coupled Plasma Mass Spectrometry) is described, and the results compared with those from conventional alpha spectrometry. The use of activated carbon filters for the separation of 99Tc from marine waters, with an adsorption efficiency in the range of 70%, is described. During 1991, 1995 and 2001 brown seaweed samples were collected at several stations along the Swedish west coast. In addition to these locations, a well-defined site (Saerdal; 56.76 deg N, 12.63 deg E) was included from which 99Tc data were collected from 1967 to 2000. The effect of discharges from the Sellafield EARP (Enhanced Actinide Removal Plant) from 1995-1996 was observed in brown seaweed from the Swedish west coast 4-5 years later, with a ten-fold increase in 99Tc activity concentration. An inverse correlation between 99Tc and 137Cs concentrations in seaweed was observed due to continuous mixing of high-Tc-low-Cs (Atlantic Sea) and low-Tc-high-Cs (Baltic Sea) waters. Radioactive materials from the Chernobyl accident contaminated various part of Sweden and by analysing lichen samples from different areas an estimate of the deposited 237Np density could be made. Through the determination of 240Pu/239Pu and 237Np/239Pu atomic ratios, source identification could be made in Swedish lichen samples. In the areas most contaminated by the Chernobyl accident in Sweden, the Chernobyl-derived 237Np contribution was up to 30% of the total

  12. Meridional circulation across the Antarctic Circumpolar Current serves as a double 231Pa and 230Th trap

    Science.gov (United States)

    Rutgers van der Loeff, Michiel; Venchiarutti, Celia; Stimac, Ingrid; van Ooijen, Jan; Huhn, Oliver; Rohardt, Gerd; Strass, Volker

    2016-12-01

    Upwelling of Circumpolar Deep Water in the Weddell Gyre and low scavenging rates south of the Antarctic Circumpolar Current (ACC) cause an accumulation of particle reactive nuclides in the Weddell Gyre. A ventilation/reversible scavenging model that successfully described the accumulation of 230Th in this area was tested with other particle reactive nuclides and failed to adequately describe the depth-distributions of 231Pa and 210Pb. We present here a modified model that includes a nutrient-like accumulation south of the Antarctic Polar Front in an upper meridional circulation cell, as well as transport to a deep circulation cell in the Weddell Gyre by scavenging and subsequent release at depth. The model also explains depletion of 231Pa and 230Th in Weddell Sea Bottom Water (WSBW) by ventilation of newly formed deep water on a timescale of 10 years, but this water mass is too dense to leave the Weddell Gyre. In order to quantify the processes responsible for the 231Pa- and 230Th-composition of newly formed Antarctic Bottom Water (AABW) we present a mass balance of 231Pa and 230Th in the Atlantic sector of the Southern Ocean based on new data from the GEOTRACES program. The ACC receives 6.0 ± 1.5 ×106 dpms-1 of 230Th from the Weddell Sea, similar in magnitude to the net input of 4.2 ± 3.0 ×106 dpms-1 from the north. For 231Pa, the relative contribution from the Weddell Sea is much smaller, only 0.3 ± 0.1 ×106, compared to 2.7 ± 1.4 ×106 dpms-1 from the north. Weddell Sea Deep Water (WSDW) leaving the Weddell Gyre northward to form AABW is exposed in the ACC to resuspended opal-rich sediments that act as efficient scavengers with a Th/Pa fractionation factor F ≤ 1. Hydrothermal inputs may provide additional removal with low F. Scavenging in the full meridional circulation across the opal-rich ACC thus acts as a double 231Pa and 230Th trap that preconditions newly formed AABW.

  13. Temporal evolution of (137)Cs, (237)Np, and (239+240)Pu and estimated vertical (239+240)Pu export in the northwestern Mediterranean Sea.

    Science.gov (United States)

    Bressac, M; Levy, I; Chamizo, E; La Rosa, J J; Povinec, P P; Gastaud, J; Oregioni, B

    2017-10-01

    The evolution of (137)Cs, (237)Np and (239+240)Pu at the DYFAMED station (NW Mediterranean) is discussed in relation to physical processes, downward fluxes of particles, and changes in the main input sources. The data set presented in this study represents the first complete (237)Np vertical profiles (0.12-0.27μBqL(-1)), and constitutes a baseline measurement to assess future changes. A similar behavior of Cs and Np has been evidenced, confirming that Np behaves conservatively. While the (137)Cs decrease has been driven by its radioactive decay, the vertical distribution of (237)Np has not substantially changed over the last decade. In the absence of recent major inputs, a homogenization of their vertical distribution occurred, partly due to deep convection events that became more intense during the last decade. In contrast, (239+240)Pu surface levels in the NW Mediterranean waters have fallen in the past four decades by a factor of 5. This decrease in surface has been balanced by higher concentrations in the deep-water layers. A first estimate of the downward (239+240)Pu fluxes in the NW Mediterranean Sea is proposed over more than two decades. This estimation, based on the DYFAMED sediment trap time-series data and published (239+240)Pu flux measurements, suggests that sinking particles have accounted for 60-90% of the upper layer (0-200m) Pu inventory loss over the period 1989-2013. The upper layer residence time of Pu is estimated to be ~28years, twice as long as the residence time estimated for the whole western Mediterranean (~15years). This difference highlights the slow removal of Pu in the open waters of the NW Mediterranean and confirms that most of the Pu removal occurs along the coastal margin where sedimentation rates are high. Copyright © 2017 Elsevier B.V. All rights reserved.

  14. Emission probabilities of {gamma}-rays from {sup 238}Np and their use for determination of the thermal neutron capture cross section of {sup 237}Np

    Energy Technology Data Exchange (ETDEWEB)

    Letourneau, A. [Irfu, CEA-Saclay, 91191 Gif-sur-Yvette (France)], E-mail: aletourneau@cea.fr; Marie, F. [Irfu, CEA-Saclay, 91191 Gif-sur-Yvette (France); Mutti, P. [Institut Laue-Langevin, 38000 Grenoble (France); AlMahamid, I. [Wadsworth Center, Laboratory of Inorganic and Nuclear Chemistry, Albany, NY (United States)

    2010-03-15

    The relevant absolute {gamma}-ray emission probabilities from the {beta}-decay of {sup 238}Np were measured by means of {alpha}- and {gamma}-spectroscopic techniques. We obtained values of (25.6{+-}0.4)%, (8.9{+-}0.2)% and (18.8{+-}0.3)% for the 984.45-, 1025.87- and 1028.54-keV {gamma}-rays, respectively, in agreement with the previous measured ones. These intensities were used to deduce the thermal neutron capture cross section of {sup 237}Np for which a value of (182.2{+-}4.5) b is obtained higher by 11% than the recommended value.

  15. On the sequential separation and quantification of (237)Np, (241)Am, thorium, plutonium, and uranium isotopes in environmental and urine samples.

    Science.gov (United States)

    Vasile, M; Jacobs, K; Bruggeman, M; Van Hoecke, K; Dobney, A; Verrezen, F

    2017-07-13

    The implementation of the one-pass-through separation technique using two stacked chromatography columns of TEVA - TRU resins for the separation of (237)Np, (241)Am, thorium, plutonium and uranium from environmental and urine samples was investigated. The sequential separation technique proved to be successful and gave similar results to those obtained when using individual separations. The analysis time was considerably improved. The amount of chemical waste was also reduced by 50% and the use of HClO4 was avoided. The technique of ICP-MS was also investigated as a complementary technique to alpha-spectrometry. Copyright © 2017 Elsevier Ltd. All rights reserved.

  16. Sediment 231Pa/230Th as a recorder of the rate of the Atlantic meridional overturning circulation: insights from a 2-D model

    Directory of Open Access Journals (Sweden)

    S. E. Allen

    2010-03-01

    Full Text Available A two dimensional scavenging model is used to investigate the patterns of sediment 231Pa/230Th generated by the Atlantic Meridional Overturning Circulation (AMOC and further advance the application of this proxy for ocean paleocirculation studies. The scavenging parameters and the geometry of the overturning circulation cell have been chosen so that the model generates meridional sections of dissolved 230Th and 231Pa consistent with published water column profiles and an additional 12 previously unpublished profiles measured in the North and Equatorial Atlantic. The processes that generate the meridional sections of dissolved and particulate 230Th, dissolved and particulate 231Pa, dissolved and particulate 231Pa/230Th, and sediment 231Pa/230Th are discussed in detail. The results indicate that the relationship between sediment 231Pa/230Th at any given site and the overturning circulation is very complex. They clearly show that constraining past changes in the strength and geometry of the AMOC requires an extensive data set and they suggest strategies to maximize information from a limited number of samples.

  17. Sediment 231Pa/230Th as a recorder of the rate of the Atlantic meridional overturning circulation: insights from a 2-D model

    Directory of Open Access Journals (Sweden)

    S. E. Allen

    2009-11-01

    Full Text Available A two dimensional scavenging-circulation model is used to investigate the patterns of sediment 231Pa/230Th generated by the Atlantic Meridional Overturning Circulation (AMOC and further advance the application of this proxy for ocean paleocirculation studies. The scavenging parameters and the geometry of the overturning circulation cell have been chosen so that the model generates meridional sections of dissolved 230Th and 231Pa consistent with published water column profiles and an additional 12 previously unpublished profiles measured in the North and Equatorial Atlantic. The processes that generate the meridional sections of dissolved and particulate 230Th, dissolved and particulate 231Pa, dissolved and particulate 231Pa/230Th, and sediment 231Pa/230Th are discussed in detail. The results indicate that the relationship between sediment 231Pa/230Th at any given site and the overturning circulation is very complex. They clearly show that constraining past changes in the strength and geometry of the AMOC requires an extensive data set and they suggest strategies to maximize information from a limited number of samples.

  18. Transmutation of 129I and 237Np using spallation neutrons produced by 1.5, 3.7 and 7.4 GeV protons

    Science.gov (United States)

    Wan, J.-S.; Schmidt, Th.; Langrock, E.-J.; Vater, P.; Brandt, R.; Adam, J.; Bradnova, V.; Bamblevski, V. P.; Gelovani, L.; Gridnev, T. D.; Kalinnikov, V. G.; Krivopustov, M. I.; Kulakov, B. A.; Sosnin, A. N.; Perelygin, V. P.; Pronskikh, V. S.; Stegailov, V. I.; Tsoupko-Sitnikov, V. M.; Modolo, G.; Odoj, R.; Phlippen, P.-W.; Zamani-Valassiadou, M.; Adloff, J. C.; Debeauvais, M.; Hashemi-Nezhad, S. R.; Guo, S.-L.; Li, L.; Wang, Y.-L.; Dwivedi, K. K.; Zhuk, I. V.; Boulyga, S. F.; Lomonossova, E. M.; Kievitskaja, A. F.; Rakhno, I. L.; Chigrinov, S. E.; Wilson, W. B.

    2001-05-01

    Small samples of 129I and 237Np, two long-lived radwaste nuclides, were exposed to spallation neutron fluences from relatively small metal targets of lead and uranium, that were surrounded with a 6 cm thick paraffin moderator, and irradiated with 1.5, 3.7 and 7.4 GeV protons. The (n,γ) transmutation rates were determined for these nuclides. Conventional radiochemical La- and U-sensors and a variety of solid-state nuclear track detectors were irradiated simultaneously with secondary neutrons. Compared with results from calculations with well-known cascade codes (LAHET from Los Alamos and DCM/CEM from Dubna), the observed secondary neutron fluences are larger.

  19. Transmutation of {sup 129}I and {sup 237}Np using spallation neutrons produced by 1.5, 3.7 and 7.4 GeV protons

    Energy Technology Data Exchange (ETDEWEB)

    Wan, J.-S.; Schmidt, T.Th.; Langrock, E.-J.; Vater, P.; Brandt, R. E-mail: brandtr@mailer.uni-marburg.de; Adam, J.; Bradnova, V.; Bamblevski, V.P.; Gelovani, L.; Gridnev, T.D.; Kalinnikov, V.G.; Krivopustov, M.I.; Kulakov, B.A.; Sosnin, A.N.; Perelygin, V.P.; Pronskikh, V.S.; Stegailov, V.I.; Tsoupko-Sitnikov, V.M.; Modolo, G.; Odoj, R.; Phlippen, P.-W.; Zamani-Valassiadou, M.; Adloff, J.C.; Debeauvais, M.; Hashemi-Nezhad, S.R.; Guo, S.-L.; Li, L.; Wang, Y.-L.; Dwivedi, K.K.; Zhuk, I.V.; Boulyga, S.F.; Lomonossova, E.M.; Kievitskaja, A.F.; Rakhno, I.L.; Chigrinov, S.E.; Wilson, W.B

    2001-05-11

    Small samples of {sup 129}I and {sup 237}Np, two long-lived radwaste nuclides, were exposed to spallation neutron fluences from relatively small metal targets of lead and uranium, that were surrounded with a 6 cm thick paraffin moderator, and irradiated with 1.5, 3.7 and 7.4 GeV protons. The (n,{gamma}) transmutation rates were determined for these nuclides. Conventional radiochemical La- and U-sensors and a variety of solid-state nuclear track detectors were irradiated simultaneously with secondary neutrons. Compared with results from calculations with well-known cascade codes (LAHET from Los Alamos and DCM/CEM from Dubna), the observed secondary neutron fluences are larger.

  20. Transmutation of 129I, 237Np, 238Pu, 239Pu, and 241Am using neutrons produced in target-blanket system `Energy plus Transmutation' by relativistic protons

    Indian Academy of Sciences (India)

    J Adam; K Katovsky; A Balabekyan; V G Kalinnikov; M I Krivopustov; H Kumawat; A A Solnyshkin; V I Stegailov; S G Stetsenko; V M Tsoupko-Sitnikov; W Westmeier

    2007-02-01

    Target-blanket facility `Energy + Transmutation' was irradiated by proton beam extracted from the Nuclotron Accelerator in Laboratory of High Energies of Joint Institute for Nuclear Research in Dubna, Russia. Neutrons generated by the spallation reactions of 0.7, 1.0, 1.5 and 2 GeV protons and lead target interact with subcritical uranium blanket. In the neutron field outside the blanket, radioactive iodine, neptunium, plutonium and americium samples were irradiated and transmutation reaction yields (residual nuclei production yields) have been determined using -spectroscopy. Neutron field's energy distribution has also been studied using a set of threshold detectors. Results of transmutation studies of 129I, 237Np, 238Pu, 239Pu and 241Am are presented.

  1. Capture and Fission rate of 232-Th, 238-U, 237-Np and 239-Pu from spallation neutrons in a huge block of lead.

    CERN Document Server

    Vlachoudis, Vasilis

    2000-01-01

    The study is centered on the research of the incineration possibility of nuclear waste, by the association of a particle accelerator with a multiplying medium of neutrons, in the project "Energy Amplifier" of C. Rubbia. It consists of the experimental determination of the rates of capture and fission of certain elements (232-Th, 238-U, 237-Np and 239-Pu) subjected to a fluence of fast spallation neutrons. These neutrons are produced by the interaction of high kinetic energy protons (several GeV) provided by the CERN-PS accelerator, on a large lead solid volume. The measurement techniques used in this work, are based on the activation of elements in the lead volume and the subsequent gamma spectroscopy of the activated elements, and also by the detection of fission fragment traces. The development, of a Monte Carlo code makes it possible, on one hand, to better understand the relevant processes, and on the other hand, to validate the code, by comparison with measurements, for the design and the construction of...

  2. 230Th and 231Pa on GEOTRACES GA03, the U.S. GEOTRACES North Atlantic transect, and implications for modern and paleoceanographic chemical fluxes

    Science.gov (United States)

    Hayes, Christopher T.; Anderson, Robert F.; Fleisher, Martin Q.; Huang, Kuo-Fang; Robinson, Laura F.; Lu, Yanbin; Cheng, Hai; Edwards, R. Lawrence; Moran, S. Bradley

    2015-06-01

    The long-lived uranium decay products 230Th and 231Pa are widely used as quantitative tracers of adsorption to sinking particles (scavenging) in the ocean by exploiting the principles of radioactive disequilibria. Because of their preservation in the Pleistocene sediment record and through largely untested assumptions about their chemical behavior in the water column, the two radionuclides have also been used as proxies for a variety of chemical fluxes in the past ocean. This includes the vertical flux of particulate matter to the seafloor, the lateral flux of insoluble elements to continental margins (boundary scavenging), and the southward flux of water out of the deep North Atlantic. In a section of unprecedented vertical and zonal resolution, the distributions of 230Th and 231Pa across the North Atlantic shed light on the marine cycling of these radionuclides and further inform their use as tracers of chemical flux. Enhanced scavenging intensities are observed in benthic layers of resuspended sediments on the eastern and western margins and in a hydrothermal plume emanating from the Mid-Atlantic Ridge. Boundary scavenging is clearly expressed in the water column along a transect between Mauritania and Cape Verde which is used to quantify a bias in sediment fluxes calculated using 230Th-normalization and to demonstrate enhanced 231Pa removal from the deep North Atlantic by this mechanism. The influence of deep ocean ventilation that leads to the southward export of 231Pa is apparent. The 231Pa/230Th ratio, however, predominantly reflects spatial variability in scavenging intensity, complicating its applicability as a proxy for the Atlantic meridional overturning circulation.

  3. Standard practice for the determination of 237Np, 232Th, 235U and 238U in urine by inductively coupled plasma-Mass spectrometry (ICP-MS) and gamma ray spectrometry.

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2005-01-01

    1.1 This practice covers the separation and preconcentration of neptunium-237 (237Np), thorium-232 (232Th), uranium-235 (235U) and uranium-238 (238U) from urine followed by quantitation using ICP-MS. 1.2 This practice can be used to support routine bioassay programs. The minimum detectable concentrations (MDC) for this method, taking the preconcentration factor into account, are approximately 1E-2Bq for 237Np (0.38ng), 2E-6Bq for 232Th (0.50ng), 4E-5Bq for 235U (0.50ng) and 6E-6Bq for 238U (0.48ng). 1.3 This standard does not purport to address all of the safety problems, if any, associated with its use. It is the responsibility of the user of this standard to establish appropriate safety and health practices and determine the applicability of regulatory limitations prior to use.

  4. High resolution measurement of the /sup 231/Pa(n,f) cross section from 0. 4 eV to 12 MeV

    Energy Technology Data Exchange (ETDEWEB)

    Plattard, S; Auchampaugh, G F; de Saussure, G

    1980-01-01

    The /sup 231/Pa(n,f) reaction was studied to shed light on the existence of a shallow third minimum in the /sup 232/Pa fission barrier. Results are plotted along with data points derived from ENDF/B-V. The occurrence of a pure vibrational state at E/sub n/ = 156.7 keV (3/sup +/) together with a nearby state of opposite parity favors the evidence for a third asymmetrically deformed minimum in the /sup 232/Pa fission barrier. 2 figures. (RWR)

  5. Measurement of the Neutron Capture Cross Sections of $^{233}$U, $^{237}$Np, $^{240,242}$Pu, $^{241,243}$Am and $^{245}$Cm with a Total Absorption Calorimeter at n_TOF

    CERN Multimedia

    Beer, H; Wiescher, M; Cox, J; Rapp, W; Embid, M; Dababneh, S

    2002-01-01

    Accurate and reliable neutron capture cross section data for actinides are necessary for the poper design, safety regulation and precise performance assessment of transmutation devices such as Fast Critical Reactors or Accelerator Driven Systems (ADS). The goal of this proposal is the measurement of the neutron capture cross sections of $^{233}$U, $^{237}$Np, $^{240,242}$Pu, $^{241,243}$Am and $^{245}$Cm at n_TOF with an accuracy of 5~\\%. $^{233}$U plays an essential role in the Th fuel cycle, which has been proposed as a safer and cleaner alternative to the U fuel cycle. The capture cross sections of $^{237}$Np,$^{240,242}$Pu, $^{241,243}$Am and $^{245}$Cm play a key role in the design and optimization of a strategy for the Nuclear Waste Transmutation. A high accuracy can be achieved at n_TOF in such measurements due to a combination of features unique in the world: high instantaneous neutron fluence and excellent energy resolution of the facility, innovative Data Acquisition System based on flash ADCs and t...

  6. Investigation of Neutron Spectra and Transmutation of ^{129}I, ^{237}Np and Other Nuclides with 1.5 GeV Protons from the Dubna Nuclotron Using the Electronuclear Setup "Energy plus Transmutation"

    CERN Document Server

    Krivopustov, M I; Balabekyan, A R; Batusov, Yu A; Bielewicz, M; Brandt, R; Chaloun, P; Chultem, D; Dwivedi, K K; Elishev, A F; Fragopoulou, M; Henzl, V; Henzlová, D; Kalinnikov, V G; Kievets, M K; Krása, A; Krizek, F; Kugler, A; Manolopoulou, Metaxia; Mariin, I I; Nourreddine, A; Odoj, R; Pavliouk, A V; Pronskikh, V S; Robotham, H; Siemon, K; Szuta, M; Stegailov, V I; Solnyshkin, A A; Sosnin, A N; Stoulos, S; Tsoupko-Sitnikov, V M; Tumendelger, T; Wojecehowski, A; Wagner, V; Wan, J S; Westmeier, W; Zamani-Valasiadou, M; Kumawat, H; Kumar, V; Zaverioukha, O S; Zhuk, I V

    2004-01-01

    Experiments which are part of the scientific program "Investigations of physical aspects of electronuclear method of energy production and transmutation for radioactive waste of atomic energetics using relativistic beams from the JINR Synchrophasotron/Nuclotron" (project "Energy plus Transmutation") are described. A large lead target surrounded by a four-section uranium blanket with total weight of 206.4 kg natural uranium was irradiated with 1.5 GeV protons from the new cryogenic accelerator Nuclotron. Radiochemical sensors were exposed to the secondary particle fluences inside and on top of the target assembly. Two long-lived radioactive waste of atomic energetics sensors ^{129}I and ^{237}Np (approximately 1 g weight each) and stable nuclides ^{27}Al, ^{59}Co, ^{127}I, ^{139}La, ^{197}Au and ^{209}Bi as well as natural and enriched uranium were used. In addition, various solid state nuclear track detectors and nuclear emulsions were exposed simultaneously. The experimental results confirm the theoretical e...

  7. Post-Irradiation Examination of 237Np Targets for 238Pu Production

    Energy Technology Data Exchange (ETDEWEB)

    Morris, Robert Noel [ORNL; Baldwin, Charles A [ORNL; Hobbs, Randy W [ORNL; Schmidlin, Joshua E [ORNL

    2015-01-01

    Oak Ridge National Laboratory is recovering the US 238Pu production capability and the first step in the process has been to evaluate the performance of a 237Np target cermet pellet encased in an aluminum clad. The process proceeded in 3 steps; the first step was to irradiate capsules of single pellets composed of NpO2 and aluminum power to examine their shrinkage and gas release. These pellets were formed by compressing sintered NpO2 and aluminum powder in a die at high pressure followed by sintering in a vacuum furnace. Three temperatures were chosen for sintering the solution precipitated NpO2 power used for pellet fabrication. The second step was to irradiate partial targets composed of 8 pellets in a semi-prototypical arrangement at the two best performing sintering temperatures to determine which temperature gave a pellet that performed the best under the actual planned irradiation conditions. The third step was to irradiate ~50 pellets in an actual target configuration at design irradiation conditions to assess pellet shrinkage and gas release, target heat transfer, and dimensional stability. The higher sintering temperature appeared to offer the best performance after one cycle of irradiation by having the least shrinkage, thus keeping the heat transfer gap between the pellets and clad small minimizing the pellet operating temperature. The final result of the testing was a target that can meet the initial production goals, satisfy the reactor safety requirements, and can be fabricated in production quantities. The current focus of the program is to verify that the target can be remotely dissembled, the pellets dissolved, and the 238Pu recovered. Tests are being conducted to examine these concerns and to compare results to code predictions. Once the performance of the full length targets has been quantified, the pellet 237Np loading will be revisited to determine if it can be increased to increase 238Pu production.

  8. Measurements of periods, relative abundances and absolute yields of delayed neutrons from fast neutron induced fission of {sup 237}Np

    Energy Technology Data Exchange (ETDEWEB)

    Piksaikine, V. [Institute of Physics and Power Engineering, Obninsk (Russian Federation)

    1997-03-01

    The experimental method for measurements of the delayed neutron yields and period is presented. The preliminary results of the total yield, relative abundances and periods are shown comparing with the previously reported values. (J.P.N.)

  9. Measurements of periods, relative abundances and absolute yields of delayed neutrons from fast neutron induced fission of {sup 237}Np

    Energy Technology Data Exchange (ETDEWEB)

    Piksaikine, V. [Institute of Physics and Power Engineering, Obninsk (Russian Federation)

    1997-03-01

    The experimental method for measurements of the delayed neutron yields and period is presented. The preliminary results of the total yield, relative abundances and periods are shown comparing with the previously reported values. (J.P.N.)

  10. 242Pu as tracer for simultaneous determination of 237Np and 239,240Pu in environmental samples

    DEFF Research Database (Denmark)

    Chen, Q.J.; Dahlgaard, H.; Nielsen, S.P.;

    2002-01-01

    A procedure has been developed using Pu-242 as tracer for simultaneous determination of Np-237 and Pu-239,Pu-240 in environmental samples. The validity of the method has been demonstrated by ICPMS and alpha-spectroscopy for up to 10 gram soil and sediment, seawater up to 200 litres. The paper...... describes a suitable chemical procedure for Np and Pu including a quantitative pre-concentration of neptunium and plutonium, preparation of Np4+ and Pu4+, NP(NO3)(6)(2-) and Pu(NO3)(6)(2-), The ratio of Np-237/Pu-242 (or Np-237/Pu-239) before and after the procedure has been determined using 10 g soil (free...... from Np and Pu) R-before/R-after = 1.004 +/- 3.3% (S.D n = 20) and 1 litre seawater R-before/R-after = 1.019+/-1.9% (S.D., n = 12). Results from the intercomparison samples LAEA-135, LAEA-381 and from environmental samples are presented....

  11. Procedures for determination of 239,240Pu, 241Am, 237Np, 234,238U, 2

    DEFF Research Database (Denmark)

    Chen, Q.J.; Aarkrog, Asker; Nielsen, Sven Poul;

    2001-01-01

    Since 1987, the Department of Nuclear Safety Research, Risø National Laboratory has developed procedures for analysis of low-level amounts of radioactivity in large samples of 200 liters seawater, 10 gram sediment, soil and other environmental materials.These analytical procedures provide high ch...

  12. Rapid determination of (237)Np and plutonium isotopes in urine by inductively-coupled plasma mass spectrometry and alpha spectrometry.

    Science.gov (United States)

    Maxwell, Sherrod L; Culligan, Brian K; Jones, Vernon D; Nichols, Sheldon T; Noyes, Gary W; Bernard, Maureen A

    2011-08-01

    A new rapid separation method was developed for the measurement of plutonium and neptunium in urine samples by inductively-coupled plasma mass spectrometry (ICP-MS) and/or alpha spectrometry with enhanced uranium removal. This method allows separation and preconcentration of plutonium and neptunium in urine samples using stacked extraction chromatography cartridges and vacuum box flow rates to facilitate rapid separations. There is an increasing need to develop faster analytical methods for emergency response samples. There is also enormous benefit to having rapid bioassay methods in the event that a nuclear worker has an uptake (puncture wound, etc.) to assess the magnitude of the uptake and guide efforts to mitigate dose (e.g., tissue excision and chelation therapy). This new method focuses only on the rapid separation of plutonium and neptunium with enhanced removal of uranium. For ICP-MS, purified solutions must have low salt content and low concentration of uranium due to spectral interference of (238)U(1)H(+) on m/z 239. Uranium removal using this method is enhanced by loading plutonium and neptunium initially onto TEVA resin, then moving plutonium to DGA resin where additional purification from uranium is performed with a decontamination factor of almost 1×10(5). If UTEVA resin is added to the separation scheme, a decontamination factor of ~3 × 10(6) can be achieved.

  13. A comparative radiological assessment of five European biosphere systems in the context of potential contamination of well water from the hypothetical disposal of radioactive waste.

    Science.gov (United States)

    Olyslaegers, G; Zeevaert, T; Pinedo, P; Simon, I; Pröhl, G; Kowe, R; Chen, Q; Mobbs, S; Bergström, U; Hallberg, B; Katona, T; Eged, K; Kanyar, B

    2005-12-01

    In the framework of the BioMoSA project for the development of biosphere assessment models for radioactive waste disposal the Reference Biosphere Methodology developed in the IAEA programme BIOMASS was applied to five locations, situated in different European countries. Specific biosphere models were applied to assess the hypothetical contamination of a range of agricultural and environmental pathways and the dose to individuals, following contamination of well water. The results of these site-specific models developed by the different BioMoSA partners, and the individual normalised dose to the exposure groups were compared against each other. Ingestion of drinking water, fruit and vegetables were found to be among the most important pathways for almost all radionuclides. Stochastic calculations revealed that consumption habits, transfer factors, irrigation rates and distribution coefficients (Kd(s)) were the most important parameters that influence the end results. Variations in the confidence intervals were found to be higher for sorbing elements (e.g. (36)Cl, (237)Np, (99)Tc, (238)U, (129)I) than for mobile elements (e.g. (226)Ra, (79)Se, (135)Cs, (231)Pa, (239)Pu). The influence of daughter products, for which the distribution into the biosphere was calculated individually, was also shown to be important. This paper gives a brief overview of the deterministic and stochastic modelling results and the parameter sensitivity. A screening methodology was introduced to identify the most important pathways, simplify a generic biosphere tool and refine the existing models.

  14. Parameters of the best approximation of reduced neutron widths distribution. Actinides

    CERN Document Server

    Sukhovoj, A M

    2011-01-01

    The data of ENDF/B-VII library on reduced neutron widths for nuclei 231Pa, 232Th, 233,234,235,236,238U, 237Np, 239,240,241,242Pu, 241,243Am and 243Cm (including p-resonances of 232Th, 238U, 239Pu) in form of cumulative sums in function on Gamma0n/ were approximated by variable number K of partial items 0

  15. Np-237 in peat and lichen in Finland

    DEFF Research Database (Denmark)

    Salminen, S.; Paatero, J.; Roos, Per;

    2009-01-01

    Activity concentrations of 237Np in peat and lichen samples in Finland were determined and contributions from nuclear weapons testing in 1950–1960s and the Chernobyl accident were estimated. 237Np was determined with ICP-MS using 235Np as a tracer. Activity concentrations of 237Np in peat samples...

  16. Application of the Spanish methodological approach for biosphere assessment to a generic high-level waste disposal site.

    Science.gov (United States)

    Agüero, A; Pinedo, P; Simón, I; Cancio, D; Moraleda, M; Trueba, C; Pérez-Sánchez, D

    2008-09-15

    A methodological approach which includes conceptual developments, methodological aspects and software tools have been developed in the Spanish context, based on the BIOMASS "Reference Biospheres Methodology". The biosphere assessments have to be undertaken with the aim of demonstrating compliance with principles and regulations established to limit the possible radiological impact of radioactive waste disposals on human health and on the environment, and to ensure that future generations will not be exposed to higher radiation levels than those that would be acceptable today. The biosphere in the context of high-level waste disposal is defined as the collection of various radionuclide transfer pathways that may result in releases into the surface environment, transport within and between the biosphere receptors, exposure of humans and biota, and the doses/risks associated with such exposures. The assessments need to take into account the complexity of the biosphere, the nature of the radionuclides released and the long timescales considered. It is also necessary to make assumptions related to the habits and lifestyle of the exposed population, human activities in the long term and possible modifications of the biosphere. A summary on the Spanish methodological approach for biosphere assessment are presented here as well as its application in a Spanish generic case study. A reference scenario has been developed based on current conditions at a site located in Central-West Spain, to indicate the potential impact to the actual population. In addition, environmental change has been considered qualitatively through the use of interaction matrices and transition diagrams. Unit source terms of (36)Cl, (79)Se, (99)Tc, (129)I, (135)Cs, (226)Ra, (231)Pa, (238)U, (237)Np and (239)Pu have been taken. Two exposure groups of infants and adults have been chosen for dose calculations. Results are presented and their robustness is evaluated through the use of uncertainty and

  17. The Separation Method of Neptunium in Reprocessed Uranium Product by TEVA-UTEVA Column Extraction Chromatography

    Institute of Scientific and Technical Information of China (English)

    JIN; Hua; SU; Yu-lan; YING; Zhe-cong; ZHAO; Sheng-yang

    2012-01-01

    <正>237Np, as a highly toxic nuclide, is limited strictly in the final uranium product of spent nuclear fuel reprocessing plant. Due to the low concentration level of 237Np, which is lower than 2.5 μg/g U, its accurate measurement is one of the most difficult analytical works in

  18. Systematic study of anomalous fragment anisotropies in subbarrier complete fusion—fission reactions

    Institute of Scientific and Technical Information of China (English)

    ZhangHuan-Qiao; LiuZu-Hua; 等

    1997-01-01

    The complete fusion-fission is separated from the transter-induced-fission with the fragment folding angle technique.The cross sections and fragment angular distributions for the complete fusion-fission reactions of 11B+ 238U(237Np),237NP,16O+232Th(238U) and 19F+232Th at near-and sub-barrier energies have been measured.The present fusion and fission standard models can reproduces both the excitation functions and the fragment anisotropies for the systems of 11B+238U(237Np)and 12C+237Np;but fail to explain both the experimental data for the other 3 systems simultaneously,The evidence of the entrance-channel dependence of fission-fragment anisotropies is revealsed by comparison of the 11B+237NP and 16O+232Th data.Based on the observations a new version model of preequilibrium fission is put forward to explain the anomaly.

  19. Inorganic, radioisotopic and organic analysis of 241-AP-101 tank waste

    Energy Technology Data Exchange (ETDEWEB)

    SK Fiskum; PR Bredt; JA Campbell; LR Greenwood; OT Farmer; GJ Lumetta; GM Mong; RT Ratner; CZ Soderquist; RG Swoboda; MW Urie; JJ Wagner

    2000-06-28

    Battelle received five samples from Hanford waste tank 241-AP-101, taken at five different depths within the tank. No visible solids or organic layer were observed in the individual samples. Individual sample densities were measured, then the five samples were mixed together to provide a single composite. The composite was homogenized and representative sub-samples taken for inorganic, radioisotopic, and organic analysis. All analyses were performed on triplicate sub-samples of the composite material. The sample composite did not contain visible solids or an organic layer. A subsample held at 10 C for seven days formed no visible solids. The characterization of the 241-AP-101 composite samples included: (1) Inductively-coupled plasma spectrometry for Ag, Al, Ba, Bi, Ca, Cd, Cr, Cu, Fe, K, La, Mg, Mn, Na, Nd, Ni, P, Pb, Pd, Ru, Rh, Si, Sr, Ti, U, Zn, and Zr (Note: Although not specified in the test plan, As, B, Be, Co, Li, Mo, Sb, Se, Sn, Tl, V, W, and Y were also measured and reported for information only) (2) Radioisotopic analyses for total alpha and total beta activities, {sup 3}H, {sup 14}C, {sup 60}Co, {sup 79}Se, {sup 90}Sr, {sup 99}Tc as pertechnetate, {sup 106}Ru/Rh, {sup 125}Sb, {sup 134}Cs, {sup 137}Cs, {sup 152}Eu, {sup 154}Eu, {sup 155}Eu, {sup 238}Pu, {sup 239+240}Pu, {sup 241}Am, {sup 242}Cm, and {sup 243+244}Cm; (3) Inductively-coupled plasma mass spectrometry for {sup 237}Np, {sup 239}Pu, {sup 240}Pu, {sup 99}Tc, {sup 126}Sn, {sup 129}I, {sup 231}Pa, {sup 233}U, {sup 234}U, {sup 235}U, {sup 236}U, {sup 238}U, {sup 241}AMU, {sup 242}AMU, {sup 243}AMU, As, B, Be, Ce, Co, Cs, Eu, I, Li, Mo, Pr, Rb, Sb, Se, Ta, Te, Th, Tl, V, and W; (4) total U by kinetic phosphorescence analysis; (5) Ion chromatography for Cl, F, NO{sub 2}, NO{sub 3}, PO{sub 4}, SO{sub 4}, acetate, formate, oxalate, and citrate; (6) Density, inorganic carbon and organic carbon by two different methods, mercury, free hydroxide, ammonia, and cyanide. The 241-AP-101 composite met all

  20. Analysis of trace neptunium in the vicinity of underground nuclear tests at the Nevada National Security Site.

    Science.gov (United States)

    Zhao, P; Tinnacher, R M; Zavarin, M; Kersting, A B

    2014-11-01

    A high sensitivity analytical method for (237)Np analysis was developed and applied to groundwater samples from the Nevada National Security Site (NNSS) using short-lived (239)Np as a yield tracer and HR magnetic sector ICP-MS. The (237)Np concentrations in the vicinity of the Almendro, Cambric, Dalhart, Cheshire, and Chancellor underground nuclear test locations range from tritium and other non-sorbing radionuclides ((14)C, (36)Cl, (99)Tc and (129)I) as expected. Surprisingly, (237)Np and plutonium ((239,240)Pu) retardation factors are very similar. It is possible that Np(IV) exists under mildly reducing groundwater conditions and exhibits a retardation behavior that is comparable to Pu(IV). Independent of the underlying process, (237)Np is migrating downgradient from NNSS underground nuclear tests at very low but measureable concentrations.

  1. Nuclear Criticality Safety of the DOT 9975 Container for237NpO2Storage, Handling, and Transport

    Energy Technology Data Exchange (ETDEWEB)

    Reed, D.A.

    2003-08-29

    Nuclear criticality safety considerations are presented to address use of the DOT 9975 shipping container for {sup 237}NpO{sub 2}. The DOT 9975 container will be used by multiple DOE sites and contractors. Various of site- and activity-specific NCS and facility safety documents are yet to be developed. For these reasons, an overall assessment of criticality safety of {sup 237}NpO{sub 2}-loaded DOT 9975 containers is considered useful to personnel involved in generating, reviewing, or approving these various documents. It is concluded that inherent container features, the loading per container (maximum of 6 kg {sup 237}Np), and the nuclear physics properties of {sup 237}NpO{sub 2} combine to preclude the potential for a nuclear criticality accident. This conclusion applies to storage, handling, and transport operations involving closed DOT 9975 packages, including credible off-normal conditions that may result in damage to packages during those operations.

  2. Palm content of production metal

    Energy Technology Data Exchange (ETDEWEB)

    Campbell, M.H.; Swift, W.H.

    1959-11-23

    Purpose of this study was to determine the {sup 237}Np input to the Purex process. The {sup 237}Np content of 639 g Pu/ton U irradiated fuel was found to be 1.78 {plus_minus} .09 g/ton of uranium at the 95% confidence level. Standard recovery for the chemical method was 96.7%, 98.0% for the sampling.

  3. Corrigendum to "Deep water provenance and dynamics of the (de)glacial Atlantic meridional overturning circulation" [Earth Planet. Sci. Lett. 445 (2016) 68-78

    Science.gov (United States)

    Lippold, Jörg; Gutjahr, Marcus; Blaser, Patrick; Christner, Emanuel; de Carvalho Ferreira, Maria Luiza; Mulitza, Stefan; Christl, Marcus; Wombacher, Frank; Böhm, Evelyn; Antz, Benny; Cartapanis, Olivier; Vogel, Hendrik; Jaccard, Samuel L.

    2017-01-01

    We have reconstructed past modes of the Atlantic Meridional Overturning Circulation (AMOC) by combining two sedimentary proxies, Nd isotopes (εNd) and the 231Pa/230Th ratio over the last deglaciation. Combined down-core 231Pa/230Th and εNd records from six Atlantic Ocean sediment archives are presented (Lippold et al., 2016).

  4. Neptunium Transport Behavior in the Vicinity of Underground Nuclear Tests at the Nevada Test Site

    Energy Technology Data Exchange (ETDEWEB)

    Zhao, P; Tinnacher, R M; Zavarin, M; Williams, R W; Kersting, A B

    2010-12-03

    We used short lived {sup 239}Np as a yield tracer and state of the art magnetic sector ICP-MS to measure ultra low levels of {sup 237}Np in a number of 'hot wells' at the Nevada National Security Site (NNSS), formerly known as the Nevada Test Site (NTS). The results indicate that {sup 237}Np concentrations at the Almendro, Cambric, Dalhart, Cheshire and Chancellor sites, are in the range of 3 x 10{sup -5} to 7 x 10{sup -2} pCi/L and well below the MCL for alpha emitting radionuclides (15 pCi/L) (EPA, 2009). Thus, while Np transport is believed to occur at the NNSS, activities are expected to be well below the regulatory limits for alpha-emitting radionuclides. We also compared {sup 237}Np concentration data to other radionuclides, including tritium, {sup 14}C, {sup 36}Cl, {sup 99}Tc, {sup 129}I, and plutonium, to evaluate the relative {sup 237}Np transport behavior. Based on isotope ratios relative to published unclassified Radiologic Source Terms (Bowen et al., 1999) and taking into consideration radionuclide distribution between melt glass, rubble and groundwater (IAEA, 1998), {sup 237}Np appears to be substantially less mobile than tritium and other non-sorbing radionuclides, as expected. However, this analysis also suggests that {sup 237}Np mobility is surprisingly similar to that of plutonium. The similar transport behavior of Np and Pu can be explained by one of two possibilities: (1) Np(IV) and Pu(IV) oxidation states dominate under mildly reducing NNSS groundwater conditions resulting in similar transport behavior or (2) apparent Np transport is the result of transport of its parent {sup 241}Pu and {sup 241}Am isotopes and subsequent decay to {sup 237}Np. Finally, measured {sup 237}Np concentrations were compared to recent Hydrologic Source Term (HST) models. The 237Np data collected from three wells in Frenchman Flat (RNM-1, RNM-2S, and UE-5n) are in good agreement with recent HST transport model predictions (Carle et al., 2005). The agreement

  5. Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean.

    Science.gov (United States)

    Lindahl, Patric; Roos, Per; Holm, Elis; Dahlgaard, Henning

    2005-01-01

    The long-lived anthropogenic radionuclides (237)Np, (239)Pu and (240)Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The (237)Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16+/-0.02 to 1.02+/-0.09 mBq kg(-1) (dry weight) and 0.65+/-0.02 to 1.69+/-0.02 mBq m(-3), respectively, depending on the location and sampling year. Most of the (237)Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The (240)Pu/(239)Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17+/-0.03. The (237)Np and (239)Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16+/-0.01 to 0.62+/-0.08 mBq m(-3) and from 0.64+/-0.05 to 4.27+/-0.08 mBq m(-3), respectively, and the (237)Np/(239)Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.

  6. Criticality experiments and benchmarks for cross section evaluation: the neptunium case

    Directory of Open Access Journals (Sweden)

    Duran I.

    2013-03-01

    Full Text Available The 237Np neutron-induced fission cross section has been recently measured in a large energy range (from eV to GeV at the n_TOF facility at CERN. When compared to previous measurement the n_TOF fission cross section appears to be higher by 5-7% beyond the fission threshold. To check the relevance of n_TOF data, we apply a criticality experiment performed at Los Alamos with a 6 kg sphere of 237Np, surrounded by enriched uranium 235U so as to approach criticality with fast neutrons. The multiplication factor ke f f of the calculation is in better agreement with the experiment (the deviation of 750 pcm is reduced to 250 pcm when we replace the ENDF/B-VII.0 evaluation of the 237Np fission cross section by the n_TOF data. We also explore the hypothesis of deficiencies of the inelastic cross section in 235U which has been invoked by some authors to explain the deviation of 750 pcm. With compare to inelastic large distortion calculation, it is incompatible with existing measurements. Also we show that the v of 237Np can hardly be incriminated because of the high accuracy of the existing data. Fission rate ratios or averaged fission cross sections measured in several fast neutron fields seem to give contradictory results on the validation of the 237Np cross section but at least one of the benchmark experiments, where the active deposits have been well calibrated for the number of atoms, favors the n_TOF data set. These outcomes support the hypothesis of a higher fission cross section of 237Np.

  7. Validation of Cross Sections with Criticality Experiment and Reaction Rates: the Neptunium Case

    Science.gov (United States)

    Leong, L. S.; Tassan-Got, L.; Audouin, L.; Berthier, B.; Le Naour, C.; Stéphan, C.; Paradela, C.; Tarrío, D.; Duran, I.

    2014-04-01

    The 237Np neutron-induced fission cross section has been recently measured in a large energy range (from eV to GeV) at the n_TOF facility at CERN. When compared to previous measurements the n_TOF fission cross section appears to be higher by 5-7% beyond the fission threshold. To check the relevance of the n_TOF data, we considered a criticality experiment performed at Los Alamos with a 6 kg sphere of 237Np, surrounded by uranium highly enriched in 235U so as to approach criticality with fast neutrons. The multiplication factor keff of the calculation is in better agreement with the experiment when we replace the ENDF/B-VII.0 evaluation of the 237Np fission cross section by the n_TOF data. We also explored the hypothesis of deficiencies of the inelastic cross section in 235U which has been invoked by some authors to explain the deviation of 750 pcm. The large modification needed to reduce the deviation seems to be incompatible with existing inelastic cross section measurements. Also we show that the νbar of 237Np can hardly be incriminated because of the high accuracy of the existing data. Fission rate ratios or averaged fission cross sections measured in several fast neutron fields seem to give contradictory results on the validation of the 237Np cross section but at least one of the benchmark experiments, where the active deposits have been well calibrated for the number of atoms, favors the n_TOF data set. These outcomes support the hypothesis of a higher fission cross section of 237Np.

  8. Criticality experiments and benchmarks for cross section evaluation: the neptunium case

    Science.gov (United States)

    Leong, L. S.; Tassan-Got, L.; Audouin, L.; Paradela, C.; Wilson, J. N.; Tarrio, D.; Berthier, B.; Duran, I.; Le Naour, C.; Stéphan, C.

    2013-03-01

    The 237Np neutron-induced fission cross section has been recently measured in a large energy range (from eV to GeV) at the n_TOF facility at CERN. When compared to previous measurement the n_TOF fission cross section appears to be higher by 5-7% beyond the fission threshold. To check the relevance of n_TOF data, we apply a criticality experiment performed at Los Alamos with a 6 kg sphere of 237Np, surrounded by enriched uranium 235U so as to approach criticality with fast neutrons. The multiplication factor ke f f of the calculation is in better agreement with the experiment (the deviation of 750 pcm is reduced to 250 pcm) when we replace the ENDF/B-VII.0 evaluation of the 237Np fission cross section by the n_TOF data. We also explore the hypothesis of deficiencies of the inelastic cross section in 235U which has been invoked by some authors to explain the deviation of 750 pcm. With compare to inelastic large distortion calculation, it is incompatible with existing measurements. Also we show that the v of 237Np can hardly be incriminated because of the high accuracy of the existing data. Fission rate ratios or averaged fission cross sections measured in several fast neutron fields seem to give contradictory results on the validation of the 237Np cross section but at least one of the benchmark experiments, where the active deposits have been well calibrated for the number of atoms, favors the n_TOF data set. These outcomes support the hypothesis of a higher fission cross section of 237Np.

  9. Method for Determination of Neptunium in Large-Sized Urine Samples Using Manganese Dioxide Coprecipitation and 242Pu as Yield Tracer

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per

    2013-01-01

    A novel method for bioassay of large volumes of human urine samples using manganese dioxide coprecipitation for preconcentration was developed for rapid determination of 237Np. 242Pu was utilized as a nonisotopic tracer to monitor the chemical yield of 237Np. A sequential injection extraction...... to 100% and high separation capacity of processing up to 5 L of human urine samples. The MnO2 coprecipitation process is simple and straightforward in which a batch (8–12) of samples can be pretreated within 4 h (i.e.,

  10. Rapid and simultaneous determination of neptunium and plutonium isotopes in environmental samples by extraction chromatography using sequential injection analysis and ICP-MS

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per

    2010-01-01

    This paper reports an automated analytical method for rapid and simultaneous determination of plutonium isotopes (239Pu and 240Pu) and neptunium (237Np) in environmental samples. An extraction chromatographic column packed with TrisKem TEVA® resin was incorporated in a sequential injection (SI...

  11. Study on behavior of long-lived radionuclides in soil environment

    Energy Technology Data Exchange (ETDEWEB)

    Morita, Shigemitsu; Watanabe, Hitoshi; Katagiri, Hiromi; Akatsu, Yasuo [Power Reactor and Nuclear Fuel Development Corp., Tokai, Ibaraki (Japan). Tokai Works

    1996-04-01

    Distribution of {sup 99}Tc, {sup 239,240}Pu and {sup 237}Np in soil in Japan was measured. Dependency of concentration on physical and chemical properties of soil was studied. High sensitivity inductively coupled plasma mass spectroscopy was applied to the quantitative analysis of long-lived radionuclides. (J.P.N.)

  12. Sequential injection approach for simultaneous determination of ultratrace plutonium and neptunium in urine with accelerator mass spectrometry.

    Science.gov (United States)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per; Lachner, Johannes; Christl, Marcus; Xu, Yihong

    2013-09-17

    An analytical method was developed for simultaneous determination of ultratrace level plutonium (Pu) and neptunium (Np) using iron hydroxide coprecipitation in combination with automated sequential injection extraction chromatography separation and accelerator mass spectrometry (AMS) measurement. Several experimental parameters affecting the analytical performance were investigated and compared including sample preboiling operation, aging time, amount of coprecipitating reagent, reagent for pH adjustment, sedimentation time, and organic matter decomposition approach. The overall analytical results show that preboiling and aging are important for obtaining high chemical yields for both Pu and Np, which is possibly related to the aggregation and adsorption behavior of organic substances contained in urine. Although the optimal condition for Np and Pu simultaneous determination requires 5-day aging time, an immediate coprecipitation without preboiling and aging could also provide fairly satisfactory chemical yields for both Np and Pu (50-60%) with high sample throughput (4 h/sample). Within the developed method, (242)Pu was exploited as chemical yield tracer for both Pu and Np isotopes. (242)Pu was also used as a spike in the AMS measurement for quantification of (239)Pu and (237)Np concentrations. The results show that, under the optimal experimental condition, the chemical yields of (237)Np and (242)Pu are nearly identical, indicating the high feasibility of (242)Pu as a nonisotopic tracer for (237)Np determination in real urine samples. The analytical method was validated by analysis of a number of urine samples spiked with different levels of (237)Np and (239)Pu. The measured values of (237)Np and (239)Pu by AMS exhibit good agreement (R(2) ≥ 0.955) with the spiked ones confirming the reliability of the proposed method.

  13. Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean

    Energy Technology Data Exchange (ETDEWEB)

    Lindahl, Patric [Department of Radiation Physics, Lund University Hospital, SE-221 85 Lund (Sweden) and Korea Ocean Research and Development Institute, Ansan P.O. Box 29, Seoul 425-600 (Korea, Republic of)]. E-mail: patriclindahl@yahoo.com; Roos, Per [Risoe National Laboratory, P.O. Box 49, DK-4000 Roskilde (Denmark); Holm, Elis [Department of Radiation Physics, Lund University Hospital, SE-221 85 Lund (Sweden); Risoe National Laboratory, P.O. Box 49, DK-4000 Roskilde (Denmark); Dahlgaard, Henning [Risoe National Laboratory, P.O. Box 49, DK-4000 Roskilde (Denmark)

    2005-07-01

    The long-lived anthropogenic radionuclides {sup 237}Np, {sup 239}Pu and {sup 240}Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The {sup 237}Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16 {+-} 0.02 to 1.02 {+-} 0.09 mBq kg{sup -1} (dry weight) and 0.65 {+-} 0.02 to 1.69 {+-} 0.02 mBq m{sup -3}, respectively, depending on the location and sampling year. Most of the {sup 237}Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The {sup 240}Pu/{sup 239}Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17 {+-} 0.03. The {sup 237}Np and {sup 239}Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16 {+-} 0.01 to 0.62 {+-} 0.08 mBq m{sup -3} and from 0.64 {+-} 0.05 to 4.27 {+-} 0.08 mBq m{sup -3}, respectively, and the {sup 237}Np/{sup 239}Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.

  14. Field test of nuclide migration in bentonite-based materials at aerated zone. Cooperative research program on field migration test between CIRP and JAERI

    Energy Technology Data Exchange (ETDEWEB)

    Fan Zhiwen; Cui Anxi; Gu Cunli [China Inst. for Radiation Protection, Taiyuan, Shanxi (China)] [and others

    2002-03-01

    A field test was jointly conducted by China Institute for Radiation Protection (CIRP) and Japan Atomic Energy Research Institute (JAERI) to explore moisture movement with Br{sup -} and migration of radioactive tracer {sup 237}Np, {sup 238}Pu and {sup 90}Sr in bentonite-based materials at aerated zone. The test ran under two rainfall conditions, the artificial rainfall with sprinkling density of 15 mm/d and 5 mm/hr, and the natural rainfall. Tracing test of Br{sup -} implies that there does have water going through the bentonite specimen. However, the curves are very complex and further work need be conducted to quantify this movement. {sup 238}Pu has no observable movement during the test period under either rainfall conditions, and {sup 237}Np has very short movement dominated by diffusion. Bentonite-based materials are effective to retard nuclide migration. (author)

  15. The Geochemical Behaviour of Tc, Np, and Pu in Spent Nuclear Fuel in an Oxidizing Environment

    Energy Technology Data Exchange (ETDEWEB)

    Buck, Edgar C.; Hanson, Brady D.; McNamara, Bruce K.; R. Giere and P. Stille

    2004-10-01

    Studies at the Nopal and Shinkolowbwe uranium deposits show that the primary uraninite (UO2) altered to a suite of secondary uranyl minerals similar to those observed in corrosion tests with uranium oxide . Although the Nopal I deposit tells us something about the possible fate of uranium, it tells us little about the likely fate of the important long-lived radionuclides; iodine (129I), cesium (135Cs), technetium (99Tc), neptunium (237Np), and plutonium (239Pu). Most performance assessment (PA) models, assume conservatively, that as the UO2 matrix corrodes, the key radionuclides (129I, 99Tc, 237Np, and 239Pu) will be released congruently. In so doing, these PA models force increased reliance on human engineered barriers.

  16. Application of off/on line sequential injection system with high resolution ICP-MS to measurement radionuclides in environmental samples

    Energy Technology Data Exchange (ETDEWEB)

    Chang-Kyu Kim (IAEA, Physics, Chemistry and Instrumentation Lab., Agency' s Laboratories, Seibersdorf (Austria))

    2010-03-15

    A sequential injection system was developed, which can be widely used for the separation and preconcentration of analytes from diverse environmental samples. The system enables the separation time to be shortened by maintaining a constant flow rate of solution and by avoiding clogging or bubbling in a chromatographic column. The SI system was successfully applied to the separation of 237Np and Pu isotopes in IAEA reference materials and environmental samples, and to the sequential separation of 210Po and 210Pb in a phosphogypsum candidate reference material. The replicate analysis results of 237Np, 239+240Pu 210Po and 210Pb in some IAEA reference materials using the SI system associated with HR-ICP-MS, alpha-spectrometry and LSC are in good agreement with the recommended value within 5% of standard deviation. The SI system enabled a halving of the separation time required for radionuclides. (author)

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

    CERN Multimedia

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

  18. Magnetic sublattices in Np2Co17 and Np2Ni17

    Science.gov (United States)

    Colineau, E.; Hen, A.; Sanchez, J.-P.; Griveau, J.-C.; Magnani, N.; Eloirdi, R.; Halevy, I.; Gaczyński, P.; Orion, I.; Shick, A. B.; Caciuffo, R.

    2016-12-01

    Rare-earth-based compounds R2T17 (R=Rare earth; T=Transition metal) have been extensively studied and developed for applications as permanent magnets. The actinide-based analogues, however, are much less documented and we report here about the magnetic properties of Np2Co17 and Np2Ni17, as inferred from 237Np Mössbauer spectroscopy, the best resonance in actinides, and specific heat.

  19. Average resonance parameters evaluation for actinides

    Energy Technology Data Exchange (ETDEWEB)

    Porodzinskij, Yu.V.; Sukhovitskij, E.Sh. [Radiation Physics and Chemistry Problems Inst., Minsk-Sosny (Belarus)

    1997-03-01

    New evaluated <{Gamma}{sub n}{sup 0}> and values for {sup 238}U, {sup 237}Np, {sup 243}Cm, {sup 245}Cm, {sup 246}Cm and {sup 241}Am nuclei in the resolved resonance region are presented. The applied method based on the idea that experimental resonance missing results in correlated changes of reduced neutron widths and level spacings distributions is discussed. (author)

  20. Analysis of the evaluated data discrepancies for minor actinides and development of improved evaluation

    Energy Technology Data Exchange (ETDEWEB)

    Ignatyuk, A. [Institute of Physics and Power Engineering, Obninsk (Russian Federation)

    1997-03-01

    The work is directed on a compilation of experimental and evaluated data available for neutron induced reaction cross sections on {sup 237}Np, {sup 241}Am, {sup 242m}Am and {sup 243}Am isotopes, on the analysis of the old data and renormalizations connected with changes of standards and on the comparison of experimental data with theoretical calculation. Main results of the analysis performed by now are presented in this report. (J.P.N.)

  1. Measurements of Fission Cross Sections of Actinides

    CERN Multimedia

    Wiescher, M; Cox, J; Dahlfors, M

    2002-01-01

    A measurement of the neutron induced fission cross sections of $^{237}$Np, $^{241},{243}$Am and of $^{245}$Cm is proposed for the n_TOF neutron beam. Two sets of fission detectors will be used: one based on PPAC counters and another based on a fast ionization chamber (FIC). A total of 5x10$^{18}$ protons are requested for the entire fission measurement campaign.

  2. Modelling of reaction cross sections and prompt neutron emission

    Science.gov (United States)

    Hambsch, F.-J.; Tudora, A.; Oberstedt, S.

    2010-10-01

    Accurate nuclear data concerning reaction cross sections and the emission of prompt fission neutrons (i.e. multiplicity and spectra) as well as other fission fragment data are of great importance for reactor physics design, especially for the new Generation IV nuclear energy systems. During the past years for several actinides (238U(n, f) and 237Np(n, f)) both the reaction cross sections and prompt neutron multiplicities and spectra have been calculated within the frame of the EFNUDAT project.

  3. Moessbauer spectroscopy with actinide elements

    Energy Technology Data Exchange (ETDEWEB)

    Potzel, W.; Moser, J.; Asch, L.; Kalvius, G.M. (Technische Univ. Muenchen, Garching (Germany, F.R.)

    1983-01-01

    Although formally equivalent to the lanthanide (4f) elements, the light actinides show a much more varied behaviour due to the larger spatial extent and ionizability of the 5f electrons. The application of Moessbauer spectroscopy for the determination of electronic properties of the actinides is outlined. Emphasis is put on high pressure Moessbauer experiments using the 60 keV transition in /sup 237/Np to study questions of delocalization of 5f electrons.

  4. Extended X-ray Absorption Fine Spectrometry for Np(Ⅴ) Adsorption to γ-FeOOH/Water Interface

    Institute of Scientific and Technical Information of China (English)

    YANG; Chun-li; ZHANG; Sheng-dong; RAO; Lin-feng

    2013-01-01

    237Np(Ⅴ)is estimated to be the most hazardous radionuclide concerning its half-time(2.14×106year),radiotoxicity and environmental behavior.It has been reported that most of actinides can be sequestered by a variety of minerals,especially iron oxides as common components of rocks,soils and sediments.Np(Ⅴ)sorption at mineral-water interfaces are of great importance in contaminant regulation

  5. Experimental study on neptunium migration under in situ geochemical conditions

    Science.gov (United States)

    Kumata, M.; Vandergraaf, T. T.

    1998-12-01

    Results are reported for migration experiments performed with Np under in situ geochemical conditions over a range of groundwater flow rates in columns of crushed rock in a specially designed facility at the 240-level of the Underground Research Laboratory (URL) near Pinawa, Manitoba, Canada. This laboratory is situated in an intrusive granitic rock formation, the Lac du Bonnet batholith. Highly altered granitic rock and groundwater were obtained from a major subhorizontal fracture zone at a depth of 250 m in the URL. The granite was wet-crushed and wet-sieved with groundwater from this fracture zone. The 180-850-μm size fraction was selected and packed in 20-cm long, 2.54-cm in diameter Teflon™-lined stainless steel columns. Approximately 30-ml vols of groundwater containing 3HHO and 237Np were injected into the columns at flow rates of 0.3, 1, and 3 ml/h, followed by elution with groundwater, obtained from the subhorizontal fracture, at the same flow rates, for a period of 95 days. Elution profiles for 3HHO were obtained, but no 237Np was detected in the eluted groundwater. After terminating the migration experiments, the columns were frozen, the column material was removed and cut into twenty 1-cm thick sections and each section was analyzed by gamma spectrometry. Profiles of 237Np were obtained for the three columns. A one-dimensional transport model was fitted to the 3HHO breakthrough curves to obtain flow parameters for this experiment. These flow parameters were in turn applied to the 237Np concentration profiles in the columns to produce sorption and dispersion coefficients for Np. The results show a strong dependence of retardation factors ( Rf) on flow rate. The decrease in the retarded velocity of the neptunium ( Vn) varied over one order of magnitude under the geochemical conditions for these experiments.

  6. Analysis of the evaluated data discrepancies for minor actinides and development of improved evaluation

    Energy Technology Data Exchange (ETDEWEB)

    Ignatyuk, A. [Institute of Physics and Power Engineering, Obninsk (Russian Federation)

    1997-03-01

    The work is directed on a compilation of experimental and evaluated data available for neutron induced reaction cross sections on {sup 237}Np, {sup 241}Am, {sup 242m}Am and {sup 243}Am isotopes, on the analysis of the old data and renormalizations connected with changes of standards and on the comparison of experimental data with theoretical calculation. Main results of the analysis performed by now are presented in this report. (J.P.N.)

  7. Average resonance parameters evaluation for actinides

    Energy Technology Data Exchange (ETDEWEB)

    Porodzinskij, Yu.V.; Sukhovitskij, E.Sh. [Radiation Physics and Chemistry Problems Inst., Minsk-Sosny (Belarus)

    1997-03-01

    New evaluated <{Gamma}{sub n}{sup 0}> and values for {sup 238}U, {sup 237}Np, {sup 243}Cm, {sup 245}Cm, {sup 246}Cm and {sup 241}Am nuclei in the resolved resonance region are presented. The applied method based on the idea that experimental resonance missing results in correlated changes of reduced neutron widths and level spacings distributions is discussed. (author)

  8. The Study on the Migration of Radionuclides in the Shallow Land

    Energy Technology Data Exchange (ETDEWEB)

    Li, S.; Wang, Z.; Li, Z.; Zhao Y.; Guo, Z.; Guo, L.; Shi, Y.; Ogawa, H.; Maeda, T.; Matsumoto, J.; Mukai, M.; Tanaka, T.

    2002-02-25

    >From 1995 through 2001 a cooperative study project on the migration of radionuclides in shallow land was carried out by CIRP and JAERI, which covers field test, laboratory simulation test, other laboratory studies and related model development. The radionuclides studied involve 90Sr, 237Np, 238Pu. For comparison the nonradioactive elements Sr, Nd and Ce were also studied. The field test was performed both in aerated zone and aquifer zone of loess. In the aerated zone the nuclide migration in engineering materials were also studied. The study in the aerated zone was carried out in 9 pits with the size of 2m x 2m under natural conditions or artificial sprinkling conditions. The study in the aquifer was carried out in a new built Underground Research Facility with the area of 142m2. The test results show that the order of adsorption activity of the nuclide on the loess is 238Pu > 237Np > 90Sr and Nd, Ce > Sr. During the 3 years period of test the migration of 238Pu and Nd, Ce was not observable in both aerated zone and aquifer zone, the nuclide of 237Np migrated a small distance, and the nuclide of 90Sr had a relative large migration. The migration of the nuclides in engineering materials was not detected, which include cement, degraded cement, cement mortar, Chinese bentonite and Japanese bentonite.

  9. Distribution of Np and Pu in Swedish lichen samples (Cladonia stellaris) contaminated by atmospheric fallout

    Energy Technology Data Exchange (ETDEWEB)

    Lindahl, Patric E-mail: patric.lindahl@radfys.lu.se; Roos, Per; Eriksson, Mats; Holm, Elis

    2004-07-01

    The activity concentrations of {sup 237}Np and the two Pu isotopes, {sup 239}Pu and {sup 240}Pu, were determined in lichen samples (Cladonia stellaris) contaminated by fallout from atmospheric nuclear test explosions and the Chernobyl accident. The samples were collected at 18 locations in Sweden, from north to south, between 1986 and 1988 and analysed with high-resolution inductively coupled plasma mass spectrometry (HR-ICP-MS) and alpha spectrometry. Data on the activity ratios {sup 238}Pu/{sup 239+240}Pu and {sup 134}Cs/{sup 137}Cs measured previously were also included in this study for comparison. The {sup 237}Np activity concentration ranged from 0.08{+-}0.01 to 2.08{+-}0.17 mBq kg{sup -1}, depending on the location of the sampling site and time of collection. The {sup 239+240}Pu activity concentration ranged from 0.09{+-}0.01 to 4.09{+-}0.15 Bq kg{sup -1}, with the {sup 240}Pu/{sup 239}Pu atomic ratio ranging between 0.16{+-}0.01 and 0.44{+-}0.03, the higher ratios indicating a combination of weapons test fallout and Chernobyl fallout. The {sup 237}Np/{sup 239}Pu atomic ratios ranged between 0.06{+-}0.01 and 0.42{+-}0.04, the lower ratios indicating combination of weapons test fallout and Chernobyl fallout. At a well-defined sampling site at Lake Rogen (62.32 deg. N, 12.38 deg. E), additional lichen samples were collected between 1987 and 1998 to study the distribution of Np and Pu in different layers. The concentrations of the two elements follow each other quite well in the profile.

  10. Reanalysis of the Gas-cooled fast reactor experiments at the zero power facility Proteus – Spectral indices

    Directory of Open Access Journals (Sweden)

    Girardin G.

    2013-03-01

    Full Text Available PROTEUS is a zero power reactor at the Paul Scherrer Institute which has been employed during the 1970’s to study experimentally the physics of the gas-cooled fast reactor. Reaction rate distributions, flux spectrum and reactivity effects have been measured in several configurations featuring PuO2/UO2 fuel, absorbers, large iron shields, and thorium oxide and thorium metal fuel either distributed quasihomogeneously in the reference PuO2/UO2 lattice or introduced in the form of radial and axial blanket zones. This papers focus on the spectral indices – including fission and capture in 232Th and 237Np - measured in the reference PuO2/UO2 lattices and their predictions with an MCNPX model specially developed for the PROTEUS-GCFR core. Predictions were obtained with JEFF-3.1 and -3.11, ENDF/B-VII.0 and VII.1, and JENDL-3.3 and -4.0. A general good agreement was demonstrated. The ratio of 232Th fission to 239Pu fission, however, was under-predicted by 8.7±2.1% and 6.5±2.1% using ENDF/B-VII.0 and VII.1, respectively. Finally, the capture rates in 237Np tended to be underpredicted by the JEFF and JENDL libraries, although the new cross section in JEFF-3.1.1 slightly improved the 237Np capture to 239Pu fission results (3.4±2.4%.

  11. Fission cross section calculations of actinides with EMPIRE code

    Energy Technology Data Exchange (ETDEWEB)

    Sin, M.; Oblozinsky, P.; Herman,M.; Capote,R.

    2010-04-30

    The cross sections of the neutron induced reactions on {sup 233,234,236}U, {sup 237}Np, {sup 238,242}Pu, {sup 241,243}Am, {sup 242,246}Cm carried out in the energy range 1 keV-20 MeV with EMPIRE code are presented, emphasizing the fission channel. Beside a consistent, accurate set of evaluations, the paper contains arguments supporting the choice of the reaction models and input parameters. A special attention is paid to the fission parameters and their uncertainties.

  12. TANGRA-Setup for the Investigation of Nuclear Fission induced by 14.1 MeV neutrons

    OpenAIRE

    RUSKOV I.; Kopatch, Y; BYSTRITSKY V.; Skoy, V.; SHVETSOV V.; Hambsch, Franz-Josef; Oberstedt, Stephan; CAPOTE NOY R.; Sedyshev, P.; GROZDANOV D.; IVANOV I. Zh.; ALEKSAKHIN V. Yu.; BOGOLUBOV E. P.; BARMAKOV Y.; Khabarov, S. V.

    2015-01-01

    The new experimental setup TANGRA (Tagged Neutrons & Gamma Rays), for the investigation of neutron induced nuclear reactions, e.g. (n,xn’), (n,xn’γ), (n,γ), (n,f), on a number of important isotopes for nuclear science and engineering (235,238U, 237Np, 239Pu, 244,245,248Cm) is under construction and being tested at the Frank Laboratory of Neutron Physics (FLNP) of the Joint Institute for Nuclear Research (JINR) in Dubna. The TANGRA setup consists of: a portable neutron generator ING-27, wit...

  13. Advances in fuel materials for the transmutation of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Prunier, C.

    1994-12-31

    The physical feasibility of actinides, spent fuels and fission products burning in fission reactors is well understood. In fast reactors, this operation is more favourable. The homogeneous recycling mode has had a preliminary validation in Phenix (the Super fact experiment). For the heterogenous recycling mode, past experience for {sup 238} Pu production in thermal spectrum was obtained with Np O{sub 2}-Mg O targets. An irradiation experiment in Phenix blanket is foreseen with the same type of target. The {sup 237} Np problem seems to be most conveniently treated, even in the short term, by homogeneous recycling with Pu in fast reactors. (author). 15 figs., 4 tabs.

  14. Modelling of reaction cross sections and prompt neutron emission

    Directory of Open Access Journals (Sweden)

    Oberstedt S.

    2010-10-01

    Full Text Available Accurate nuclear data concerning reaction cross sections and the emission of prompt fission neutrons (i.e. multiplicity and spectra as well as other fission fragment data are of great importance for reactor physics design, especially for the new Generation IV nuclear energy systems. During the past years for several actinides (238U(n, f and 237Np(n, f both the reaction cross sections and prompt neutron multiplicities and spectra have been calculated within the frame of the EFNUDAT project.

  15. Reactivity worth measurements with Caliban and Silene experimental reactors

    Energy Technology Data Exchange (ETDEWEB)

    Casoli, P.; Authier, N. [CEA Valduc, 21 - Is-sur-Tille (France)

    2008-07-01

    Reactivity worth measurements of material samples put in the central cavities of nuclear reactors allow to test cross section nuclear databases or to extract information about the critical masses of fissile elements. Such experiments have already been completed on the CALIBAN and SILENE experimental reactors operated by the Criticality and Neutronics Research Laboratory of Valduc (Cea, France), using the perturbation measurement technique. Feasibility studies have been performed to prepare future experiments on new materials (beryllium, copper, tantalum, {sup 237}Np) and results show that the obtained values for most materials are clearly above the measurement limits and then the perturbation technique can be used even with smaller size samples.

  16. Speciation of Long-Lived Radionuclides in the Environment

    DEFF Research Database (Denmark)

    Hou, Xiaolin

    , isotopes of Pu, and 237Np in seawater, fresh water, soil, sediment, vegetations, and concrete. The developed methods are used for the investigation of the chemical speciation of these radionuclides as well as their environmental behaviours, especially in Danish environment. In addition the speciation of Pu......This project started in November 2005 and ended in November 2008, the work and research approaches are summarized in this report. This project studied the speciation of radionuclides in environment. A number of speciation analytical methods are developed for determination of species of 129I, 99Tc...

  17. Leaching characteristics of actinides from simulated reactor waste glass

    Energy Technology Data Exchange (ETDEWEB)

    Weed, H.C.; Coles, D.G.; Bradley, D.J.; Mensing, R.W.; Schweiger, J.S.; Rego, J.H.

    1979-08-01

    Even without statistical analysis, some general trends can be seen in the results: leach rate increases with flow rate at high temperature, but is approximately independent of it at room temperature; agreement between the results from the one-pass method and those from the IAEA method are fair in the case of WIPP brine solution, and good in the case of the others; and the /sup 237/Np leach rate increases with temperature, but the /sup 239/Pu leach rate either decreases with temperature or does not change.

  18. Systematics of fission cross sections at the intermediate energy region

    Energy Technology Data Exchange (ETDEWEB)

    Fukahori, Tokio; Chiba, Satoshi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1997-03-01

    The systematics was obtained with fitting experimental data for proton induced fission cross sections of Ag, {sup 181}Ta, {sup 197}Au, {sup 206,207,208}Pb, {sup 209}Bi, {sup 232}Th, {sup 233,235,238}U, {sup 237}Np and {sup 239}Pu above 20 MeV. The low energy cross section of actinoid nuclei is omitted from systematics study, since the cross section has a complicated shape and strongly depends on characteristic of nucleus. The fission cross sections calculated by the systematics are in good agreement with experimental data. (author)

  19. Magnetic sublattices in Np{sub 2}Co{sub 17} and Np{sub 2}Ni{sub 17}

    Energy Technology Data Exchange (ETDEWEB)

    Colineau, E., E-mail: eric.colineau@ec.europa.eu; Hen, A. [Institute for Transuranium Elements (ITU), European Commission, Joint Research Centre (JRC) (Germany); Sanchez, J.-P. [CEA, INAC-SPSMS (France); Griveau, J.-C.; Magnani, N.; Eloirdi, R. [Institute for Transuranium Elements (ITU), European Commission, Joint Research Centre (JRC) (Germany); Halevy, I. [Ben Gurion University, Nuclear Engineering Department (Israel); Gaczyński, P. [Institute for Transuranium Elements (ITU), European Commission, Joint Research Centre (JRC) (Germany); Orion, I. [Ben Gurion University, Nuclear Engineering Department (Israel); Shick, A. B. [Institute of Physics, ASCR (Czech Republic); Caciuffo, R. [Institute for Transuranium Elements (ITU), European Commission, Joint Research Centre (JRC) (Germany)

    2016-12-15

    Rare-earth-based compounds R{sub 2}T{sub 17} (R=Rare earth; T=Transition metal) have been extensively studied and developed for applications as permanent magnets. The actinide-based analogues, however, are much less documented and we report here about the magnetic properties of Np{sub 2}Co{sub 17} and Np{sub 2}Ni{sub 17}, as inferred from {sup 237}Np Mössbauer spectroscopy, the best resonance in actinides, and specific heat.

  20. Photofissility of heavy nuclei at intermediate energies

    Energy Technology Data Exchange (ETDEWEB)

    Deppman, A.; Arruda Neto, J.D.T.; Likhachev, V.P. [Sao Paulo Univ., SP (Brazil). Inst. de Fisica; Tavares, O.A.P.; Duarte, S.B.; Oliveira, E.C. de [Centro Brasileiro de Pesquisas Fisicas (CBPF), Rio de Janeiro, RJ (Brazil); Goncalves, M. [Instituto de Radioprotecao e Dosimetria (IRD), Rio de Janeiro, RJ (Brazil)

    2002-10-01

    We use the recently developed MCMC/MCEF (Multi Collisional Monte Carlo plus Monte Carlo for Evaporation-Fission calculations) model to calculate the photo fissility and the photofission cross section at intermediate energies for the {sup 243} Am and for {sup 209} Bi, and compare them to results obtained for other actinides and to available experimental data. As expected, the results for {sup 243} Am are close to those for {sup 237} Np. The fissility for pre actinide nuclei is nearly one order of magnitude lower than that for the actinides. Both fissility and photofission cross section for {sup 209} Bi are in good agreement with the experimental data. (author)

  1. Fissility of actinide nuclei induced by 60-130 MeV photons; Fissionabilidade de nucleos actnideos induzida por fotons de energia 60-130 MeV

    Energy Technology Data Exchange (ETDEWEB)

    Morcelle, Viviane; Tavares, Odilon A.P

    2004-06-15

    Nuclear fissilities obtained from recent photofission reaction cross section measurements carried out at Saskatchewan Accelerator Laboratory (Saskatoon, Canada) in the energy range 60-130 MeV for {sup 232} Th, {sup 233} U, {sup 235} U, {sup 238} U, and {sup 237} Np nuclei have been analysed in a systematic way. To this aim, a semiempirical approach has been developed based on the quasi-deuteron nuclear photoabsorption model followed by the process of competition between neutron evaporation and fission for the excited nucleus. The study reproduces satisfactorily well the increasing trend of nuclear fissility with parameter Z{sup 2}=A. (author)

  2. Partitioning of protactinium, uranium, thorium and other trace elements between columbite and hydrous silicate melt

    Science.gov (United States)

    Huang, F.; Schmidt, M. W.; Günther, D.; Eikenberg, J.

    2009-12-01

    U-series disequilibria are a unique powerful tool to constrain the time-scales and processes of magmatism in mid-ocean ridge, intra-plate, and convergent margin settings. 235U-231Pa is one of the important parent-daughter pairs (231Pa half life = 33 kyr) because protactinium is normally much more incompatible than U during magmatism and thus the ubiquitously observed 231Pa excess in young igneous rocks most likely reflects melting processes. However, because of the extreme incompatibility of protactinium in most silicate minerals (mineral/meltDPa determined at the permissible Pa doping level of 10 ppm (bulk). Experiments were run in a piston cylinder apparatus at 0.5 GPa and 1115 oC using Pt double capsules with NNO or FMQ as external fO2 buffers. The starting material is a hydrous per-aluminous granitic composition, doped with Pa solution in the Paul Scherrer Institute and also contains other trace elements including U, Th, REE, Zr, Hf, W, Mo, Ti, V, Ge, P, and Sn. Experiments employing an oscillating rather than constant temperature have produced columbite crystals up to 30 μm and large areas of crystal-free water-saturated silicate melts. Columbite/silicate melt partition coefficients of non-radioactive trace elements are presently measured by LA-ICP-MS, and Pa will be added as a next stage. The result will give the oxidation state of Pa at oxygen fugacities of the mantle and crust, and have important implications for the partitioning of Pa between silicate minerals and melt and on our understanding of 231Pa-235U disequilibrium in natural magmatic systems.

  3. U-series disequilibria of trachyandesites from minor volcanic centers in the Central Andes

    Science.gov (United States)

    Huang, Fang; Sørensen, Erik V.; Holm, Paul M.; Zhang, Zhao-Feng; Lundstrom, Craig C.

    2017-10-01

    Young trachyandesite lavas from minor volcanic centers in the Central Andes record the magma differentiation processes at the base of the lower continental crust. Here we report U-series disequilibrium data for the historical lavas from the Andagua Valley in Southern Peru to define the time-scale and processes of magmatism from melting in the mantle wedge to differentiation in the crust. The Andagua lavas show (230Th)/(238U), (231Pa)/(235U), and (226Ra)/(230Th) above unity except for one more evolved lava with 230Th depletion likely owing to fractional crystallization of accessory minerals. The 226Ra excess indicates that the time elapsed since magma emplacement and differentiation in the deep crust is within 8000 years. Based on the correlations of U-series disequilibria with SiO2 content and ratios of incompatible elements, we argue that the Andagua lavas were produced by mixing of fresh mantle-derived magma with felsic melt of earlier emplaced basalts in the deep crust. Because of the lack of sediment in the Chile-Peru trench, there is no direct link of recycled slabs with 230Th and 231Pa excesses in the Andagua lavas. Instead, 230Th and 231Pa excesses are better explained by in-growth melting in the upper mantle followed by magma differentiation in the crust. Such processes also produced the 226Ra excess and the positive correlations among (226Ra)/(230Th), Sr/Th, and Ba/Th in the Andagua lavas. The time-scale of mantle wedge melting should be close to the half-life of 231Pa (ca. 33 ka), while it takes less than a few thousand years for magma differentiation to form intermediate volcanic rocks at a convergent margin.

  4. High-resolution fission cross section of 231Pa. [0. 4 eV to 12 MeV

    Energy Technology Data Exchange (ETDEWEB)

    Plattard, S.; Auchampaugh, G. F.; Hill, N. W.; de Saussure, G.; Perez, R. B.; Harvey, J. A.

    1979-01-01

    The /sup 231/Pa fission cross section was measured with high resolution at OREA from 0.1 to 12 MeV and between 0.4 eV and 10 keV. The data show evidence for fractionated vibrational structures in the threshold region of the fission cross section, and narrow fission resonances above 0.4 eV with an average fission width < GAMMA/sub f/ > = 8 ..mu..eV. 3 figures, 3 tables.

  5. Study for 228Th reduction in thermal reactor with Th-U fuel cycls

    Institute of Scientific and Technical Information of China (English)

    1999-01-01

    By using computercode WIMS/CENDL, the effects of some parameters, core configuration such as fuel element structure, neutron flux and burn-up, are discussed in thispaper.It is shown that high neutron flux, small fuel rod diameter,large volume ratio of coolant to fuel, seed-blank heterogeneous corearrangement and 231Pa chemical separation are necessary for reducing 228Th production in reactor.

  6. Mantle Plume Upwelling Rates: Evidence from U-Series in Young Ocean Island Basalts

    Science.gov (United States)

    Bourdon, B.; Turner, S. P.; Stracke, A.; Saal, A. E.

    2004-12-01

    U-series disequilibria measured in recent lavas at intraplate volcanoes provide a powerful probe to examine the validity of the plume model. U-Th and U-Pa fractionation produced during melting is a function of the melting rate. In turn, this parameter should scale with mantle upwelling velocities. Simply stated, a larger melting rate (larger mantle upwelling velocity) yields smaller Th and Pa excess relative to their parent nuclides. A number of observations supports this approach: (1) there is a negative correlation between 230Th excess and buoyancy fluxes (2) based on new measurements of 231Pa in the Azores, Iceland and the Galapagos and literature data, we show here that there is also a well defined correlation between 231Pa excess and buoyancy flux (3) For Hawaii, Iceland and the Azores, 230Th excess (or 231Pa excess) increases as a function of the distance from the centre of the `hotspot'. These observations suggests that `hotspot' buoyancy fluxes are associated with a greater melt production per unit of time and that the centre of `hotspot' corresponds to a faster mantle upwelling velocity than its periphery. This is therefore in strong support of a model where ocean islands are associated with faster upwelling at depth. However, there is in fact not a simple relationship between melt productivity and upwelling velocities. Notably, the presence of volatiles, of mafic lithologies or of variably enriched peridotitic source could all affect melting rate and hence U-Th-Pa fractionation. We have considered these issues in great detail using a large data base for the Azores islands. While there are clear variations in mantle source composition, they cannot explain the observations of increasing 231Pa/235U ratio with distance from the centre of the Azores hotspot . If we take into account the effect of water in the source of the Azores, it clearly affects the scaling between U-series fractionation and upwelling velocity but not the overall conclusions.

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

    Science.gov (United States)

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

    2015-06-02

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

  8. Stuies of neptunium(V) sorption on montmorillonite, clinoptilolite, quartz and {alpha}-alumina

    Energy Technology Data Exchange (ETDEWEB)

    Bertetti, F.P.; Pabalan, R.T.; Turner, D.R.; Almendarez, M.G. [Southwest Research Institute, San Antonio, TX (United States)

    1996-10-01

    {sup 237}Np is a particular concern to the safety suitability of Yucca Mountain, Nevada, as a geologic repository for high-level nuclear wastes. In this study, montmorillonite, clinoptilolite, quartz, and {alpha}-alumina were reacted with {sup 237}Np-bearing solutions to characterize the sorption behavior of Np(V) on these minerals. Batch experiments were conducted at room temperature (20{plus_minus}2{degrees}C) over a range of conditions in which solution pH, sorbent surface area, initial concentration of N(V), ionic strength, and partial pressure of CO{sub 2} were varied. For all the minerals studied, Np(V) sorption begins at pH values coincident with the start of Np hydrolysis in solution ({approximately}6.5-7). For solutions undersaturated with respect to atmospheric CO{sub 2}, sorption increases continuously with increasing pH. For solutions at equilibrium with atmospheric CO{sub 2}, the {open_quotes}sorption envelope{close_quotes} is coincident with the calculated predominance field (pH {approximately}7-9.5) of the NpO{sub 2}(OH){sup 0}(aq) species, and sorption is inhibited at higher pH where neptunyl carbonate complexes predominate. Modeling of the sorption behavior of Np(V) was performed using a surface complexation-approach (Diffuse-Layer Model).

  9. Analytical method for the determination of Np and Pu in sea water by AMS with respect to the Fukushima accident

    Energy Technology Data Exchange (ETDEWEB)

    Hain, K., E-mail: karin.hain@mytum.de [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Faestermann, T.; Famulok, N.; Fimiani, L.; Gómez-Guzmán, J.M.; Korschinek, G. [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Kortmann, F.; Lierse von Gostomski, Ch. [Radiochemie München, Technische Universität München, Walther-Meißner-Str.3, 85748 Garching (Germany); Ludwig, P. [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Shinonaga, T. [Helmholtz Zentrum München, German Research Center for Environmental Health, Institute of Radiation Protection, Ingolstädter Landstrasse 1, 855764 Neuherberg (Germany)

    2015-10-15

    A chemical separation procedure for plutonium (Pu) and neptunium (Np) was developed using extraction chromatography, mass spectrometry and radiometric analysis to determine their concentrations and isotopic ratios in sea water. {sup 241}Am, which causes isobaric background to {sup 241}Pu in mass spectrometric measurements, was successfully separated from the Pu fraction by this method. Water samples which were spiked with {sup 242}Pu and {sup 237}Np or {sup 239}Np, respectively, were used for chemical yield determination. The chemical yields of Pu and Np, which were determined by alpha and gamma spectrometry at the Radiochemie München (RCM), of more than 85% were obtained. The developed method was applied to analyze the concentration of Pu and Np in the certified reference material, IAEA-443, by Accelerator Mass Spectrometry (AMS) at the Maier–Leibnitz-Laboratory (MLL) to check the applicability of the method to sea water samples. The concentrations of {sup 240}Pu, {sup 241}Pu and {sup 237}Np obtained in this study are in agreement with the certified and literature values within the uncertainties. Due to strong isotopic interference of {sup 239}Pu with {sup 238}U, it was not possible to analyze the concentration of {sup 239}Pu. Some modifications of the chemical separation method to suppress the uranium (U) fraction are under consideration. This method can be used for the analysis of Pu and Np in Pacific Ocean water samples collected after the Fukushima accident.

  10. Safe management of actinides in the nuclear fuel cycle: Role of mineralogy

    Science.gov (United States)

    Ewing, Rodney C.

    2011-02-01

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

  11. EA-MC Neutronic Calculations on IAEA ADS Benchmark 3.2

    Energy Technology Data Exchange (ETDEWEB)

    Dahlfors, Marcus [Uppsala Univ. (Sweden). Dept. of Radiation Sciences; Kadi, Yacine [CERN, Geneva (Switzerland). Emerging Energy Technologies

    2006-01-15

    The neutronics and the transmutation properties of the IAEA ADS benchmark 3.2 setup, the 'Yalina' experiment or ISTC project B-70, have been studied through an extensive amount of 3-D Monte Carlo calculations at CERN. The simulations were performed with the state-of-the-art computer code package EA-MC, developed at CERN. The calculational approach is outlined and the results are presented in accordance with the guidelines given in the benchmark description. A variety of experimental conditions and parameters are examined; three different fuel rod configurations and three types of neutron sources are applied to the system. Reactivity change effects introduced by removal of fuel rods in both central and peripheral positions are also computed. Irradiation samples located in a total of 8 geometrical positions are examined. Calculations of capture reaction rates in {sup 129}I, {sup 237}Np and {sup 243}Am samples and of fission reaction rates in {sup 235}U, {sup 237}Np and {sup 243}Am samples are presented. Simulated neutron flux densities and energy spectra as well as spectral indices inside experimental channels are also given according to benchmark specifications. Two different nuclear data libraries, JAR-95 and JENDL-3.2, are applied for the calculations.

  12. Moessbauer spectroscopy in neptunium compounds

    Energy Technology Data Exchange (ETDEWEB)

    Nakamoto, Tadahiro; Nakada, Masami; Masaki, Nobuyuki; Saeki, Masakatsu [Japan Atomic Energy Research Inst., Tokyo (Japan)

    1997-03-01

    Moessbauer effects are observable in seven elements of actinides from {sup 232}Th to {sup 247}Cm and Moesbauer spectra have been investigated mainly with {sup 237}Np and {sup 238}U for the reasons of availability and cost of materials. This report describes the fundamental characteristics of Moessbauer spectra of {sup 237}Np and the correlation between the isomer shift and the coordination number of Np(V) compounds. The isomer shifts of Np(V) compounds had a tendency to increase as an increase of coordination number and the isomer shifts of Np(V) compounds showed broad distribution as well as those of Np(VI) but {delta} values of the compounds with the same coordination number were distributed in a narrow range. The {delta} values of Np(VI) complexes with O{sub x} donor set suggest that the Np atom in its hydroxide (NpO{sub 2}(OH){center_dot}4H{sub 2}O)might have pentagonal bipyramidal structure and at least, pentagonal and hexagonal bipyramidal structures might coexist in its acetate and benzoate. Really, such coexistence has been demonstrated in its nitrate, (NpO{sub 2}){sub 2}(NO{sub 3}){sub 2}{center_dot}5H{sub 2}O. (M.N.)

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-02-15

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

  14. The influence of source heterogeneity on the U-Th-Pa-Ra disequilibria in post-glacial tholeiites from Iceland

    Science.gov (United States)

    Koornneef, J. M.; Stracke, A.; Bourdon, B.; Grönvold, K.

    2012-06-01

    We investigate the relative influence of mantle upwelling velocity and source heterogeneity on the melting rates recorded by 230Th-238U, 231Pa-235U and 226Ra-230Th disequilibria in post-glacial tholeiites from Iceland's main rift areas. The measured (230Th/238U) ratios range from 1.085 to 1.247, the (231Pa/235U) ratios from 1.333 to 1.925, and the (226Ra/230Th) ratios from 0.801 to 1.218. A general positive correlation between 230Th excesses and distance from the inferred plume centre is consistent with a model of decreasing mantle upwelling velocity with increasing distance from the plume axis. However, the model is not substantiated by the (231Pa/235U) data as the correlation with distance from the plume centre is weak. On the scale of individual eruption centres, the observed U-series are influenced by variations in melt transport time, source porosity, and local variations in mantle upwelling velocity. Broad correlations between (230Th/238U) and (231Pa/235U) and highly incompatible trace element ratios for samples from the Western Volcanic Zone provide, however, evidence for a significant underlying effect of source heterogeneity on the U-series data. Low 230Th and 231Pa excesses in enriched samples from the Western Volcanic Zone with high U/Th, Nb/U and Nb/La indicate that partial melts from an enriched source component, characterised by high melt productivity but low bulk DU/DTh, influence the U-series systematics of the erupted melts. These results re-affirm the presence of comparatively larger abundances of enriched material in the mantle source beneath the South Western Rift of Iceland, which has been suggested based on relationships between highly incompatible element and Pb isotope ratios in Icelandic basalts. Overall, our results highlight the importance of lithological heterogeneity on the melting behaviour of the upper mantle and the composition of oceanic basalts.

  15. Effect of reducing groundwater on the retardation of redox-sensitive radionuclides

    Directory of Open Access Journals (Sweden)

    Rose TP

    2008-12-01

    Full Text Available Abstract Laboratory batch sorption experiments were used to investigate variations in the retardation behavior of redox-sensitive radionuclides. Water-rock compositions were designed to simulate subsurface conditions at the Nevada Test Site (NTS, where a suite of radionuclides were deposited as a result of underground nuclear testing. Experimental redox conditions were controlled by varying the oxygen content inside an enclosed glove box and by adding reductants into the testing solutions. Under atmospheric (oxidizing conditions, radionuclide distribution coefficients varied with the mineralogic composition of the sorbent and the water chemistry. Under reducing conditions, distribution coefficients showed marked increases for 99Tc (from 1.22 at oxidizing to 378 mL/g at mildly reducing conditions and 237Np (an increase from 4.6 to 930 mL/g in devitrified tuff, but much smaller variations in alluvium, carbonate rock, and zeolitic tuff. This effect was particularly important for 99Tc, which tends to be mobile under oxidizing conditions. A review of the literature suggests that iodine sorption should decrease under reducing conditions when I- is the predominant species; this was not consistently observed in batch tests. Overall, sorption of U to alluvium, devitrified tuff, and zeolitic tuff under atmospheric conditions was less than in the glove-box tests. However, the mildly reducing conditions achieved here were not likely to result in substantial U(VI reduction to U(IV. Sorption of Pu was not affected by the decreasing Eh conditions achieved in this study, as the predominant sorbed Pu species in all conditions was expected to be the low-solubility and strongly sorbing Pu(OH4. Depending on the aquifer lithology, the occurrence of reducing conditions along a groundwater flowpath could potentially contribute to the retardation of redox-sensitive radionuclides 99Tc and 237Np, which are commonly identified as long-term dose contributors in the risk

  16. Determination of {sup 236}U and transuranium elements in depleted uranium ammunition by {alpha}-spectrometry and ICP-MS

    Energy Technology Data Exchange (ETDEWEB)

    Desideri, D.; Meli, M.A.; Roselli, C.; Testa, C. [General Chemistry Institute, Urbino University, Urbino (Italy); Boulyga, S.F.; Becker, J.S. [Central Department of Analytical Chemistry, Research Centre Juelich, Juelich (Germany)

    2002-11-01

    It is well known that ammunition containing depleted uranium (DU) was used by NATO during the Balkan conflict. To evaluate the origin of DU (the enrichment of natural uranium or the reprocessing of spent nuclear fuel) it is necessary to directly detect the presence of activation products ({sup 236}U, {sup 239}Pu, {sup 240}Pu, {sup 241}Am, and {sup 237}Np) in the ammunition. In this work the analysis of actinides by {alpha}-spectrometry was compared with that by inductively coupled plasma mass spectrometry (ICP-MS) after selective separation of ultratraces of transuranium elements from the uranium matrix. {sup 242}Pu and {sup 243}Am were added to calculate the chemical yield. Plutonium was separated from uranium by extraction chromatography, using tri-n-octylamine (TNOA), with a decontamination factor higher than 10{sup 6}; after elution plutonium was determined by ICP-MS ({sup 239}Pu and {sup 240}Pu) and {alpha}-spectrometry ({sup 239+240}Pu) after electroplating. The concentration of Pu in two DU penetrator samples was 7 x 10{sup -12} g g{sup -1} and 2 x 10{sup -11} g g{sup -1}. The {sup 240}Pu/{sup 239}Pu isotope ratio in one penetrator sample (0.12{+-}0.04) was significantly lower than the {sup 240}Pu/{sup 239}Pu ratios found in two soil samples from Kosovo (0.35{+-}0.10 and 0.27{+-}0.07). {sup 241}Am was separated by extraction chromatography, using di(2-ethylhexyl)phosphoric acid (HDEHP), with a decontamination factor as high as 10{sup 7}. The concentration of {sup 241}Am in the penetrator samples was 2.7 x 10{sup -14} g g{sup -1} and <9.4 x 10{sup -15} g g{sup -1}. In addition {sup 237}Np was detected at ultratrace levels. In general, ICP-MS and {alpha}-spectrometry results were in good agreement.The presence of anthropogenic radionuclides ({sup 236}U, {sup 239}Pu,{sup 240}Pu, {sup 241}Am, and {sup 237}Np) in the penetrators indicates that at least part of the uranium originated from the reprocessing of nuclear fuel. Because the concentrations of

  17. Determination of (236)U and transuranium elements in depleted uranium ammunition by alpha-spectrometry and ICP-MS.

    Science.gov (United States)

    Desideri, D; Meli, M A; Roselli, C; Testa, C; Boulyga, S F; Becker, J S

    2002-11-01

    It is well known that ammunition containing depleted uranium (DU) was used by NATO during the Balkan conflict. To evaluate the origin of DU (the enrichment of natural uranium or the reprocessing of spent nuclear fuel) it is necessary to directly detect the presence of activation products ((236)U, (239)Pu, (240)Pu, (241)Am, and (237)Np) in the ammunition. In this work the analysis of actinides by alpha-spectrometry was compared with that by inductively coupled plasma mass spectrometry (ICP-MS) after selective separation of ultratraces of transuranium elements from the uranium matrix. (242)Pu and (243)Am were added to calculate the chemical yield. Plutonium was separated from uranium by extraction chromatography, using tri- n-octylamine (TNOA), with a decontamination factor higher than 10(6); after elution plutonium was determined by ICP-MS ((239)Pu and (240)Pu) and alpha-spectrometry ((239+240)Pu) after electroplating. The concentration of Pu in two DU penetrator samples was 7 x 10(-12) g g(-1) and 2 x 10(-11) g g(-1). The (240)Pu/(239)Pu isotope ratio in one penetrator sample (0.12+/-0.04) was significantly lower than the (240)Pu/(239)Pu ratios found in two soil samples from Kosovo (0.35+/-0.10 and 0.27+/-0.07). (241)Am was separated by extraction chromatography, using di(2-ethylhexyl)phosphoric acid (HDEHP), with a decontamination factor as high as 10(7). The concentration of (241)Am in the penetrator samples was 2.7 x 10(-14) g g(-1) and <9.4 x 10(-15) g g(-1). In addition (237)Np was detected at ultratrace levels. In general, ICP-MS and alpha-spectrometry results were in good agreement. The presence of anthropogenic radionuclides ((236)U, (239)Pu,(240)Pu, (241)Am, and (237)Np) in the penetrators indicates that at least part of the uranium originated from the reprocessing of nuclear fuel. Because the concentrations of radionuclides are very low, their radiotoxicological effect is negligible.

  18. Basin-Scale nd Isotope Gradients in South Atlantic Marine Sedimentary Records

    Science.gov (United States)

    Ran, W.; Abouchami, W.; Zahn, R.; Masque, P.

    2012-12-01

    Recent 231Pa/230Th and Nd isotopes studies have suggested a slower and re-configured Meridional Overturning Circulation in the Atlantic (AMOC) during the Last Glacial Maximum (LGM) [1]. We have undertaken a Sr and Nd isotope study on sediment core MD02-2594 (34°43'S, 17°20'E, 2440 m) located in the Cape Basin where nutrient-based proxies - δ13C and Cd/Ca ratios - and low 231Pa/230Th, a tracer of deep water overturning rate, indicate the presence of Southern Component Water (SCW) and a weaker AMOC during the LGM [1]. Samples cover the LGM and Holocene sections of the core previously analysed for Pa/Th [1]. Sr and Nd isotope data were obtained on the bulk sediment as well as on the Fe-Mn oxides leachates and the residual detrital fraction extracted using established sequential leaching procedure. Analyses were performed on a ThermoFisher Triton TIMS at MPIC and Nd isotopes measured as NdO. Our results show that the bulk sediment Nd isotope record is, as expected, overprinted by the Nd isotope composition of the lithogenic fraction and follows closely the 231Pa/230Th record. Sr isotope ratios in Fe-Mn leachates have been used as diagnostic of a seawater origin for the Fe-Mn oxides which should yield modern seawater Sr isotopic composition. Our samples have 87Sr/86Sr ratios similar to or slightly higher than those measured for seawater [2]. The Nd isotope composition of the Fe-Mn leachates show, nevertheless, a distinct signature from both the bulk sediment and the detrital fraction, both of which display systematically less radiogenic Nd isotope ratios throughout the whole record. The seawater ɛNd record exhibits a decreasing trend from the LGM into the Bolling-Allerød and Younger Dryas, prior to stabilizing at a value of about -9 during the Holocene. Covariations between Nd isotope ratios of Fe-Mn leachates and 231Pa/230Th reveal contrasted behaviour during the LGM and the Holocene period: low and nearly constant glacial Pa/Th values are associated with

  19. Current activities and future plans for nuclear data measurements at J-PARC

    Energy Technology Data Exchange (ETDEWEB)

    Kimura, Atsushi; Harada, Hideo; Nakamura, Shoji; Iwamoto, Osamu; Toh, Yosuke; Koizumi, Mitsuo; Kitatani, Fumito; Furutaka, Kazuyoshi [Japan Atomic Energy Agency, Ibaraki (Japan); Igashira, Masayuki; Katabuchi, Tatsuya; Mizumoto, Motoharu [Tokyo Institute of Technology, Research Laboratory for Nuclear Reactors, Tokyo (Japan); Hori, Jun-ichi [Kyoto University, Research Reactor Institute, Osaka (Japan); Kino, Koichi [Hokkaido University, Faculty of Engineering, Sapporo (Japan); Kiyanagi, Yoshiaki [Nagoya University, Graduate School of Engineering, Nagoya (Japan)

    2015-12-15

    In order to improve the data accuracy of neutron-capture cross-sections of minor actinides (MAs) and long-lived fission products (LLFPs), a new experimental instrument named ''Accurate Neutron-Nucleus Reaction measurement Instrument'' (ANNRI) has been constructed in the Materials and Life science experimental Facility (MLF) at the Japan Proton Accelerator Research Complex (J-PARC), and measurements of neutron-capture cross-sections of MAs, LLFPs and some stable isotopes with high-intensity pulsed neutrons have been started. The analyses for {sup 244}Cm, {sup 246}Cm, {sup 241}Am and {sup 237}Np were finished; those for {sup 129}I, {sup 107}Pd, {sup 99}Tc, {sup 93}Zr and some stable isotopes are in progress. These results will give significant contributions in the field of developing innovative nuclear systems. (orig.)

  20. Measurements of fast neutron-induced fission data of Np-237

    Energy Technology Data Exchange (ETDEWEB)

    Win, Than; Saito, Keiichiro; Baba, Mamoru; Iwasaki, Tomohiko; Ibaraki, Masanobu; Miura, Takako; Sanami, Toshiya; Nauchi, Yasushi; Hirakawa, Naohiro [Tohoku Univ., Sendai (Japan). Faculty of Engineering

    1998-03-01

    We have performed the following measurements for {sup 237}Np using the 4.5 MV Dynamitron accelerator of Tohoku University as the pulsed neutron source: (1) Prompt fission neutron spectrum for 0.62 MeV incident neutrons, and (2) Neutron-Induced fission cross-section between 10 and 100 keV. The prompt fission neutron spectrum was measured using TOF method with a heavily shielded NE213 scintillation detector. The Maxwellian temperature T{sub m} derived is 1.28 MeV, which is lower than that of 1.38 MeV in JENDL-3.2. The fission cross sections were measured between 10 - 100 keV. The results are between JENDL-3.2 and ENDF/B-VI. (author)

  1. Neutron-induced cross sections of actinides via the surrogate-reaction method

    Directory of Open Access Journals (Sweden)

    Ducasse Q.

    2013-12-01

    Full Text Available The surrogate-reaction method is an indirect way of determining cross sections for reactions that proceed through a compound nucleus. This technique may enable neutron-induced cross sections to be extracted for short-lived nuclei that otherwise cannot be measured. However, the validity of the surrogate method has to be investigated. In particular, the absence of a compound nucleus formation and the Jπ dependence of the decay probabilities may question the method. In this work we study the reactions 238U(d,p239U, 238U(3He,t238Np, 238U(3He,4He237U as surrogates for neutron-induced reactions on 238U, 237Np and 236U, respectively, for which good quality data exist. The experimental set-up enabled the measurement of fission and gamma-decay probabilities. The first results are hereby presented.

  2. Improved Neutron Capture Cross Section Measurements with the n_TOF Total Absorption Calorimeter

    CERN Document Server

    Mendoza, E; Perkowski, J; Andriamonje, S; Carrapico, C; Moinul, M; Vannini, G; Quesada, J M; Harrisopulos, S; Milazzo, P M; Berthier, B; Lozano, M; Krticka, M; Domingo-Pardo, C; Nolte, R; Chiaveri, E; Saarmento, H; Jericha, E; Ferrari, A; Massimi, C; Giubrone, G; Avrigeanu, V; Martinez, T; Guerrero, C; Andrzejewski, J; Karadimos, D; Mengoni, A; Ganesan, S; Vlachoudis, V; Becares, V; Cortes, G; Variale, V; Losito, H; Calvino, F; Kappeler, F; Gunsing, F; Gramegna, F; Colonna, N; Marrone, S; Pavlik, A; Berthoumieux, E; Paradela, C; Mastinu, P F; Vaz, P; Tassan-Got, L; Kadi, Y; Tarrio, D; Cano-Ott, D; Brugger, M; Wallner, A; Audouin, L; Fernandez-Ordonez, M; Becvar, F; Goncalves, I F; Cerutti, F; Ventura, A; Mosconi, M; Tagliente, G; Duran, I; Casado, A; Ioannides, K; Weiss, C; Mirea, M; Gomez-Hornillos, M B; Vlastou, R; Calviani, M; Lederer, C; Gonzalez-Romero, E; Marganiec, J; Vidriales, J J; Lebbos, E; Leeb, H; Heil, M; Dillmann, I; Tain, J L; Belloni, F

    2011-01-01

    The n\\_TOF collaboration operates a Total Absorption Calorimeter (TAC) {[}1] for measuring neutron capture cross-sections of low-mass and/or radioactive samples. The results obtained with the TAC have led to a substantial improvement of the capture cross sections of (237)Np and (240)Pu {[}2]. The experience acquired during the first measurements has allowed us to optimize the performance of the TAC and to improve the capture signal to background ratio, thus opening the way to more complex and demanding measurements on rare radioactive materials. The new design has been reached by a series of detailed Monte Carlo simulations of complete experiments and dedicated test measurements. The new capture setup will be presented and the main achievements highlighted.

  3. Speciation of long-lived radionuclides in the environment

    Energy Technology Data Exchange (ETDEWEB)

    Xiaolin Hou

    2008-11-15

    This project started in November 2005 and ended in November 2008, the work and research approaches are summarized in this report. This project studied the speciation of radionuclides in environment. A number of speciation analytical methods are developed for determination of species of 129I, 99Tc, isotopes of Pu, and 237Np in seawater, fresh water, soil, sediment, vegetations, and concrete. The developed methods are used for the investigation of the chemical speciation of these radionuclides as well as their environmental behaviours, especially in Danish environment. In addition the speciation of Pu isotopes in waste samples from the decommissioning of Danish nuclear facilities is also investigated. The report summarizes these works completed in this project. Through this research project, a number of research papers have been published in the scientific journals, the research results has also been presented in the Nordic and international conference/meeting and communicated to international colleagues. Some publications are also enclosed to this report. (au)

  4. Fast data acquisition in Moessbauer spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Kalvius, G.M. (Technische Universitaet Muenchen, Garching, Ger.); Potzel, W.; Koch, W.; Forster, A.; Asch, L.; Wagner, F.E.; Halder, N.

    1977-01-01

    Three different gamma-ray detection systems for Moessbauer measurements at count rates above 10/sup 5/ s/sup -1/ are described. The first uses the fast output of an uncooled NaI(Tl) scintillation counter and will still provide energy discrimination at total pulse rates up to 10/sup 6/ s/sup -1/. Count rates up to some 10/sup 7/ s/sup -1/ can be handled by a tin-loaded plastic scintillation detector, but only with very limited energy resolution. For even higher photon intensities, the method of current integration is available. The various techniques are illustrated and compared on the basis of measurements with the Moessbauer resonances in /sup 170/Yb (84 keV), /sup 199/Hg (158 keV) and /sup 237/Np (60 keV).

  5. Pressure-dependent hyperfine interactions in NpAl/sub 2/

    Energy Technology Data Exchange (ETDEWEB)

    Litterst, F.J.; Moser, J.; Potzel, W.; Potzel, U.; Kalvius, G.M.; Asch, L.; Gal, J.; Spirlet, J.C.

    1986-12-01

    /sup 237/Np Moessbauer data of NpAl/sub 2/ are reported for pressures up to 90 kbar in a temperature range from 1.5 K to 77 K. Application of pressure yields a continuous reduction of the Curie temperature T/sub c/, of the saturation hyperfine magnetic field and of the isomer shift indicating an increasing delocalization of 5 f electrons. Severe relaxational broadenings of the magnetic patterns are found especially for high pressures and close to T/sub c/. In part these may be connected with interconfigurational fluctuations but major role play fluctuations within the lowest electronic levels of Np at rates in the range of 1-10 GHz.

  6. Sequential Injection Method for Rapid and Simultaneous Determination of 236U, 237Np, and Pu Isotopes in Seawater

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Steier, Peter;

    2013-01-01

    An automated analytical method implemented in a novel dual-column tandem sequential injection (SI) system was developed for simultaneous determination of 236U, 237Np, 239Pu, and 240Pu in seawater samples. A combination of TEVA and UTEVA extraction chromatography was exploited to separate and purify...... target analytes, whereupon plutonium and neptunium were simultaneously isolated and purified on TEVA, while uranium was collected on UTEVA. The separation behavior of U, Np, and Pu on TEVA–UTEVA columns was investigated in detail in order to achieve high chemical yields and complete purification...... for the radionuclides of interest. 242Pu was used as a chemical yield tracer for both plutonium and neptunium. 238U was quantified in the sample before the separation for deducing the 236U concentration from the measured 236U/238U atomic ratio in the separated uranium target using accelerator mass spectrometry...

  7. The simultaneous neutron and photon interrogation method for fissile and non-fissile element separation in radioactive waste drums

    Energy Technology Data Exchange (ETDEWEB)

    Jallu, F. E-mail: fanny.jallu@cea.fr; Lyoussi, A.; Passard, C.; Payan, E.; Recroix, H.; Nurdin, G.; Buisson, A.; Allano, J

    2000-10-01

    Measuring {alpha}-emitters such as ({sup 234,235,236,238}U, {sup 238,239,240,242,244}Pu, {sup 237}Np, {sup 241,243}Am, ...), in solid radioactive waste allows us to quantify the {alpha}-activity in a drum and then to classify it. The simultaneous photon and neutron interrogation experiment (SIMPHONIE) method dealt with in this paper, combines both active neutron interrogation and induced photofission interrogation techniques simultaneously. Its purpose is to quantify fissile ({sup 235}U, {sup 239,241}Pu, ...) and non-fissile ({sup 236,238}U, {sup 238,240}Pu, ...) elements separately in only one measurement. This paper presents the principle of the method, the experimental setup, and the first experimental results obtained using the DGA/ETCA Linac and MiniLinatron pulsed linear electron accelerators located at Arcueil, France. First studies were carried out with U and Pu bare samples.

  8. Determination of spatial and energy distributions of neutrons in experiments on transmutation of radioactive waste using relativistic protons

    Energy Technology Data Exchange (ETDEWEB)

    Zhuk, I.V.; Lomonosova, E.M.; Boulyga, S.F.; Kievitskaia, A.I.; Rakhno, I.L.; Chigrinov, S.E.; Bradnova, V.; Krivopustov, M.I.; Kulakov, B.A.; Brandt, R.; Ochs, M.; Wan, J.-S

    1999-06-01

    The experiments on transmutation of {sup 129}I and {sup 237}Np using uranium-lead targets surrounded by a paraffin moderator were performed at the Joint Institute for Nuclear Research (JINR, Russia). The targets were irradiated by 1.5 GeV and 7.4 GeV protons at the Synchrophasotron of JINR. In the frame of present work spatial and energy distributions of neutrons on the surface of the paraffin moderator were measured using SSNTD technique. It is shown that measured values of spectral indices do not depend on the energy of incident protons but depend on the target composition. The presence of the uranium insertion softens neutron spectra.

  9. National Low-Level Waste Management Program Radionuclide Report Series

    Energy Technology Data Exchange (ETDEWEB)

    J.P. Adams; M.L. Carboneau; W.E. Allred

    1999-02-01

    The National Low Level Waste Management Program at the Idaho National Engineering and Environmental Laboratory has published a report containing key information about selected radionuclides that are most likely to contribute significantly to the radiation exposures estimated from a performance assessment of a low-level radioactive waste (LLW) disposal facility. The information includes physical and chemical characteristics, production means, waste forms, behavior of the radionuclide in soils, plants, groundwater, and air, and biological effects in animals and humans. The radionuclides included in this study comprise all of the nuclides specifically listed in 10CFR61.55, Tables 1 and 2, 3 H, 14 C, 59 Ni, 60 Co, 63 Ni, 90 Sr, 94 Nb, 99 Tc, 129 I, 137 Cs, 241 Pu, and 242 Cm. Other key radionuclides addressed in the report include 237 Np, 238 U, 239 Pu, and 241 Am. This paper summarizes key information contained within this report.

  10. National Low-Level Waste Management Program Radionuclide Report Series

    Energy Technology Data Exchange (ETDEWEB)

    Adams, James Paul; Carboneau, Michael Leonard; Allred, William Edgar

    1999-03-01

    The National Low Level Waste Management Program at the Idaho National Engineering and Environmental Laboratory has published a report containing key information about selected radionuclides that are most likely to contribute significantly to the radiation exposures estimated from a performance assessment of a low-level radioactive waste (LLW) disposal facility. The information includes physical and chemical characteristics, production means, waste forms, behavior of the radionuclide in soils, plants, groundwater, and air, and biological effects in animals and humans. The radionuclides included in this study comprise all of the nuclides specifically listed in 10CFR61.55, Tables 1 and 2, 3 H, 14 C, 59 Ni, 60 Co, 63 Ni, 90 Sr, 94 Nb, 99 Tc, 129 I, 137 Cs, 241 Pu, and 242 Cm. Other key radionuclides addressed in the report include 237 Np, 238 U, 239 Pu, and 241 Am. This paper summarizes key information contained within this report.

  11. Energetic identification of ions of very low fluence; Identificacion energetica de iones de muy baja fluencia

    Energy Technology Data Exchange (ETDEWEB)

    Mut C, D.A.; Balcazar, M. [ININ, 52045 Ocoyoacac, Estado de Mexico (Mexico)

    2005-07-01

    The calibration of 2 types of plastics is presented (cellulose nitrate and polycarbonate) that detect and identify the energy of helium slight ions (1.5 to 10 MeV) and protons (0.3 to 6 MeV) in flows so low of a single particle /cm{sup 2}. This methodology is of importance in radiological protection to identify the actinides {sup 232} Th, {sup 241} Am, {sup 238} U, {sup 235} U, {sup 237} Np by means of its alpha emissions, or to carry out neutron spectroscopy in an ignored energy field by protons retrocession. The ion identification is adjusted for all the cases to a simple expression of the exponential type. The comparison is achieved among detection efficiencies for the detectors. (Author)

  12. Intermediate mass fragment production in the proton-induced reactions of heavy targets

    CERN Document Server

    Deppman, A; Guimaraes, V; Karapetyan, G S; Balabekyan, A R; Demekhina, N A; Adam, J

    2013-01-01

    The production of intermediate-mass fragments (IMFs) formed in the proton-induced reaction with $^{238}$U and $^{237}$Np at 660 MeV was measured in the LNP Phasotron and in U-400M Cyclotron, Joint Institute for Nuclear Research (JINR), Dubna, Russia. We have applied the induced-activation method in off-line analysis. A total of 115 isotopes of all elements in the range $7 \\leq A \\leq 69$ were unambiguously identified with high precision. There is a consideration that the formed nuclides could be produced in a very asymmetric binary decay of heavy nuclei originating from the spallation of heavy targets. Mass-yield distributions were derived from the data, and were compared with the the simulation code CRISP for multi modal fission.

  13. Transmutation studies using SSNTD and radiochemistry and the associated production of secondary neutrons

    CERN Document Server

    Brandt, R; Wan, J S; Schmidt, T; Langrock, E J; Vater, P; Adam, J; Bamblevski, V P; Bradnova, V; Gelovani, L K; Kalinnikov, V K; Krivopustov, M I; Kulakov, B A; Sosnin, A N; Perelygin, V P; Pronskikh, V S; Stegailov, V I; Tsoupko-Sitnikov, V M; Modolo, G; Odoj, R; Philippen, P W; Adloff, J C; Pape, F; Debeauvais, M; Zamani-Valassiadou, M; Hashemi-Nezhad, S R; Dwivedi, K K; Guo Shi Lun; Li, L; Wang, Y L; Wilson, B

    1999-01-01

    Experiments using 1.5 GeV, 3.7 GeV and 7.4 GeV protons from the Synchrophasotron, LHE, JINR, Dubna, Russia, on extended Pb- and U- targets were carried out using SSNTD and radiochemical sensors for the study of secondary neutron $9 fluences. We also carried out first transmutation studies on the long-lived radwaste nuclei /sup 129/I and /sup 237/Np. In addition, we carried out computer code simulation studies on these systems using LAHET and DCM/CEM codes. We $9 have difficulties to understand rather large transmutation rates observed experimentally when they are compared with computer simulations. There seems to be a rather fundamental problem understanding the large transmutation rates as $9 observed experimentally in Dubna and CERN, as compared to those theoretical computer simulations mentioned above. (10 refs).

  14. Level density and gamma-ray strength function in the odd-odd 238Np

    CERN Document Server

    Tornyi, Tamás Gábor; Eriksen, Tomas Kvalheim; Görgen, Andreas; Giacoppo, Francesca; Hagen, Trine Wiborg; Krasznahorkay, Attila; Larsen, Ann-Cecilie; Renstrøm, Therese; Rose, Sunniva Johanne; Siem, Sunniva; Tveten, Gry Merete

    2014-01-01

    The level density and gamma-ray strength function in the quasi-continuum of 238Np has been measured using the Oslo method. The level density function follows closely the constant-temperature level density formula and reaches 43 million levels per MeV at Sn = 5.488 MeV of excitation energy. The gamma-ray strength function displays a two-humped resonance at low-energy as also seen in previous investigations of Th, Pa and U isotopes. The structure is interpreted as the scissors resonance and has an average centroid of wSR = 2.26(5) MeV and a total strength of BSR = 10.8(12)m2N, which is in excellent agreement with sum-rule estimates. The scissors resonance is shown to have an impact on the 237Np(n; g)238Np cross section.

  15. Measurements of thermal fission and capture cross sections of minor actinides within the Mini-INCA project

    Energy Technology Data Exchange (ETDEWEB)

    Bringer, O.; Chabod, S.; Dupont, E.; Letourneau, A.; Panebianco, S.; Veyssiere, Ch. [CEA Saclay, Dept. d' Astrophysique de Physique des Particules, de Physique Nucleaire et de l' Instrumentation Associee, 91- Gif sur Yvette (France); Oriol, L. [CEA Cadarache, Dept. d' Etudes des Reacteurs, 13 - Saint Paul lez Durance (France); Chartier, F. [CEA Saclay, Dept. de Physico-Chimie, 91 - Gif sur Yvette (France); Mutti, P. [Institut Laue Langevin, 38 - Grenoble, (France); AlMahamid, I. [Wadsworth Center, New York State Dept. of Health, Albany, NY (United States)

    2008-07-01

    In the framework of nuclear waste transmutation studies, the Mini-INCA project has been initiated at Cea/DSM to determine optimal conditions for transmutation and incineration of Minor Actinides in high intensity neutron fluxes in the thermal region. Our experimental tool is based on alpha- and gamma-spectroscopy of irradiated samples and microscopic fission-chambers. It can provide both microscopic information on nuclear reactions (total and partial cross sections for neutron capture and/or fission reactions) and macroscopic information on transmutation and incineration potentials. The {sup 232}Th, {sup 237}Np, {sup 241}Am, and {sup 244}Cm transmutation chains have been explored in details, showing some discrepancies in comparison with evaluated data libraries but in overall good agreement with recent experimental data. (authors)

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

    Energy Technology Data Exchange (ETDEWEB)

    Bringer, O

    2007-10-15

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

  17. Study on the properties of saline HLLW in China

    Institute of Scientific and Technical Information of China (English)

    LiangJun-Fu; TianGuo-Xing; 等

    1997-01-01

    The properties and the component of HLLW(High Level Liquid Waste)were studied.The senuine saline HLLW is a blue-green liquid without any deposition.Its density and acidity are 1.399 g/ml(23±1℃) and 2.1 mol/L NHO3,respectively.The activities of 137Cs, 90Sr,99Tc,237Np,239Pu,241Am,total α,totalβ,totalγ are determined.The extractabilities of actinides in the genuine HLLW were examined with a five-stage cross extraction experiment.More than 98% of Pu is in Pu4+ species,and more than 70% of Np is in Np4+ species.More than 99.97% α-nuclides could be extracted by 30% TRPO-Kerosene in 1mol/L NHO3 from the HLLW.

  18. Critical comparison of radiometric and mass spectrometric methods for the determination of radionuclides in environmental, biological and nuclear waste samples.

    Science.gov (United States)

    Hou, Xiaolin; Roos, Per

    2008-02-11

    The radiometric methods, alpha (alpha)-, beta (beta)-, gamma (gamma)-spectrometry, and mass spectrometric methods, inductively coupled plasma mass spectrometry, accelerator mass spectrometry, thermal ionization mass spectrometry, resonance ionization mass spectrometry, secondary ion mass spectrometry, and glow discharge mass spectrometry are reviewed for the determination of radionuclides. These methods are critically compared for the determination of long-lived radionuclides important for radiation protection, decommissioning of nuclear facilities, repository of nuclear waste, tracer application in the environmental and biological researches, these radionuclides include (3)H, (14)C, (36)Cl, (41)Ca, (59,63)Ni, (89,90)Sr, (99)Tc, (129)I, (135,137)Cs, (210)Pb, (226,228)Ra, (237)Np, (241)Am, and isotopes of thorium, uranium and plutonium. The application of on-line methods (flow injection/sequential injection) for separation of radionuclides and automated determination of radionuclides is also discussed.

  19. Leaching tests of simulated Cogema bituminized waste form

    Energy Technology Data Exchange (ETDEWEB)

    Nakayama, S.; Akimoto, T.; Iida, Y.; Nagano, T. [Japan Atomic Energy Research Institute, Tokai, Ibaraki (Japan)

    2000-07-01

    The leaching behavior of COGEMA-type bituminized radioactive waste was studied for the atmospheric and anaerobic conditions. Active and inactive laboratory-scale bitumen samples, including two major salts of NaNO{sub 3} and BaSO{sub 4}, were contacted with deionized water, an alkaline solution (0.01 mol/L Ca(OH){sub 2} or 0.03 mol/L KOH), or a saline solution (0.5 mol/L KCl). It was found that the release of salt was reduced in the Ca(OH){sub 2} solution compared with deionized water under the atmospheric conditions. No significant difference in the concentrations of {sup 237}Np in leachants contacted with the samples for 7 days was observed between the atmospheric and the anaerobic conditions. (authors)

  20. Neutron-induced cross sections of actinides via the surrogate-reaction method

    Directory of Open Access Journals (Sweden)

    Tveten G. M.

    2013-03-01

    Full Text Available The surrogate-reaction method is an indirect way of determining cross sections for reactions that proceed through a compound nucleus. This technique may enable neutron-induced cross sections to be extracted for short-lived nuclei that otherwise cannot be measured. However, the validity of the surrogate method for extracting capture cross sections has to be investigated. In this work we study the reactions 238U(d,p239U, 238U(3He,t238Np, 238U(3He,4He237U as surrogates for neutroninduced reactions on 238U, 237Np and 236U, respectively, for which good quality data exist. The experimental set-up enabled the measurement of fission and gamma-decay probabilities. First results are presented and discussed.

  1. Some results from the second iteration of total-system performance assessment for Yucca Mountain

    Energy Technology Data Exchange (ETDEWEB)

    Wilson, M.L. [Sandia National Labs., Albuquerque, NM (United States)

    1994-12-31

    The second preliminary total-system performance assessment for the potential radioactive-waste-repository site at Yucca Mountain has recently been completed. This paper summarizes results for nominal aqueous and gaseous releases using the composite-porosity flow model. The results are found to be sensitive to the type of unsaturated-zone flow, to percolation flux and climate change, to saturated-zone dilution, to container-wetting processes and container-corrosion processes, to fuel-matrix alteration rate and radionuclide solubilities (especially for {sup 237}Np), and to bulk permeability and retardation of gases {sup 14}C. There are areas that should be given priority in the site-characterization program. Specific recommendations are given in the full report of the study.

  2. Photon and proton induced fission on heavy nuclei at intermediate energies

    Directory of Open Access Journals (Sweden)

    Andrade-II E.

    2014-04-01

    Full Text Available We present an analysis of fission induced by intermediate energy protons or photons on actinides. The 660 MeV proton induced reactions are on 241Am, 238U, and 237Np targets and the Bremmstrahlung-photons with end-point energies at 50 MeV and 3500 MeV are on 232Th and 238U targets. The study was performed by means of the Monte Carlo simulation code CRISP. A multimodal fission extension was added to the code within an approach which accounts for the contribution of symmetric and asymmetric fission. This procedure allowed the investigation of fission cross sections, fissility, number of evaporated nucleons and fission-fragment charge distributions. The comparison with experimental data show a good agreement between calculations and experiments.

  3. Single-pass continuous-flow leach test of PNL 76-68 glass: some selected Bead Leach I results

    Energy Technology Data Exchange (ETDEWEB)

    Coles, D.G.

    1981-08-20

    A single-pass continuous-flow leach test of PNL 76-68 glass beads (7 mm dia) was concluded after 420 days of uninterrupted operation. Variables included in the experimental matrix were flow-rate, leachant composition, and temperature. Analysis was conducted on all leachate samples for /sup 237/Np and /sup 239/Pu as well as a number of nonradioactive elements. Results indicated that flow-rate and leachant systematically affected the leach rate, but only slightly. Temperature effects were significant. Plutonium leach rate was lower at higher temperature suggesting that Pu sorption onto the beads was enhanced at the higher temperature. The range of leach rates for all analyzed elements (except Pu), at both temperatures, at all three flow rates, and with all three leachant compositions varied over only three orders of magnitude. The range of variables used in this experiment covered those expected in many proposed repository environments.

  4. Neptunium(V) sorption behavior on clinoptilolite, quartz and montmorillonite

    Energy Technology Data Exchange (ETDEWEB)

    Bertetti, F.P.; Pabalan, R.T.; Turner, D.R.; Almendarez, M.G. [Southwest Research Inst., San Antonio, TX (United States). Center for Nuclear Waste Regulatory Analyses

    1996-08-01

    Performance assessment models have identified {sup 237}Np as a radionuclide of concern in meeting release limits established for the geologic disposal of high-level nuclear waste at the proposed repository at Yucca Mountain, Nevada. In this study, quartz, clinoptilolite, and montmorillonite, which are minerals representative of phases that occur both in the rock matrix and as fracture coatings at Yucca Mountain, were reacted with {sup 237}Np-bearing solutions to characterize the sorption behavior of Np(V) on these minerals. Batch experiments were conducted over a wide range of conditions in which pH of solution, surface loading, sorbent surface area, initial concentration of Np(V), and partial pressure of CO{sub 2} were varied. Initial Np(V) concentrations were between 1 {times} 10{sup {minus}7} and 1 {times} 10{sup {minus}6} M in electrolyte solutions of 0.1 or 0.01 M NaNO{sub 3}. The oxidation state of Np in solution was verified with NIR spectroscopy and by solvent extraction. Prior to the start of experiments, minerals were pretreated to eliminate impurities, and the clinoptilolite and montmorillonite were converted to Na-form by ion exchange with NaCl solutions. Results indicate that, for all three minerals, Np(V) sorption begins at pH values coincident with the start of hydrolysis in solution ({approximately}7). For solutions undersaturated with respect to atmospheric CO{sub 2}, sorption increases continuously with increasing pH. Under equilibrium with atmospheric CO{sub 2}, Np(V) sorption is important in the pH range (7--9.5) where NpO{sub 2}(OH){sup 0}(aq) is significant, whereas sorption is inhibited at higher pH where neptunyl carbonate complexes are the predominant species.

  5. Critical role of water content in the formation and reactivity of uranium, neptunium, and plutonium iodates under hydrothermal conditions: implications for the oxidative dissolution of spent nuclear fuel.

    Science.gov (United States)

    Bray, Travis H; Ling, Jie; Choi, Eun Sang; Brooks, James S; Beitz, James V; Sykora, Richard E; Haire, Richard G; Stanbury, David M; Albrecht-Schmitt, Thomas E

    2007-04-30

    The reactions of 237NpO2 with excess iodate under acidic hydrothermal conditions result in the isolation of the neptunium(IV), neptunium(V), and neptunium(VI) iodates, Np(IO3)4, Np(IO3)4.nH2O.nHIO3, NpO2(IO3), NpO2(IO3)2(H2O), and NpO2(IO3)2.H2O, depending on both the pH and the amount of water present in the reactions. Reactions with less water and lower pH favor reduced products. Although the initial redox processes involved in the reactions between 237NpO2 or 242PuO2 and iodate are similar, the low solubility of Pu(IO3)4 dominates product formation in plutonium iodate reactions to a much greater extent than does Np(IO3)4 in the neptunium iodate system. UO2 reacts with iodate under these conditions to yield uranium(VI) iodates solely. The isotypic structures of the actinide(IV) iodates, An(IO3)4 (An=Np, Pu), are reported and consist of one-dimensional chains of dodecahedral An(IV) cations bridged by iodate anions. The structure of Np(IO3)4.nH2O.nHIO3 is constructed from NpO9 tricapped-trigonal prisms that are bridged by iodate into a polar three-dimensional framework structure. Second-harmonic-generation measurements on a polycrystalline sample of the Th analogue of Np(IO3)4.nH2O.nHIO3 reveal a response of approximately 12x that of alpha-SiO2. Single-crystal magnetic susceptibility measurements of Np(IO3)4 show magnetically isolated Np(IV) ions.

  6. Effect of Reducing Groundwater on the Retardation of Redox-Sensitive Radionuclides

    Energy Technology Data Exchange (ETDEWEB)

    Hu, Q; Zavarin, M; Rose, T P

    2008-04-21

    Laboratory batch sorption experiments were used to investigate variations in the retardation behavior of redox-sensitive radionuclides. Water-rock compositions used during these experiments were designed to simulate subsurface conditions at the Nevada Test Site (NTS), where a suite of radionuclides were deposited as a result of underground nuclear testing. Experimental redox conditions were controlled by varying the oxygen content inside an enclosed glove box and by adding reductants into the testing solutions. Under atmospheric (oxidizing) conditions, the radionuclide distribution coefficients varied with the mineralogical composition of the sorbent and the water chemistry. Under reducing conditions, distribution coefficients showed marked increases for {sup 99}Tc and {sup 237}Np in devitrified tuff, but much smaller variations in alluvium, carbonate rock, and zeolitic tuff. This effect was particularly important for {sup 99}Tc, which tends to be mobile under oxidizing conditions. Unlike other redox-sensitive radionuclides, iodine sorption may decrease under reducing conditions when I{sup -} is the predominant species. Overall, sorption of U to alluvium, devitrified tuff, and zeolitic tuff under atmospheric conditions was less than in the glove-box tests. However, the mildly reducing conditions achieved here were not likely to result in substantial U(VI) reduction to U(IV). Sorption of Pu was not affected by the decreasing redox conditions achieved in this study, as the predominant sorbed Pu species in all conditions was expected to be the low-solubility and strongly sorbing Pu(OH){sub 4}. Depending on the aquifer lithology, the occurrence of reducing conditions along a groundwater flowpath could potentially contribute to the retardation of redox-sensitive radionuclides {sup 99}Tc and {sup 237}Np, which are commonly identified as long-term dose contributors in the risk assessment in various nuclear facilities.

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

    Energy Technology Data Exchange (ETDEWEB)

    G. S. Chang; Hongbin Zhang

    2009-09-01

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

  8. Determination of Neptunium, Americium and Curium in Spent Nuclear Fuel Samples by Alpha Spectrometry Using {sup 239}Np and {sup 243}Am as a Spike and a Tracer

    Energy Technology Data Exchange (ETDEWEB)

    Jeo, Kih-Soo; Song, Byung-Chul; Kim, Young-Bok; Han, Sun-Ho; Jeon, Young-Shin; Jung, Euo-Chang; Jee, Kwang-Yong [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

    2007-07-01

    Determination of actinide elements and fission products in spent nuclear fuels is of importance for a burnup determination and source term evaluation. Especially, the amounts of uranium and plutonium isotopes are used for the evaluation of a burnup credit in spent nuclear fuels. Additionally, other actinides such as Np, Am and Cm in spent nuclear fuel samples is also required for the purposes mentioned above. In this study, {sup 237}Np, {sup 241}Am and {sup 244}Cm were determined by an alpha spectrometry for the source term data for high burnup spent nuclear fuels ranging from 37 to 62.9 GWD/MtU as a burnup. Generally, mass spectrometry has been known as the most powerful method for isotope determinations such as high concentrations of uranium and plutonium. However, in the case of minor actinides such as Np, Am and Cm, alpha spectrometry would be recommended instead. Determination of the transuranic elements in spent nuclear fuel samples is different from that for environmental samples because the amount of each nuclide in the spent fuel samples is higher and the relative ratios between each nuclide are also different from those for environmental samples. So, it is important to select an appropriate tracer and an optimum sample size depending on the nuclides and analytical method. In this study {sup 237}Np was determined by an isotope dilution alpha(gamma) spectrometry using {sup 239}Np as a spike, and {sup 241}Am and curium isotopes were determined by alpha spectrometry using {sup 243}Am as a tracer. The content of each nuclide was compared with that by the Origen-2 code.

  9. Preconceptual Feasibility Study to Evaluate Alternative Means to Produce Plutonium-238

    Energy Technology Data Exchange (ETDEWEB)

    John D. Bess; Matthew S. Everson

    2013-02-01

    There is currently no large-scale production of 238Pu in the United States. Feasibility studies were performed at the Idaho National Laboratory to assess the capability of developing alternative 238Pu production strategies. Initial investigations indicate potential capability to provision radioisotope-powered systems for future space exploration endeavors. For the short term production of 238Pu, sealed canisters of dilute 237Np solution in nitric acid could be irradiated in the Advanced Test Reactor (ATR). Targets in the large and medium “I” positions of the ATR were irradiated over a simulated period of 306 days and analyzed using MCNP5 and ORIGEN2.2. Approximately 0.5 kg of 238Pu could be produced annually in the ATR with purity greater than 92%. Optimization of the irradiation cycles could further increase the purity to greater than 98%. Whereas the typical purity of space batteries is between 80 to 85%, the higher purity 238Pu produced in the ATR could be blended with existing lower-purity inventory to produce useable material. Development of irradiation methods in the ATR provides the fastest alterative to restart United States 238Pu production. The analysis of 238Pu production in the ATR provides the technical basis for production using TRIGA® (Training, Research, Isotopes, General Atomics) nuclear reactors. Preliminary analyses envisage a production rate of approximately 0.7 kg annually using a single dedicated 5-MW TRIGA reactor with continuous flow loops to achieve high purity product. Two TRIGA reactors represent a robust means of providing at over 1 kg/yr of 238Pu annually using dilute solution targets of 237Np in nitric acid. Further collaboration and optimization of reactor design, radiochemical methods, and systems analyses would further increase annual 238Pu throughput, while reducing the currently evaluated reactor requirements.

  10. Electron spin resonance (ESR) dating of hominid-bearing deposits in the Caverna delle Fate, Ligure, Italy

    Science.gov (United States)

    Falgueres, Christophe; Yokoyama, Yuji; Bibron, Roland

    1990-07-01

    Stalagmitic floors interstratified with Mousterian deposits from the Caverna delle Fate (Italy) have been dated by the electron spin resonance (ESR) method. Three samples dated fall between 60,000 and 74,000 yr and indicate the age of the Mousterian deposits. They are in good agreement with ages determined by nondestructive γ-ray spectrometry of the human remains from 231Pa/ 235U and 230Th /234U ratios, which are, respectively, 75,000 -14,000+21,000 and 82,000 -25,000+36,000 yr. These dates are consistent with the morphological characteristics of the bones as Neanderthal remains.

  11. Changes in the geometry and strength of the Atlantic meridional overturning circulation during the last glacial (20-50 ka)

    Science.gov (United States)

    Burckel, Pierre; Waelbroeck, Claire; Luo, Yiming; Roche, Didier M.; Pichat, Sylvain; Jaccard, Samuel L.; Gherardi, Jeanne; Govin, Aline; Lippold, Jörg; Thil, François

    2016-11-01

    We reconstruct the geometry and strength of the Atlantic meridional overturning circulation during the Heinrich stadial 2 and three Greenland interstadials of the 20-50 ka period based on the comparison of new and published sedimentary 231Pa / 230Th data with simulated sedimentary 231Pa / 230Th. We show that the deep Atlantic circulation during these interstadials was very different from that of the Holocene. Northern-sourced waters likely circulated above 2500 m depth, with a flow rate lower than that of the present-day North Atlantic deep water (NADW). Southern-sourced deep waters most probably flowed northwards below 4000 m depth into the North Atlantic basin and then southwards as a return flow between 2500 and 4000 m depth. The flow rate of this southern-sourced deep water was likely larger than that of the modern Antarctic bottom water (AABW). Our results further show that during Heinrich stadial 2, the deep Atlantic was probably directly affected by a southern-sourced water mass below 2500 m depth, while a slow, southward-flowing water mass originating from the North Atlantic likely influenced depths between 1500 and 2500 m down to the equator.

  12. MA Transmutation Strategy%MA嬗变策略研究

    Institute of Scientific and Technical Information of China (English)

    左国平; 柯国土; 龚学余

    2011-01-01

    According to the development plan envisagement for nuclear power plant in China, the development of China's nuclear power in the next decades is predicted with the. nuclear fuel cycle software NFCSS provided by IAEA. The amounts of the spent fuel generated and accumulated by the year of 2050 are analyzed. According to the assumption model, the accumulated spent fuel by the year of 2050 will reach at 54791t including 57.89t Minor Actinides (MA) (237Np, 42.91t; Am, ll.17t; Cm, 3.81t) and 2778t FP. One group effective cross section of MA in the thermal, well thermalized, and fast neutron field is calculated based on ENDF/B-VII nuclear evaluation database. The transmutation way for three main MA, i.e. 237Np, 241Am, and 246Cm is also analyzed. It is more suitable for 237Np transmutation in well thermalized neutron field and for 241Am, the high flux thermalized neutron field is better. But it is difficult for 246Cm transmutation in thermal or fast neutron field due to its little fission cross section. Its transmutation ability can be improved if transmutation occurs in a high fluxes resonance energy area. The two-stage transmutation strategy is presented according to their characteristics in the thermal, well thermalized, and fast neutron field. Based on the two stage transmutation concept, the transmutation is performed in a well thermalized neutron field first. Small amount of residual of the first stage transmutation is transmuted in a thermal field with a spectrum. It is expected to achieve a good result.%根据中国核电发展战略,采用国际原子能机构(IAEA)的核燃料循环软件NFCSS,对未来中国核电发展情景进行了预测,分析了2050年以前中国乏燃料的产生和累积情况.采用NJOY和ENDF/B-VII数据库,计算分析了次锕系核素在热谱、超热谱和快谱中的一群等效截面,分析了研237Np、241Am、246Cm等主要次锕系核素的可能嬗变途径,提出了两阶段嬗变MA策略.即将从压水堆中分离出来

  13. Uranium in the Nuclear Fuel Cycle: Creation of Plutonium (Invited)

    Science.gov (United States)

    Ewing, R. C.

    2009-12-01

    One of the important properties of uranium is that it can be used to “breed” higher actinides, particularly plutonium. During the past sixty years, more than 1,800 metric tonnes of Pu, and substantial quantities of the “minor” actinides, such as Np, Am and Cm, have been generated in nuclear reactors - a permanent record of nuclear power. Some of these transuranium elements can be a source of energy in fission reactions (e.g., 239Pu), a source of fissile material for nuclear weapons (e.g., 239Pu and 237Np), and of environmental concern because of their long-half lives and radiotoxicity (e.g., 239Pu and 237Np). In fact, the new strategies of the Advance Fuel Cycle Initiative (AFCI) are, in part, motivated by an effort to mitigate some of the challenges of the disposal of these long-lived actinides. There are two basic strategies for the disposition of these heavy elements: 1.) to “burn” or transmute the actinides using nuclear reactors or accelerators; 2.) to “sequester” the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, such as zircon or isometric pyrochlore, A2B2O7 (A= rare earths; B = Ti, Zr, Sn, Hf), for the immobilization of actinides, particularly plutonium, both as inert matrix fuels and nuclear waste forms. Systematic studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high doses of alpha-decay event damage1. The radiation stability of these compositions is closely related to the structural distortions that can be accommodated for specific pyrochlore compositions and the electronic structure of the B-site cation. Recent developments in the understanding of the properties of heavy element solids have opened up new possibilities for the design of advanced nuclear fuels and waste forms.

  14. The 237U(n,f) Cross Section

    Energy Technology Data Exchange (ETDEWEB)

    Younes, W; Britt, H C; Wilhelmy, J B

    2003-03-03

    The purpose of this note is to combine existing information on the {sup 237}U(n,f) cross section to determine if some consistency can be obtained for the neutron induced fission excitation of {sup 237}U. The neutron induced fission cross section of the 6.8 day {sup 237}U was measured directly by McNally et al. in 1968 using the Pommard nuclear device test. At the same time critical assembly measurements were done at Los Alamos using the Flattop assembly. A previous measurement was also made at LASL in 1954 with two different neutron sources, each peaked near 200 keV. The results were 0.66 {+-} 0.10 b and 0.70 {+-} 0.07 b for the (n,f) cross section. More recently Younes and Britt have reanalyzed direct reaction charged particle data of Cramer and Britt that had determined the fission probability of the {sup 238}U compound nucleus as a function of nuclear excitation energy. They have combined fission probabilities with calculated neutron absorption cross sections, including corrections for the differences in angular momentum between the direct and neutron induced reactions. From this analysis they have extracted equivalent {sup 237}U(n,f) cross sections. The technique for extracting surrogate (n,f) cross sections from (t,pf) data has been demonstrated in a recent publication for the test case {sup 235}U(n,f). In addition to this experimental information, Lynn and Hayes have recently done a new theoretical study of the fission cross sections for a series of isotopes in this region. A summary plot of the data is shown in Fig. 1. Below 0.5 MeV the McNally, Cowan, and Younes-Britt results are in reasonable agreement. The average cross section in the Younes-Britt results, for En = 0.1 to 0.4 MeV, is 0.80 times the McNally values which is well within the errors of the McNally experiment. Above 0.5 MeV the McNally results diverge toward higher values. It should be noted that this divergence begins approximately at the {sup 237}Np threshold and that {sup 237}Np is the

  15. Assessment and reduction of proliferation risk of reactor-grade plutonium regarding construction of ‘fizzle bombs’ by terrorists

    Energy Technology Data Exchange (ETDEWEB)

    Serfontein, Dawid E., E-mail: Dawid.Serfontein@nwu.ac.za [School for Mechanical and Nuclear Engineering, North West University (PUK-Campus), PRIVATE BAG X6001 (Internal Post Box 360), Potchefstroom 2520 (South Africa); Mulder, Eben J. [School for Mechanical and Nuclear Engineering, North West University (South Africa); Reitsma, Frederik [Calvera Consultants (South Africa)

    2014-05-01

    The approximately 23.7 wt% {sup 240}Pu in reactor-grade plutonium denatures the {sup 239}Pu to the extent that it cannot fuel high yield nuclear weapons. {sup 240}Pu has a high spontaneous fission rate, which increases the spontaneous neutron flux within the fuel. When such a nuclear weapon is triggered, these neutrons cause the nuclear fission chain reaction to pre-detonate which blows the imploding fuel shell apart before the designed level of compression and reactivity could be attained, thereby greatly reducing the average energy yield of such “fizzle” bombs. Therefore reactor-grade plutonium is normally viewed as highly proliferation resistant. In this article the literature on the proliferation resistance of reactor-grade plutonium and on the mechanism and effect of fizzle bombs is reviewed in order to test this view. It is shown that even very low yield fizzle bombs, exploded in urban areas, would still cause serious blast damage as well as radioactive contamination. Combined with the high levels of induced terror, fizzle bombs might thus be attractive psychological weapons for terrorists. Therefore reactor-grade plutonium may not be sufficiently proliferation resistant against nuclear terrorism. However, denaturisation with more than 9% {sup 238}Pu produces high levels of decay heat which will melt or explode the high explosives around uncooled implosion type weapons, rendering them useless. Unfortunately, reactor-grade Pu contains only 2.7% {sup 238}Pu and is thus not sufficiently proliferation resistant in this respect. It is also shown that the associated neptunium poses a substantial proliferation risk. In the present study strong improvement of the proliferation resistance was demonstrated by simulation of incineration of reactor-grade plutonium in the 400 MW{sub th} Pebble Bed Modular Reactor Demonstration Power Plant. Results for modified fuel cycles, aimed at transmutating {sup 237}Np to {sup 238}Pu are also reported. However, these

  16. Extraction and purification of {sup 227}Ac and development of solid {sup 219}Rn source

    Energy Technology Data Exchange (ETDEWEB)

    Tang, Quan; Qiu, Shoukang; Xiao, Detao; Zhou, Yaohui; An, Xiaogang [University of South China, Hengyang (China). Radon Key Laboratory of Hunan Province/School of Nuclear Science and Technology

    2014-04-01

    The method of {sup 227}Ac extraction and purification from high-grade uranium ore and the test results of solid {sup 219}Rn source made from {sup 227}Ac are reported in this paper. With five years of follow-up monitoring, radiochemical purity of {sup 227}Ac and the emanation power of solid {sup 219}Rn source has been checked by emanation method and γ-spectrometry, the results showed that {sup 228}Th, {sup 231}Pa and {sup 226}Ra have been effectively removed and the emanation power of {sup 219}Rn source is about 80%. The long-term test results also showed that the {sup 219}Rn emanation rate remains stable in a wide air humidity range (40% ∝ 90%). Though the {sup 219}Rn source has not been accurately calibrated yet, it has been applied in the research for delay coincidence measurement of {sup 223}Ra. (orig.)

  17. Mound Facility activities in chemical and physical research: July--December 1977. [Kr-Xe and Kr-Ar diffusion; Ne-Ar thermal diffusion

    Energy Technology Data Exchange (ETDEWEB)

    1978-05-01

    Isotope separation of Ar, C, /sup 3/He, Kr, Ne, O, and Xe isotopes is reported. TiFeH/sub x/, TiCoH/sub x/, TiCuH/sub x/, and VH/sub x/ were studied using NMR (proton relaxation times). VD/sub x/ and VT/sub x/ were synthesized. The problem of calculating the valence state of Pu is discussed. A series solution to the plutonium (N,H) characteristic equation is suggested. Shipments of /sup 231/Pa, /sup 230/Th, and /sup 229/Th are reported. Separation and processing of /sup 234/U are also reported. Theoretical methods were developed to calculate temperature distributions as functions of water flow rate in liquid thermal diffusion columns. Diffusion coefficients were measured from 300 to 1200/sup 0/K for Kr-Xe and Kr-Ar. New thermal diffusion factors are submitted for Ne-Ar.

  18. U—Series Dating of Fossil Bones:Results from Chinese Sites and Discussions on Its Reliability

    Institute of Scientific and Technical Information of China (English)

    沈冠军

    1996-01-01

    Calculations,according to some open-system models,point out that while a statistically significant discrepancy between the results of two U-series methods,230Th/234U and 227Th/220Th(or 231Pa/235U),attests a relatively recent and important uranium migration,concordant dates cannot guarantee closes-system behavior of sample.The results of 20 fossil bones from 10 Chinese sites,19 of which are determined by two U-series methods,are given,Judging from independent age controls,8 out of the 11 concordant age sets are unacceptable,The results in this paper suggest that uranium may cycle into or out of fossil bones,such geochemical events may take place at any time and no known preserving condition may securely protect them from being affected.So for the sitew we have studied,the U-series dating of fossil bones is of limited reliability.

  19. Non-destructive γ spectrum analysis of polymetallic nodules from the eastern Pacific

    Institute of Scientific and Technical Information of China (English)

    刘广山; 黄奕普; 蔡毅华; 陈敏

    2002-01-01

    -- Non-destructive γ spectrum analyses of 20 polymetallic nodules from the eastern Pacific were carried out. Numerous nuclides, such as 238 U, 230 Th, 226 Ra, 210 Pb, 228 Ra, 228 Th, 235 U, 227 Ac ( or 231pa) and 40K were detected. The count rates of the nuclides in the top or bottom side of nodules facing detector were measured and the ratio R of the count rates of nuclides in the top and the bottom sides was obtained. From counts and ratios, some useful information relating to the growth and movement of the nodules, the source of nuclide and relationship between those and environment can be gotten. A new method for clear distinction between the top and bottom sides of the nodule based on the R value of 226Ra or 210pb was developed. In addition, one can infer the turnover of nodules according to the R value of 230Th.

  20. Hybrid fusion-fission reactor with a thorium blanket: Its potential in the fuel cycle of nuclear reactors

    Science.gov (United States)

    Shmelev, A. N.; Kulikov, G. G.; Kurnaev, V. A.; Salahutdinov, G. H.; Kulikov, E. G.; Apse, V. A.

    2015-12-01

    Discussions are currently going on as to whether it is suitable to employ thorium in the nuclear fuel cycle. This work demonstrates that the 231Pa-232U-233U-Th composition to be produced in the thorium blanket of a hybrid thermonuclear reactor (HTR) as a fuel for light-water reactors opens up the possibility of achieving high, up to 30% of heavy metals (HM), or even ultrahigh fuel burnup. This is because the above fuel composition is able to stabilize its neutron-multiplying properties in the process of high fuel burnup. In addition, it allows the nuclear fuel cycle (NFC) to be better protected against unauthorized proliferation of fissile materials owing to an unprecedentedly large fraction of 232U (several percent!) in the uranium bred from the Th blanket, which will substantially hamper the use of fissile materials in a closed NFC for purposes other than power production.

  1. Analysis of Operating Strategies Using Different Target Designs For 238Pu Production

    Energy Technology Data Exchange (ETDEWEB)

    Thomas, Tomcy [University of Tennessee (UT); Sherman, Steven R [ORNL; Sawhney, Dr. Rapinder [University of Tennessee (UT)

    2017-01-01

    An engineering effort is underway to re-establish capability to produce 238Pu oxide at the kilogram scale in the United States. A multi-step batch process is being developed to produce this important material. Recently, a portion of this process was studied using discrete-event simulation tools to determine whether the conceptual process might achieve its yearly production goal. The study showed the conceptual process can meet the yearly production goal under some circumstances, but process improvements would be needed to ensure greater likelihood of success. This study extends the work performed previously by examining the effects of changing the reactor target design on the yearly process output. Two new reactor target configurations are considered an aluminum-clad reactor target containing 50% greater 237Np oxide content than the original target, and a zirconium alloy-clad target using no aluminum. The results indicate that use of the new aluminum-clad target configuration may allow the process to achieve the same yearly production goal in less time using fewer targets. If the zirconium alloy-clad target is used, then even fewer targets would be needed to reach the production goal, but some process changes would be required to handle the zirconium cladding. The number of days needed to process a target batch to completion, and the steady state 238Pu oxide production rate, for each configuration are compared to the results from the initial simulation study.

  2. Criticality safety aspects of spent fuel arrays from emerging nuclear fuel cycles

    Energy Technology Data Exchange (ETDEWEB)

    Nicolaou, G. [University of Thrace, Department of Electrical and Computer Engineering, Laboratory of Nuclear Technology, Kimmerria Campus, 67100 Xanthi (Greece)

    2010-07-01

    Emerging nuclear fuel cycles: fuels with Pu or minor actinides (MA) for their self-generated recycling or transmutation in PWR or FR {yields} reduction of radiotoxicity of HLW. The aim of work is to assess criticality (k{sub {infinity}}) of arrays of spent nuclear fuels from these emerging fuel cycles. Procedures: Calculations of - k{sub {infinity}}, using MCNP5 based on fresh and spent fuel compositions (infinite arrays), - spent fuel compositions using ORIGEN. Fuels considered: - commercial PWR-UO{sub 2} (R1) and -MOX (R2), [45 GWd/t] and fast reactor [100 GWd/t] (R3), - PWR self-generated Pu recycling (S1) and MA recycling (S2), FR self-generated MA recycling (S3), FR with 2% {sup 237}Np for transmutation purposes (T). Results: k{sub {infinity}} based on fresh and spent fuel compositions is shown. Fuels are clustered in two distinct families: - fast reactor fuels, - thermal reactor fuels; k{sub {infinity}} decreases when calculated on the basis of actinide and fission product inventory. In conclusions: - Emerging fuels considered resemble their corresponding commercial fuels; - k{sub {infinity}} decreases in all cases when calculated on the basis of spent fuel compositions (reactivity worth {approx}-20%{Delta}k/k), hence improving the effectiveness of packaging. (author)

  3. Transmutation of $^{239}$Pu and Other Nuclides Using Spallation Neutrons Produced by Relativistic Protons Reacting with Massive U- and Pb-Targets

    CERN Document Server

    Adam, J; Bamblevski, V P; Barabanov, M Yu; Bradnova, V; Chaloun, P; Hella, K M; Kalinnikov, V G; Krivopustov, M I; Kulakov, B A; Perelygin, V P; Pronskikh, V S; Pavliouk, A V; Solnyshkin, A A; Sosnin, A N; Stegailov, V I; Tsoupko-Sitnikov, V M; Zaverioukha, O S; Adloff, J C; Debeauvais, M; Brandt, R; Langrock, E J; Vater, P; Van, J S; Westmeier, W; Dwivedi, K K; Guo Shi Lun; Li Li Qiang; Hashemi-Nezhad, S R; Kievets, M K; Lomonosova, E M; Zhuk, I V; Modolo, G; Odoj, R; Zamani-Valassiadou, M

    2001-01-01

    Experimental studies on the transmutation of some long-lived radioactive waste nuclei, such as ^{129}I, ^{237}Np, and ^{239}Pu, as well as on natural uranium and lanthanum (all of them used as sensors) were carried out at the Synchrophasotron of the Laboratory for High Energies (JINR, Dubna). Spallation neutrons were produced by relativistic protons with energies in the range of 0.5 GeV\\le E(p)\\le 1.5 GeV interacting with 20 cm long uranium or lead target stacks. The targets were surrounded by 6 cm paraffin moderators. The radioactive sensors mentioned above were positioned on the outside surface of the moderator and contained typically approximately 0.5 up to 1 gram of long-lived isotopes. The highly radioactive targets were produced perfectly well-sealed in aluminum containers by the Institute of Physics and Power Engineering, Obninsk, Russia. From the experimentally observed transmutation rates one can easily extrapolate, that in a subcritical nuclear power assembly (or "energy amplifier") using a 10 mA pr...

  4. Neptunium(V) partitioning to uranium(VI) oxide and peroxide solids.

    Science.gov (United States)

    Douglas, Matthew; Clark, Sue B; Friese, Judah I; Arey, Bruce W; Buck, Edgar C; Hanson, Brady D

    2005-06-01

    Metaschoepite, [(UO2)8O2(OH)12] x 10H2O, and metastudtite, UO4 x 4H2O, are alteration phases anticipated in a spent nuclear fuel repository following the moist oxidation of UO2 on a geologic time scale. Dissolved concentrations and hence potential mobility of other radionuclides in the fuel, such as the neptunyl cation (NpO2+), will likely be determined by the extent of their partitioning into these U(VI) solids. 237Np is of particular interest due to its potential high mobility and long half-life (2.1 x 10(6) years.) In this study, metaschoepite has been precipitated and subsequently transformed to studtite in the presence of dissolved Np. The metaschoepite and studtite solids that formed initially contained dissolution studies of these solids at pH 6 demonstrate release of Np that exceeds congruent dissolution of U from metastudtite; furthermore, the released Np cation remains in solution. Thus, although the Np partitions into the metastudtite solid initially, it is released to solution over time, indicating that metastudtite is not likely to serve as a host solid for Np incorporation or sorption of the neptunyl cation on long time scales.

  5. Investigation of Space and Energy Distributions of Neutrons Generated in Lead Target and Uranium Blanket of the Electronuclear System "Energy plus Transmutation" under Irradiation with Protons at 1.5 GeV

    CERN Document Server

    Zhuk, I V; Krivopustov, M I; Sosnin, A N; Chultem, D; Vestmaer, V; Tumendelger, T; Zaveryukha, O S; Pavlyuk, A B

    2002-01-01

    The work contains the results of space-energy distributions of neutrons in U/Pb assembly, consisting of extended lead target and the model of natural uranium blanket irradiated with relativistic protons at 1.5 GeV. The research is carried out in the framework of a series of experiments using the model of subcritical heterogeneous electronuclear system at the Laboratory of High Energies, JINR, Dubna ("Investigation of Physical Aspects of Electronuclear Method of Energy Production and Transmutation of Radioactive Waste Using Beams from JINR Synchrophasotron/Nuclotron" - project "Energy plus Transmutation"). The results of measurements and calculations of ^{235}U, ^{238}U and ^{232}Th fission rate distributions as well as threshold spectral indexes {\\bar\\sigma_f^{^{232}Th}}/{\\bar\\sigma_f^{^{235}U}} and {\\bar\\sigma_f^{^{238}U}}/{\\bar\\sigma_f^{^{235}U}} along the radius of the target and model uranium blanket are presented. The results of measurements and calculations of ^{234}U, ^{236}U and ^{237}Np fission rate ...

  6. Comparison of ICRP2 and ICRP30 for estimating the dose and adverse health effects from potential radionuclide releases from a geologic waste repository

    Energy Technology Data Exchange (ETDEWEB)

    Runkle, G.E.; Soldat, J.K.

    1982-01-01

    This paper presents a comparison of the calculated risk of adverse health effects from the radionuclides considered in the inventory of a high-level waste repository using the ICRP2 and ICRP30 internal dosimetry models. A CRPC (cancer risk per curie) index was calculated to compare the two models. The CRPC indices for the ICRP30 model are approximately 2 to 20 times higher than the ICRP2 indices for most radionuclides for ingestion intakes. However, the /sup 237/Np index is approximately 200 times greater for the ICRP30 model and the /sup 228/Ra and /sup 226/Ra indices are approximately 30 to 90 times greater for the ICRP2 model. Generally, there is closer agreement of the CRPC indices for the inhalation intakes. A scenario that considers a U-tube effect and withdrawal of water from wells downdip from the repository was analyzed. This analysis, based on a hypothetical waste disposal site, considered groundwater transport and environmental transport with subsequent uptake by the human via ingestion and inhalation. The ICRP30 risks are higher by approximately 20 at 10,000 years post closure for the ingestion pathway. However, the ICRP2 risks are higher by factors of approximately 2 to 10 at times greater than 50,000 years. Differences in the mathematical modeling assumptions, gut uptakes and other metabolic parameters between the two models account for most of the variability in the risk estimates.

  7. Update of the α - n Yields for Reactor Fuel Materials for the Interest of Nuclear Safeguards

    Science.gov (United States)

    Simakov, S. P.; van den Berg, Q. Y.

    2017-01-01

    The neutron yields caused by spontaneous α-decay of actinides and subsequent (α,xn) reactions were re-evaluated for the reactor fuel materials UO2, UF6, PuO2 and PuF4. For this purpose, the most recent reference data for decay parameters, α-particle stopping powers and (α,xn) cross sections were collected, analysed and used in calculations. The input data and elaborated code were validated against available thick target neutron yields in pure and compound materials measured at accelerators or with radioactive sources. This paper provides the specific neutron yields and their uncertainties resultant from α-decay of actinides 241Am, 249Bk, 252Cf, 242,244Cm, 237Np, 238-242Pu, 232Th and 232-236,238U in oxide and fluoride compounds. The obtained results are an update of previous reference tables issued by the Los Alamos National Laboratory in 1991 which were used for the safeguarding of radioactive materials by passive non-destructive techniques. The comparison of the updated values with previous ones shows an agreement within one estimated uncertainty (≈ 10%) for oxides, and deviations of up to 50% for fluorides.

  8. The Surrogate Method: Past, Present and Future

    Energy Technology Data Exchange (ETDEWEB)

    Lesher, S R; Bernstein, L A; Burke, J T; Lyles, B F; Clark, R M; Fallon, P; Phair, L

    2008-01-09

    The STARS/LiBerACE collaboration has been exploring the surrogate technique with success in the actinide region. This method uses a direct reaction to measure the decay probability of the same compound nucleus produced via a neutron-induced channel. This paper serves as an overview of these activities. Using the STARS array at 88-inch Cyclotron at Lawrence Berkeley National Laboratory we have explored the following surrogate reactions: {sup 234}U({alpha}, {alpha}{prime}f), {sup 235}U({sup 3}He, {alpha}f), {sup 236}U({alpha}, {alpha}{prime}f), {sup 238}U ({alpha},{alpha}{prime}f), {sup 238}U({sup 3}He,{alpha}f), {sup 238}U({sup 3}He, tf) surrogates for {sup 233}U(n,f), {sup 233}U(n,f), {sup 235}U(n,f), {sup 237}U(n,f), {sup 236}U(n,f), and {sup 237}Np(n,f), respectively.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-07-09

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

  10. Review and Assessment of Neutron Cross Section and Nubar Covariances for Advanced Reactor Systems

    Energy Technology Data Exchange (ETDEWEB)

    Maslov,V.M.; Oblozinsky, P.; Herman, M.

    2008-12-01

    In January 2007, the National Nuclear Data Center (NNDC) produced a set of preliminary neutron covariance data for the international project 'Nuclear Data Needs for Advanced Reactor Systems'. The project was sponsored by the OECD Nuclear Energy Agency (NEA), Paris, under the Subgroup 26 of the International Working Party on Evaluation Cooperation (WPEC). These preliminary covariances are described in two recent BNL reports. The NNDC used a simplified version of the method developed by BNL and LANL that combines the recent Atlas of Neutron Resonances, the nuclear reaction model code EMPIRE and the Bayesian code KALMAN with the experimental data used as guidance. There are numerous issues involved in these estimates of covariances and it was decided to perform an independent review and assessment of these results so that better covariances can be produced for the revised version in future. Reviewed and assessed are uncertainties for fission, capture, elastic scattering, inelastic scattering and (n,2n) cross sections as well as prompt nubars for 15 minor actinides ({sup 233,234,236}U, {sup 237}Np, {sup 238,240,241,242}Pu, {sup 241,242m,243}Am and {sup 242,243,244,245}Cm) and 4 major actinides ({sup 232}Th, {sup 235,238}U and {sup 239}Pu). We examined available evaluations, performed comparison with experimental data, taken into account uncertainties in model parameterization and made use state-of-the-art nuclear reaction theory to produce the uncertainty assessment.

  11. Certified reference material for radionuclides in fish flesh sample IAEA-414 (mixed fish from the Irish Sea and North Sea)

    Energy Technology Data Exchange (ETDEWEB)

    Pham, M.K. [International Atomic Energy Agency (IAEA), Marine Environment Laboratory (MEL), MC 98000 (Monaco)]. E-mail: m.pham@iaea.org; Sanchez-Cabeza, J.A.; Povinec, P.P.; Gastaud, J.; La Rosa, J.; Lee, S.-H.; Liong Wee Kwong, L.; Oregioni, B.; Wyse, E. [International Atomic Energy Agency (IAEA), Marine Environment Laboratory (MEL), MC 98000 (Monaco); Arnold, D. [Physikalisch-Technische Bundesanstalt, Braunschweig, 38116 Germany (Germany); Benmansour, M. [Centre National de l' Energie, des Sciences et des Techniques Nucleaires (CNESTEN), B.P. 1382, R.P.10001, Rabat (Morocco); Bojanowski, R. [Institute of Oceanology, Polish Academy of Sciences, PL-81-712 Sopot (Poland); Carvalho, F.P. [Instituto Tecnologico e Nuclear, Departamento de Proteccao Radiologica e Seguranca Nuclear, P-2685-953 Sacavem (Portugal); Kim, C.K. [Department of Radiological Environmental Assessment, Korea Institute of Nuclear Safety, Yo-song, Taejon 305-600, Korea (Korea); Esposito, M. [Laboratorio di Ingegneria Nucleare, Universita di Bologna, 40136 Bologna (Italy); Gasco, C.L. [CIEMAT-DIAE, Radioecologia del Medio Acuatico, 28040 Madrid (Spain); Ham, G.J. [National Radiological Protection Board, Chilton, Didcot, Oxon, OX11 0RA (United Kingdom); Hegde, A.G. [Environmental Survey Laboratory, Bhabha Atomic Research Center, Tarapur Atomic Power Station, Maharashtra 401 504 (India); Holm, E. [Department of Medical Radiation Physics, Lund University Hospital, 22185 Lund (Sweden); Jaskierowicz, D. [Lab. d' Analyses de Surveillance et d' Expertise de la Marine, Base Navale de Cherbourg, 50115 Cherbourg (France); Kanisch, G. [Federal Research Centre for Fisheries, Institute of Fisheries Ecology, 20539 Hamburg (Germany); Llaurado, M. [Lab. de Radiologia Ambiental, Dept. de Quimica Analitica, Facultat de Quimica, Universitat de Barcelona, 08028 Barcelona (Spain); Le Petit, G. [Commissariat a l' Energie Atomique, DASE/SRCE, 91680 Bruyeres-le-Chatel (France); Maruo, Y. [and others

    2006-10-15

    A certified reference material (CRM) for radionuclides in fish sample IAEA-414 (mixed fish from the Irish Sea and North Seas) is described and the results of the certification process are presented. Nine radionuclides ({sup 4}K, {sup 137}Cs, {sup 232}Th, {sup 234}U, {sup 235}U, {sup 238}U, {sup 238}Pu, {sup 239+24}Pu and {sup 241}Am) were certified for this material. Information on massic activities with 95% confidence intervals is given for six other radionuclides ({sup 9}Sr, {sup 21}Pb({sup 21}Po), {sup 226}Ra, {sup 239}Pu, {sup 24}Pu {sup 241}Pu). Less frequently reported radionuclides ({sup 99}Tc, {sup 129}I, {sup 228}Th, {sup 23}Th and {sup 237}Np) and information on some activity and mass ratios are also included. The CRM can be used for quality assurance/quality control of the analysis of radionuclides in fish sample, for the development and validation of analytical methods and for training purposes. The material is available from IAEA, Vienna, in 100 g units.

  12. Th and U fuel photofission study by NTD for AD-MSR subcritical assembly

    Energy Technology Data Exchange (ETDEWEB)

    Sajo-Bohus, Laszlo; Greaves, Eduardo D.; Barros, Haydn; Pino, Felix; Barrera, Maria T.; Farina, Fulvio [Universidad Simón Bolívar, Nuclear Physics Laboratory, Apdo 89000, Caracas 1080A (Venezuela, Bolivarian Republic of); Davila, Jesus [Física Médica C. A. and Universidad Central de Venezuela, Caracas (Venezuela, Bolivarian Republic of)

    2015-07-23

    During the last decade a considerable effort has been devoted for developing energy generating systems based on advanced nuclear technology within the design concepts of GEN-IV. Thorium base fuel systems such as accelerator driven nuclear reactors are one of the often mentioned attractive and affordable options. Several radiotherapy linear accelerators are on the market and due to their reliability, they could be employed as drivers for subcritical liquid fuel assemblies. Bremsstrahlung photons with energies above 5.5MeV, induce (γ,n) and (e,e’n) reactions in the W-target. Resulting gamma radiation and photo or fission neutrons may be absorbed in target materials such as thorium and uranium isotopes to induce sustained fission or nuclear transmutation in waste radioactive materials. Relevant photo driven and photo-fission reaction cross sections are important for actinides {sup 232}Th, {sup 238}U and {sup 237}Np in the radiotherapy machines energy range of 10-20 MV. In this study we employ passive nuclear track detectors (NTD) to determine fission rates and neutron production rates with the aim to establish the feasibility for gamma and photo-neutron driven subcritical assemblies. To cope with these objectives a 20 MV radiotherapy machine has been employed with a mixed fuel target. Results will support further development for a subcritical assembly employing a thorium containing liquid fuel. It is expected that acquired technological knowledge will contribute to the Venezuelan nuclear energy program.

  13. Development and synthesis of durable self-glowing crystals doped with plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Burakov, B.E. [Laboratory of Applied Mineralogy and Radiogeochemistry, V.G. Khlopin Radium Institute, 2nd Site, 1, Rentgena Street, St. Petersburg 197101 (Russian Federation); Domracheva, Ya.V. [Ioffe Physico-Technical Institute, Russian Academy of Sciences, 26, Polytekhnicheskaya Street, St. Petersburg 194021 (Russian Federation)], E-mail: y.domracheva@mail.ioffe.ru; Zamoryanskaya, M.V. [Ioffe Physico-Technical Institute, Russian Academy of Sciences, 26, Polytekhnicheskaya Street, St. Petersburg 194021 (Russian Federation); Petrova, M.A.; Garbuzov, V.M.; Kitsay, A.A.; Zirlin, V.A. [Laboratory of Applied Mineralogy and Radiogeochemistry, V.G. Khlopin Radium Institute, 2nd Site, 1, Rentgena Street, St. Petersburg 197101 (Russian Federation)

    2009-03-15

    Different crystalline materials doped with plutonium and other alpha-emitting radionuclides are characterized by self-glowing. Some of these materials, in particular, monocrystalline ones, which are highly chemically resistant, mechanically durable, and stable under radiation damage are promising for application in optical couplers, robotics and medicine. They might be used for a long time (from tens to hundreds years) in aggressive chemical media and space. Crystals with low content of radionuclides (less than 0.1 wt%) but intensive self-glowing are main subject of interest. Phosphate and silicate single crystals with zircon structure: xenotime, (Y,...)PO{sub 4} and zircon, (Zr,...)SiO{sub 4}, were doped with {sup 238}Pu, {sup 237}Np and non-radioactive elements: Eu{sup 3+}; In{sup 3+} and Tb{sup 3+}. The most intensive self-glowing was obtained for xenotime crystals doped with 0.1 wt% {sup 238}Pu and Eu; and for zircon crystals doped with 0.01 wt% {sup 238}Pu and coupled admixture of In and Tb.

  14. Isotope ratio measurement of uranium in safeguards environmental samples by inductively-coupled plasma mass spectrometry (ICP-MS)

    Energy Technology Data Exchange (ETDEWEB)

    Magara, Masaaki; Sakakibara, Takaaki; Kurosawa, Setsumi; Takahashi, Masato; Sakurai, Satoshi; Hanzawa, Yukiko; Esaka, Fumitaka; Watanabe, Kazuo; Usuda, Shigekazu [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    2002-04-01

    In order to measure isotope ratio of uranium in safeguards environmental samples with ICP-MS precisely, production of polyatomic ions of IrAr, PtAr and AuAr was measured and mass bias of ICP-MS is investigated by using isotopic standards of uranium and lead. The intensities of IrAr, PtAr and AuAr relative to the atomic ions were found to be 1.8 x 10{sup -6}, 1.6 x 10{sup -5} and 4.1 x 10{sup -5}, respectively. The production of {sup 193}Ir{sup 40}Ar is too small to interfere with the measurement of {sup 233}U, if the concentration of Ir is the same level as that of {sup 233}U. However, there is possibility that the presence of Pt and Au interferes with the measurement of minor isotopes of uranium and {sup 237}Np. On the other hand, the mass biases of {sup 235}U/{sup 238}U and {sup 208}Pb/{sup 206}Pb were measured with the parameter of {sup 238}U{sup 16}O/{sup 238}U. Since unexpected change of the mass bias during measurements causes frequently erroneous results, the monitoring of {sup 238}U{sup 16}O/{sup 238}U is effective for the precise isotope ratio measurement. (author)

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1994-06-01

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

  16. Transuranic contamination of stainless steel in nitric acid

    Science.gov (United States)

    Kerry, Timothy; Banford, Anthony W.; Thompson, Olivia R.; Carey, Thomas; Schild, Dieter; Geist, Andreas; Sharrad, Clint A.

    2017-09-01

    Stainless steels coupons have been exposed to transuranic species in conditions representative of those found in a spent nuclear fuel reprocessing plant. Stainless steel was prepared to different surface finishes and exposed to nitric acid of varying concentrations containing 237Np, 239Pu or 243Am for one month at 50 °C. Contamination by these transuranics has been observed on all surfaces exposed to the solution through the use of autoradiography. This technique showed that samples held in 4 M HNO3 bind 2-3 times as much radionuclide as those held in 10.5 M HNO3. It was also found that the polished steel surfaces generally took up more transuranic contamination than the etched and ;as received; steel finishes. The extent of corrosion on the steel surfaces was found, by scanning electron microscopy, to be greater in solutions containing Np and Pu in comparison to that observed from contact with Am containing solutions, indicating that redox activity of transuranics can influence the mechanism of stainless steel corrosion.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2003-07-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2008-07-01

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

  19. Estimated (n,f) cross sections for 236,236m237,238-Np, 237,237m-Pu, and 240,241,242,242m,243,244,244m-Am isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Younes, W; Becker, J; Britt, H

    2004-01-16

    Neutron-induced fission cross sections on targets of {sup 236,236m,237,238}Np, {sup 237,237m}Pu, and {sup 240,241,242,242m,243,244,244m}Am have been estimated for incident neutron energies of up to 6 MeV, using the ''surrogate'' technique and the ({sup 3}He,df) and ({sup 3}He,tf) reactions on stable targets to measure fission probabilities. In isotopes where low-lying isomeric states are known to exist, the (n,f) cross section on the corresponding isomeric targets has been estimated, using the surrogate technique. For targets of {sup 237}Np, {sup 241}Am, {sup 242m}Am, {sup 243}Am, measurements of the (n,f) cross section exist, and comparison with the surrogate-method results suggests that the (n,f) cross sections estimated by the surrogate technique are reliable to within 10% for incident neutron energies E{sub n}{approx}>2 MeV. Tabulated values of the estimated (n,f) cross sections are given in an appendix.

  20. Study on transfer behavior of radionuclides from soil to plants

    Energy Technology Data Exchange (ETDEWEB)

    Morita, Shigemitsu; Watanabe, Hitoshi; Katagiri, Hiromi; Shinohara, Kunihiko [Environmental Protection Section, Environment and Safety Division, Japan Nuclear Cycle Development Institute, Tokai, Ibaraki (Japan)

    1999-03-01

    Technetium-99 (Tc-99), Iodine-129 (I-129) and Neptunium-237 (Np-237) are important radionuclides for environmental assessment around nuclear fuel cycle facilities, because they have long half-lives and relatively high mobilities in the environment. Therefore, we have studied on the determination method, distribution and behavior of such long-lived radionuclides in surface soil environment. A new analytical technique using Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and Microwave Induced Plasma Mass Spectrometry (MIP-MS) were applied to the determination of long-lived radionuclides in environmental samples. The sensitivity of ICP-MS method was 10 to 100,000 times higher, and the counting time was 100 to 100,000 times shorter than the conventional radioanalytical methods. The depth profiles showed that more than 90% of Tc-99, I-129, Np-237 and Pu-239, 240 were retained in the surface layer, up to 10 cm in depth, which contained much amount of organic materials. The result suggests that the content of organic materials in soil is related to adsorption of these nuclides on soil. (author)

  1. Dose coefficients and derived guidance and clinical decision levels for contaminated wounds

    Energy Technology Data Exchange (ETDEWEB)

    Bertelli, Luiz [Los Alamos National Laboratory; Toohey, Richard E [ORISE/ORAU; Sugarman, Steven A [ORISE/ORAU; Christensen, Doran R [ORISE/ORAU

    2009-01-01

    The NCRP Wound Model describing the retention of selected radionuclides at the site of a contaminated wound and their uptake into the transfer compartment has been combined with the ICRP element-specific systemic models for those radionuclides to derive dose coefficients for intakes via contaminated wounds. Those coefficients have been used to generate derived guidance levels (i.e., the activity in a wound that would result in an effective dose of 20 or 50 mSv, or in some cases, a committed organ equivalent dose of 500 mSv), and clinical decision levels (i.e., activity levels that would indicate the need for consideration of medical intervention to remove activity from the wound site or administration of decorporation therapy or both), typically set at 5 times the derived guidance levels. Data are provided for the radionuclides commonly encountered at nuclear power plants and nuclear weapons, fuel fabrication or recycling, waste disposal, medical and research facilities. These include: {sup 60}Co, {sup 90}Sr, {sup 99m}Tc, {sup 131}I, {sup 137}Cs, {sup 192}Ir, {sup 210}Po, {sup 226,228}Ra, {sup 228,232}Th, {sup 235,238}U, {sup 237}Np, {sup 238,239}Pu, {sup 241}Am, {sup 242,244}Cm, and {sup 252}Cf.

  2. Radiation-induced decomposition of U(VI) phases to nanocrystals of UO"2 [rapid communication

    Science.gov (United States)

    Utsunomiya, Satoshi; Ewing, Rodney C.; Wang, Lu-Min

    2005-12-01

    U 6+-phases are common alteration products, under oxidizing conditions, of uraninite and the UO 2 in spent nuclear fuel. These U 6+-phases are subjected to a radiation field caused by the α-decay of U, or in the case of spent nuclear fuel, incorporated actinides, such as 239Pu and 237Np. In order to evaluate the effects of α-decay events on the stability of the U 6+-phases, we report, for the first time, the results of ion beam irradiations (1.0 MeV Kr 2+) of U 6+-phases. The heavy-particle irradiations are used to simulate the ballistic interactions of the recoil-nucleus of an α-decay event with the surrounding structure. The Kr 2+-irradiation decomposed the U 6+-phases to UO 2 nanocrystals at doses as low as 0.006 displacements per atom (dpa). U 6+-phases accumulate substantial radiation doses (˜1.0 displacement per atom) within 100,000 yr if the concentration of incorporated 239Pu is as high as 1 wt.%. Similar nanocrystals of UO 2 were observed in samples from the natural fission reactors at Oklo, Gabon. Multiple cycles of radiation-induced decomposition to UO 2 followed by alteration to U 6+-phases provide a mechanism for the remobilization of incorporated radionuclides.

  3. Semianalytical Solutions of Radioactive or Reactive Tracer Transport in Layered Fractured Media

    Energy Technology Data Exchange (ETDEWEB)

    G.J. Moridis; G. S. Bodvarsson

    2001-10-01

    In this paper, semianalytical solutions are developed for the problem of transport of radioactive or reactive tracers (solutes or colloids) through a layered system of heterogeneous fractured media with misaligned fractures. The tracer transport equations in the matrix account for (a) diffusion, (b) surface diffusion (for solutes only), (c) mass transfer between the mobile and immobile water fractions, (d) linear kinetic or equilibrium physical, chemical, or combined solute sorption or colloid filtration, and (e) radioactive decay or first order chemical reactions. Any number of radioactive decay daughter products (or products of a linear, first-order reaction chain) can be tracked. The tracer-transport equations in the fractures account for the same processes, in addition to advection and hydrodynamic dispersion. Additionally, the colloid transport equations account for straining and velocity adjustments related to the colloidal size. The solutions, which are analytical in the Laplace space, are numerically inverted to provide the solution in time and can accommodate any number of fractured and/or porous layers. The solutions are verified using analytical solutions for limiting cases of solute and colloid transport through fractured and porous media. The effect of important parameters on the transport of {sup 3}H, {sup 237}Np and {sup 239}Pu (and its daughters) is investigated in several test problems involving layered geological systems of varying complexity. {sup 239}Pu colloid transport problems in multilayered systems indicate significant colloid accumulations at straining interfaces but much faster transport of the colloid than the corresponding strongly sorbing solute species.

  4. Semianalytical Solutions of Radioactive or Reactive Transport in Variably-Fractured Layered Media: 1. Solutes

    Energy Technology Data Exchange (ETDEWEB)

    George J. Moridis

    2001-10-01

    In this paper, semianalytical solutions are developed for the problem of transport of radioactive or reactive solute tracers through a layered system of heterogeneous fractured media with misaligned fractures. The tracer transport equations in the non-flowing matrix account for (a) diffusion, (b) surface diffusion, (c) mass transfer between the mobile and immobile water fractions, (d) linear kinetic or equilibrium physical, chemical, or combined solute sorption or colloid filtration, and (e) radioactive decay or first-order chemical reactions. The tracer-transport equations in the fractures account for the same processes, in addition to advection and hydrodynamic dispersion. Any number of radioactive decay daughter products (or products of a linear, first-order reaction chain) can be tracked. The solutions, which are analytical in the Laplace space, are numerically inverted to provide the solution in time and can accommodate any number of fractured and/or porous layers. The solutions are verified using analytical solutions for limiting cases of solute and colloid transport through fractured and porous media. The effect of important parameters on the transport of {sup 3}H, {sup 237}Np and {sup 239}Pu (and its daughters) is investigated in several test problems involving layered geological systems of varying complexity.

  5. Semianalytical solutions of radioactive or reactive transport invariably-fractured layered media: 1. Solutes

    Energy Technology Data Exchange (ETDEWEB)

    Moridis, George J.

    2001-10-10

    In this paper, semianalytical solutions are developed for the problem of transport of radioactive or reactive solute tracers through a layered system of heterogeneous fractured media with misaligned fractures. The tracer transport equations in the non-flowing matrix account for (a) diffusion, (b) surface diffusion, (c) mass transfer between the mobile and immobile water fractions, (d) linear kinetic or equilibrium physical, chemical, or combined solute sorption or colloid filtration, and (e) radioactive decay or first-order chemical reactions. The tracer-transport equations in the fractures account for the same processes, in addition to advection and hydrodynamic dispersion. Any number of radioactive decay daughter products (or products of a linear, first-order reaction chain) can be tracked. The solutions, which are analytical in the Laplace space, are numerically inverted to provide the solution in time and can accommodate any number of fractured and/or porous layers. The solutions are verified using analytical solutions for limiting cases of solute and colloid transport through fractured and porous media. The effect of important parameters on the transport of {sup 3}H, {sup 237}Np and {sup 239}Pu (and its daughters) is investigated in several test problems involving layered geological systems of varying complexity.

  6. Burnup analysis of the VVER-1000 reactor using thorium-based fuel

    Energy Technology Data Exchange (ETDEWEB)

    Korkmaz, Mehmet E.; Agar, Osman; Bueyueker, Eylem [Karamanoglu Mehmetbey Univ., Karaman (Turkey). Faculty of Kamil Ozdag Science

    2014-12-15

    This paper aims to investigate {sup 232}Th/{sup 233}U fuel cycles in a VVER-1000 reactor through calculation by computer. The 3D core geometry of VVER-1000 system was designed using the Serpent Monte Carlo 1.1.19 Code. The Serpent Code using parallel programming interface (Message Passing Interface-MPI), was run on a workstation with 12-core and 48 GB RAM. {sup 232}Th/{sup 235}U/{sup 238}U oxide mixture was considered as fuel in the core, when the mass fraction of {sup 232}Th was increased as 0.05-0.1-0.2-0.3-0.4 respectively, the mass fraction of {sup 238}U equally was decreased. In the system, the calculations were made for 3 000 MW thermal power. For the burnup analyses, the core is assumed to deplete from initial fresh core up to a burnup of 16 MWd/kgU without refuelling considerations. In the burnup calculations, a burnup interval of 360 effective full power days (EFPDs) was defined. According to burnup, the mass changes of the {sup 232}Th, {sup 233}U, {sup 238}U, {sup 237}Np, {sup 239}Pu, {sup 241}Am and {sup 244}Cm were evaluated, and also flux and criticality of the system were calculated in dependence of the burnup rate.

  7. Heavy element radionuclides (Pu, Np, U) and {sup 137}Cs in soils collected from the Idaho National Engineering and Environmental Laboratory and other sites in Idaho, Montana, and Wyoming

    Energy Technology Data Exchange (ETDEWEB)

    Beasley, T.M.; Rivera, W. Jr. [Dept. of Energy, New York, NY (United States). Environmental Measurements Lab.; Kelley, J.M.; Bond, L.A. [Pacific Northwest National Lab., Richland, WA (United States); Liszewski, M.J. [Bureau of Reclamation (United States); Orlandini, K.A. [Argonne National Lab., IL (United States)

    1998-10-01

    The isotopic composition of Pu in soils on and near the Idaho National Engineering and Environmental Laboratory (INEEL) has been determined in order to apportion the sources of the Pu into those derived from stratospheric fallout, regional fallout from the Nevada Test Site (NTS), and facilities on the INEEL site. Soils collected offsite in Idaho, Montana, and Wyoming were collected to further characterize NTS fallout in the region. In addition, measurements of {sup 237}Np and {sup 137}Cs were used to further identify the source of the Pu from airborne emissions at the Idaho Chemical Processing Plant (ICPP) or fugitive releases from the Subsurface Disposal Area (SDA) in the Radioactive Waste Management Complex (RWMC). There is convincing evidence from this study that {sup 241}Am, in excess of that expected from weapons-grade Pu, constituted a part of the buried waste at the SDA that has subsequently been released to the environment. Measurements of {sup 236}U in waters from the Snake River Plain aquifer and a soil core near the ICPP suggest that this radionuclide may be a unique interrogator of airborne releases from the ICPP. Neptunium-237 and {sup 238}Pu activities in INEEL soils suggest that airborne releases of Pu from the ICPP, over its operating history, may have recently been overestimated.

  8. Neutron-emission measurements at a white neutron source

    Energy Technology Data Exchange (ETDEWEB)

    Haight, Robert C [Los Alamos National Laboratory

    2010-01-01

    Data on the spectrum of neutrons emittcd from neutron-induced reactions are important in basic nuclear physics and in applications. Our program studies neutron emission from inelastic scattering as well as fission neutron spectra. A ''white'' neutron source (continuous in energy) allows measurements over a wide range of neutron energies all in one experiment. We use the tast neutron source at the Los Alamos Neutron Science Center for incident neutron energies from 0.5 MeV to 200 MeV These experiments are based on double time-of-flight techniques to determine the energies of the incident and emitted neutrons. For the fission neutron measurements, parallel-plate ionization or avalanche detectors identify fission in actinide samples and give the required fast timing pulse. For inelastic scattering, gamma-ray detectors provide the timing and energy spectroscopy. A large neutron-detector array detects the emitted neutrons. Time-of-flight techniques are used to measure the energies of both the incident and emitted neutrons. Design considerations for the array include neutron-gamma discrimination, neutron energy resolution, angular coverage, segmentation, detector efficiency calibration and data acquisition. We have made preliminary measurements of the fission neutron spectra from {sup 235}U, {sup 238}U, {sup 237}Np and {sup 239}Pu. Neutron emission spectra from inelastic scattering on iron and nickel have also been investigated. The results obtained will be compared with evaluated data.

  9. Progress on radiochemical analysis for nuclear waste management in decommissioning

    Energy Technology Data Exchange (ETDEWEB)

    Hou, X. (Technical Univ. of Denmark. Center for Nuclear Technologies (NuTech), Roskilde (Denmark))

    2012-01-15

    This report summarized the progress in the development and improvement of radioanalytical methods for decommissioning and waste management completed in the NKS-B RadWaste 2011 project. Based on the overview information of the analytical methods in Nordic laboratories and requirement from the nuclear industry provided in the first phase of the RadWaste project (2010), some methods were improved and developed. A method for efficiently separation of Nb from nuclear waste especially metals for measurement of long-lived 94Nb by gamma spectrometry was developed. By systematic investigation of behaviours of technetium in sample treatment and chromatographic separation process, an effective method was developed for the determination of low level 99Tc in waste samples. An AMS approachment was investigated to measure ultra low level 237Np using 242Pu for AMS normalization, the preliminary results show a high potential of this method. Some progress on characterization of waste for decommissioning of Danish DR3 is also presented. (Author)

  10. Reference Materials for Reactor Neutron Fluence Rate and Temperature Measurements

    Science.gov (United States)

    Ingelbrecht, C.

    2003-06-01

    Certified reference materials are distributed by the European Commission through the BCR® programme (over 500 CRMs) including a series of activation and fission monitor materials originally proposed by the Euratom Working Group on Reactor Dosimetry. The current range (18 CRMs) includes materials to cover the complete energy spectrum, and suitable for different irradiation times. Fission monitors are 238UO2 or 237NpO2 in the form of microspheres. Activation monitors are high purity metals (Ni, Cu, Al, Fe, Nb, Rh, or Ti), certified for interfering trace impurities, or dilute aluminium-based alloys. Reference materials newly certified are IRMM-530R A1-0.1%Au, replacing the exhausted IRMM-530 material, used as comparator for k0- standardisation, and three new Al-Co alloys (0.01, 0.1 and 1.0%Co). Others in the process of certification are A1-0.1%Ag and A1-2%Sc for thermal and epithermal fluence rate measurements and two uranium-doped glass materials intended for dosimetry by the fission-track technique. Various alloy compositions have been prepared for use as melt-wire temperature monitors with melting points ranging from 198 to 327ºC.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1994-06-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-02-18

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

  13. Effects of fasting and/or oxidizing and reducing agents on absorption of neptunium from the gastrointestinal tract of mice and adult or neonatal rats.

    Science.gov (United States)

    Sullivan, M F; Ruemmler, P S; Ryan, J L

    1984-12-01

    Neptunium-237(V) nitrate was administered by gavage to groups of fed or fasted adult and 5-day-old rats. Some groups also received the oxidants quinhydrone or ferric iron, and others received the reducing agent ferrous iron. Adult mice received ferric or ferrous iron and 235Np. When the adult rats were killed at 7 days after gavage, measurements showed that, compared with rats that were fed, a 24-hr fast caused a fivefold increase in 237Np absorption and retention. Both quinhydrone and ferric iron caused an even greater increase in absorption in both fed and fasted rats. Ferrous iron, on the other hand, decreased absorption in fasted rats to values lower than those obtained in fed rats. Similar results were obtained in mice treated with 235Np and either ferric or ferrous iron. The highest absorption obtained after gavage of ferric iron to fasted rats and mice was about two orders of magnitude higher than the value obtained in animals that were fed before gavage. The effects of ferric and ferrous iron on neptunium absorption by neonatal rats were similar to their effects on adult animals but of lesser magnitude. These results are consistent with the hypothesis that Np(V), when given in small mass quantities to fed animals, is reduced in the gastrointestinal tract to Np(IV), which is less well absorbed than Np(V).

  14. RESEARCH AND DEVELOPMENT ACTIVITIES AT SAVANNAH RIVER SITE'S H CANYON FACILITY

    Energy Technology Data Exchange (ETDEWEB)

    Sexton, Lindsay; Fuller, Kenneth

    2013-07-09

    The Savannah River Site's (SRS) H Canyon Facility is the only large scale, heavily shielded, nuclear chemical separations plant still in operation in the U.S. The facility's operations historically recovered uranium-235 (U-235) and neptunium-237 (Np-237) from aluminum-clad, enriched-uranium fuel tubes from Site nuclear reactors and other domestic and foreign research reactors. Today the facility, in conjunction with HB Line, is working to provide the initial feed material to the Mixed Oxide Facility also located on SRS. Many additional campaigns are also in the planning process. Furthermore, the facility has started to integrate collaborative research and development (R&D) projects into its schedule. H Canyon can serve as the appropriate testing location for many technologies focused on monitoring the back end of the fuel cycle, due to the nature of the facility and continued operation. H Canyon, in collaboration with the Savannah River National Laboratory (SRNL), has been working with several groups in the DOE complex to conduct testing demonstrations of novel technologies at the facility. The purpose of conducting these demonstrations at H Canyon will be to demonstrate the capabilities of the emerging technologies in an operational environment. This paper will summarize R&D testing activities currently taking place in H Canyon and discuss the possibilities for future collaborations.

  15. Production of {sup 234,235}Np and {sup 236}Pu in bombardment of {sup 236}U with protons in the energy range from 17 to 40 MeV

    Energy Technology Data Exchange (ETDEWEB)

    Aaltonen, J.; Helariutta, K. [Univ. of Helsinki, Lab. of Radiochemistry, Dept. of Chemistry, Univ. of Helsinki (Finland); Gromova, E.A.; Jakovlev, V.A. [V. G. Khlopin Radium Inst., Lab. of Nuclear Reactions and Nuclear Medicine, St. Petersburg (Russian Federation); Trzaska, W.H.; Huikari, J.; Kolhinen, V.S.; Rinta-Antila, S. [Univ. of Jyvaeskylae, Accelerator Lab., Dept. of Physics, Jyvaeskylae (Finland)

    2005-07-01

    The production of {sup 235}Np and {sup 236}Pu by the reactions {sup 236}U(p, 2n){sup 235}Np and {sup 236}U(p, n{beta}{sup -}){sup 236}Pu using the K-130 cyclotron of the University of Jyvaeskylaewas investigated. The cross sections for the reactions were determined. Thick-target yield curves were derived based on the cross sections. The results are discussed and compared with previous data on other reactions leading to the formation of the same end products. The thick-target yield of {sup 235}Np in the {sup 236}U(p, 2n) reaction is about 50 percent higher than the yield obtained in the {sup 238}U(p, 4n) reaction leading to this nuclide at comparable particle energies. The purity of {sup 236}Pu produced in the {sup 236}U(p, n{beta}{sup -}) reaction is more than ten times better than for earlier known as the purest reaction {sup 237}Np(p, 2n + pn{beta}{sup -}){sup 236}Pu. (orig.)

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2013-07-01

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

  17. Status report of the 1 MV AMS facility at the Centro Nacional de Aceleradores

    Energy Technology Data Exchange (ETDEWEB)

    Calvo, Elena Chamizo; Santos, Francisco Javier [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); López-Gutiérrez, José María [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); Dpto. de Física Aplicada I, Escuela Universitaria Politécnica, Universidad de Sevilla. Virgen de África 7, 41011 Seville (Spain); Padilla, Santiago [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); García-León, Manuel [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); Dpto. de Física Atómica Molecular y Nuclear, Universidad de Sevilla, Reina Mercedes s/n, 41012 Seville (Spain); Heinemeier, Jan [AMS 14C Dating Centre, Department of Physics and Astronomy, Aarhus University, Ny Munkegade 120, DK-8000 Aarhus C (Denmark); and others

    2015-10-15

    SARA (Spanish Accelerator for Radionuclides Analysis) was the first multielemental AMS facility installed in Spain in 2005. Since then it has been dedicated to the routine analysis of several radionuclides, such as {sup 10}Be, {sup 14}C, {sup 26}Al, {sup 129}I and Pu isotopes. Tests have been carried out with other isotopes, such as {sup 41}Ca, {sup 236}U and {sup 237}Np, and several changes have been made to the original facility to improve performance. First, an upgraded version of the ion source SO-110 has allowed us more stable measurement conditions for volatile elements (i.e. iodine), and a better general performance. Besides, changes in the target geometry have improved the ionization efficiency and long-term stability of the source output. Moreover, different software upgrades have been introduced to meet our routine operational needs. Finally, changing the movable Faraday-cup associated electronics now allows the measurement of smaller currents (in the range of pA), which has been key for the study of {sup 236}U/{sup 238}U atomic ratio in environmental samples. Apart from these modifications it has to be noted that routine radiocarbon measurements have been moved to a Micadas system (200 kV) installed at CNA in 2012. In this paper we will illustrate the evolution of the facility up to now, and our future prospects will be introduced.

  18. Anthropogenic radionuclides in the environment

    Energy Technology Data Exchange (ETDEWEB)

    Hu, Q; Weng, J; Wang, J

    2007-11-15

    Studies of radionuclides in the environment have entered a new era with the renaissance of nuclear energy and associated fuel reprocessing, geological disposal of high-level nuclear wastes, and concerns about national security with respect to nuclear non-proliferation. This work presents an overview of anthropogenic radionuclide contamination in the environment, as well as the salient geochemical behavior of important radionuclides. We first discuss the following major anthropogenic sources and current development that contribute to the radionuclide contamination of the environment: (1) nuclear weapons program; (2) nuclear weapons testing; (3) nuclear power plants; (4) commercial fuel reprocessing; (5) geological repository of high-level nuclear wastes, and (6) nuclear accidents. Then, we summarize the geochemical behavior for radionuclides {sup 99}Tc, {sup 129}I, and {sup 237}Np, because of their complex geochemical behavior, long half-lives, and presumably high mobility in the environment. Biogeochemical cycling and environment risk assessment must take into account speciation of these redox-sensitive radionuclides.

  19. Th and U fuel photofission study by NTD for AD-MSR subcritical assembly

    Science.gov (United States)

    Sajo-Bohus, Laszlo; Greaves, Eduardo D.; Davila, Jesus; Barros, Haydn; Pino, Felix; Barrera, Maria T.; Farina, Fulvio

    2015-07-01

    During the last decade a considerable effort has been devoted for developing energy generating systems based on advanced nuclear technology within the design concepts of GEN-IV. Thorium base fuel systems such as accelerator driven nuclear reactors are one of the often mentioned attractive and affordable options. Several radiotherapy linear accelerators are on the market and due to their reliability, they could be employed as drivers for subcritical liquid fuel assemblies. Bremsstrahlung photons with energies above 5.5MeV, induce (γ,n) and (e,e'n) reactions in the W-target. Resulting gamma radiation and photo or fission neutrons may be absorbed in target materials such as thorium and uranium isotopes to induce sustained fission or nuclear transmutation in waste radioactive materials. Relevant photo driven and photo-fission reaction cross sections are important for actinides 232Th, 238U and 237Np in the radiotherapy machines energy range of 10-20 MV. In this study we employ passive nuclear track detectors (NTD) to determine fission rates and neutron production rates with the aim to establish the feasibility for gamma and photo-neutron driven subcritical assemblies. To cope with these objectives a 20 MV radiotherapy machine has been employed with a mixed fuel target. Results will support further development for a subcritical assembly employing a thorium containing liquid fuel. It is expected that acquired technological knowledge will contribute to the Venezuelan nuclear energy program.

  20. Measurement of cross-sections of fission reactions induced by neutrons on actinides from the thorium cycle at n-TOF facility; Mesures de sections efficaces de fission induite par neutrons sur des actinides du cycle du thorium a n-TOF

    Energy Technology Data Exchange (ETDEWEB)

    Ferrant, L

    2005-09-01

    In the frame of innovating energy source system studies, thorium fuel cycle reactors are considered. Neutron induced fission cross section on such cycle involved actinides play a role in scenario studies. To feed them, data bases are built with experimental results and nuclear models. For some nuclei, they are not complete or in disagreement. In order to complete these data bases, we have built an original set up, consisting in an alternation of PPACs (Parallel Plate Avalanche Chamber) and ultra - thin targets, which we installed on n-TOF facility. We describe detectors, set up, and the particular care brought to target making and characterization. Fission products in coincidence are detected with precise time measurement and localization with delay line read out method. We contributed, within the n-TOF collaboration, to the CERN brand new intense spallation neutron source characterization, based on time of flight measurement, and we describe its characteristics and performances. We were able to measure such actinide fission cross sections as {sup 232}Th, {sup 234}U, {sup 233}U, {sup 237}Np, {sup 209}Bi, and {sup nat}Pb relative to {sup 235}U et {sup 238}U standards, using an innovative acquisition system. We took advantage of the lame accessible energy field, from 0.7 eV to 1 GeV, combined with the excellent energy resolution in this field. Data treatment and analysis advancement are described to enlighten performance and limits of the obtained results. (author)

  1. Single-pass continuous-flow leach test of PNL 76-68 glass: some selected Bead Leach I results

    Energy Technology Data Exchange (ETDEWEB)

    Coles, D.G.

    1981-01-22

    A single-pass continuous-flow leach test of PNL 76-68 glass beads (7 mm dia) was concluded after 420 days of uninterrupted operation. Variables included in the experimental matrix were flow-rate, leachant composition, and temperature. Analysis was conducted on all leachate samples for /sup 237/Np and /sup 239/Pu as well as a number of nonradioactive elements. Results indicated that flow-rate and leachant systematically affected the leach rate, but only slightly. Temperature effects were significant. Plutonium leach rate was lower at higher temperature suggesting that Pu sorption onto the beads was enhanced at the higher temperature. The range of leach rates for all analyzed elements (except Pu), at both temperature, at all three flow rates, and with all three leachant compositions varied only three orders of magnitude. The range of variables used in this experiment covered those expected in many proposed repository environments. The preliminary interpretation of the results also indicated that matrix dissolution may be the dominant leaching mechanism, at least for Np in bicarbonate leachant. Regardless of the leaching mechanism the importance of this study is that it bounds the effects of repository environments when the ground water is oxidizing and when it doesn't reach the waste form until the waste has cooled to ambient rock temperature.

  2. Semianalytical solutions of radioactive or reactive tracer transport in layered fractured media

    Energy Technology Data Exchange (ETDEWEB)

    Moridis, G.J.; Bodvarsson, G.S.

    2001-10-10

    In this paper, semianalytical solutions are developed for the problem of transport of radioactive or reactive tracers (solutes or colloids) through a layered system of heterogeneous fractured media with misaligned fractures. The tracer transport equations in the matrix account for (a) diffusion, (b) surface diffusion (for solutes only), (c) mass transfer between the mobile and immobile water fractions, (d) linear kinetic or equilibrium physical, chemical, or combined solute sorption or colloid filtration, and (e) radioactive decay or first order chemical reactions. Any number of radioactive decay daughter products (or products of a linear, first-order reaction chain) can be tracked. The tracer-transport equations in the fractures account for the same processes, in addition to advection and hydrodynamic dispersion. Additionally, the colloid transport equations account for straining and velocity adjustments related to the colloidal size. The solutions, which are analytical in the Laplace space, are numerically inverted to provide the solution in time and can accommodate any number of fractured and/or porous layers. The solutions are verified using analytical solutions for limiting cases of solute and colloid transport through fractured and porous media. The effect of important parameters on the transport of {sup 3}H, {sup 237}Np and {sup 239}Pu (and its daughters) is investigated in several test problems involving layered geological systems of varying complexity. {sup 239}Pu colloid transport problems in multilayered systems indicate significant colloid accumulations at straining interfaces but much faster transport of the colloid than the corresponding strongly sorbing solute species.

  3. LOS ALAMOS NEUTRON SCIENCE CENTER CONTRIBUTIONS TO THE DEVELOPMENT OF FUTURE POWER REACTORS

    Energy Technology Data Exchange (ETDEWEB)

    GAVRON, VICTOR I. [Los Alamos National Laboratory; HILL, TONY S. [Los Alamos National Laboratory; PITCHER, ERIC J. [Los Alamos National Laboratory; TOVESSON, FREDERIK K. [Los Alamos National Laboratory

    2007-01-09

    The Los Alamos Neutron Science Center (LANSCE) is a large spallation neutron complex centered around an 800 MeV high-currently proton accelerator. Existing facilities include a highly-moderated neutron facility (Lujan Center) where neutrons between thermal and keV energies are produced, and the Weapons Neutron Research Center (WNR), where a bare spallation target produces neutrons between 0.1 and several hundred MeV.The LANSCE facility offers a unique capability to provide high precision nuclear data over a large energy region, including that for fast reactor systems. In an ongoing experimental program the fission and capture cross sections are being measured for a number of minor actinides relevant for Generation-IV reactors and transmutation technology. Fission experiments makes use of both the highly moderated spallation neutron spectrum at the Lujan Center, and the unmoderated high energy spectrum at WNR. By combininb measurements at these two facilities the differential fission cross section is measured relative to the {sup 235}U(n,f) standard from subthermal energies up to about 200 MeV. An elaborate data acquisition system is designed to deal with all the different types of background present when spanning 10 energy decades. The first isotope to be measured was {sup 237}Np, and the results were used to improve the current ENDF/B-VII evaluation. Partial results have also been obtained for {sup 240}Pu and {sup 242}Pu, and the final results are expected shortly. Capture cross sections are measured at LANSCE using the Detector for Advanced Neutron Capture Experiments (DANCE). This unique instrument is highly efficient in detecting radiative capture events, and can thus handle radioactive samples of half-lives as low as 100 years. A number of capture cross sections important to fast reaction applications have been measured with DANCE. The first measurement was on {sup 237}Np(n,{gamma}), and the results have been submitted for publication. Other capture

  4. Plutonium, Mineralogy and Radiation Effects

    Science.gov (United States)

    Ewing, R. C.

    2006-05-01

    During the past fifty years, more than 1,800 metric tonnes of Pu and substantial quantities of other "minor" actinides, such as Np, Am and Cm, have been generated in nuclear reactors. Some of these transuranic elements can be a source of energy in fission reactions (e.g., 239Pu), a source of fissile material for nuclear weapons (e.g., 239Pu and 237Np), or are of environmental concern because of their long half- lives and radiotoxicity (e.g., 239Pu, t1/2 = 24,100 years, and 237Np, t1/2 = 2.1 million years). There are two basic strategies for the disposition of these elements: 1.) to "burn" or transmute the actinides using nuclear reactors or accelerators; 2.) to "sequester" the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, such as zircon or isometric pyrochlore, A2B2O7 (A = rare earths; B = Ti, Zr, Sn, Hf; Fd3m; Z=8), for the immobilization of actinides, particularly plutonium. One of the principal concerns has been the accumulation of structural damage caused by alpha-decay events, particularly from the recoil nucleus. Systematic ion beam irradiation studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high fluences of alpha-decay event damage. Some compositions, Gd2Ti2O7, are amorphized at relatively low doses (0.2 displacements per atom, dpa, at room temperature), while other compositions, Gd2Zr2O7, do not amorphize (even at doses of > 40 dpa at 25K), but instead disorder to a defect fluorite structure. By changing the composition of the A-site (e.g., substitution of different rare earth elements), the temperature above which the pyrochlore composition can no longer be amorphized, Tc, varies by >600 K (e.g., Lu2Ti2O7: Tc = 480 K; Gd2Ti2O7: Tc = 1120 K). The variation in response to irradiation as a function of composition can be used to model the long

  5. Development of an ultra-sensitive detection method for transuranium elements with respect to ocean water samples from Fukushima

    Energy Technology Data Exchange (ETDEWEB)

    Hain, Karin Margarete

    2016-03-30

    The development of a detection method for the identification of a possible emission of actinides into the Pacific Ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, was the major aim of this PhD thesis. It is shown in this work that in addition to the isotopic plutonium ratio {sup 240}Pu/{sup 239}Pu, which is an important signature for different contamination sources, the {sup 241}Pu/{sup 239}Pu ratio has to be determined, to distinguish between a Fukushima entry of actinides and nuclear weapon fallout in the Pacific Ocean. Furthermore, this study was aiming for the improvement of the data on the neptunium ({sup 237}Np) distribution in the ocean. For the detection of the trace concentrations of actinides in the order of mBq/m{sup 3} in a small sample volume of 20 L ocean water, the ultra-sensitive method accelerator mass spectrometry (AMS) was chosen. A chemical separation procedure for Pu and Np based on extraction chromatography was developed using mass spectrometry and radiometric analysis to determine the chemical recovery. {sup 241}Am, which causes isobaric background to {sup 241}Pu in mass spectrometric measurements, was separated with a suppression of at least 10{sup -4} from Pu by this method. The detection method adjusted to Pu and Np was successfully verified by analyzing the concentration of Pu in certified reference material with AMS at the Maier-Leibnitz-Laboratory (MLL) in Munich. Due to a temporary closure of the MLL, 12 sea water samples, collected in autumn 2012, were prepared at the Radiochemie Muenchen and measured at the Vienna Environmental Research Laboratory (VERA). The sampling station closest to the FDNPP was located at a distance of 39.6 km. Three of the samples showed a slightly elevated {sup 240}Pu/{sup 239}Pu ratio of up to 0.23{sup +0.04}{sub -0.03} compared to global fallout ({sup 240}Pu/{sup 239}Pu = 0.180±0.007), whereas all measured {sup 241}Pu/{sup 239}Pu ratios were clearly consistent with nuclear weapon

  6. A comparison between the example reference biosphere model ERB 2B and a process-based model: simulation of a natural release scenario.

    Science.gov (United States)

    Almahayni, T

    2014-12-01

    The BIOMASS methodology was developed with the objective of constructing defensible assessment biospheres for assessing potential radiological impacts of radioactive waste repositories. To this end, a set of Example Reference Biospheres were developed to demonstrate the use of the methodology and to provide an international point of reference. In this paper, the performance of the Example Reference Biosphere model ERB 2B associated with the natural release scenario, discharge of contaminated groundwater to the surface environment, was evaluated by comparing its long-term projections of radionuclide dynamics and distribution in a soil-plant system to those of a process-based, transient advection-dispersion model (AD). The models were parametrised with data characteristic of a typical rainfed winter wheat crop grown on a sandy loam soil under temperate climate conditions. Three safety-relevant radionuclides, (99)Tc, (129)I and (237)Np with different degree of sorption were selected for the study. Although the models were driven by the same hydraulic (soil moisture content and water fluxes) and radiological (Kds) input data, their projections were remarkably different. On one hand, both models were able to capture short and long-term variation in activity concentration in the subsoil compartment. On the other hand, the Reference Biosphere model did not project any radionuclide accumulation in the topsoil and crop compartments. This behaviour would underestimate the radiological exposure under natural release scenarios. The results highlight the potential role deep roots play in soil-to-plant transfer under a natural release scenario where radionuclides are released into the subsoil. When considering the relative activity and root depth profiles within the soil column, much of the radioactivity was taken up into the crop from the subsoil compartment. Further improvements were suggested to address the limitations of the Reference Biosphere model presented in this paper.

  7. Actinide partitioning and transmutation program. Progress report, July 1--September 30, 1977

    Energy Technology Data Exchange (ETDEWEB)

    Tedder, D.W.; Blomeke, J.O. (comps.)

    1978-02-01

    In Purex process modifications, two cold runs with mixer-settlers were made on the extraction and stripping of ruthenium and zirconium without the presence of uranium. Efforts in actinide recovery from solids were directed toward the determination of dissolution parameters in various reagents for /sup 241/Am and /sup 239/Pu oxide mixtures, /sup 233/U oxide, /sup 237/Np oxide, /sup 244/Cm oxide, /sup 232/Th oxide, and PuO/sub 2/. Studies in americium-curium recovery with OPIX (oxalate precipitation and ion exchange), Talspeak, and cation exchange chromatography focused on the feasibility of forming oxalate precipitates in continuous systems, the effects of zirconium on Talspeak, and methods for removing solvent degradation products of the Talspeak system. In studies of americium-curium recovery using bidentate extractants, additional distribution coefficients for actinides and other key elements between reduced synthetic LWR waste solution and 30 percent dihexyl-N, N-diethyl-carbamylmethylene phosphonate in diisopropylbenzene were measured. Studies in the americium-curium recovery using inorganic ion exchange media to determine the pH dependence of lanthanide ion affinity for niobate, titanate, and zirconate ion exchange materials have been completed. A modified flowsheet for the extraction of uranium, neptunium, plutonium, americium, and curium from high-level liquid waste is presented. Evaluation of methods for measuring actinides from incinerator ash is continuing. A preliminary evaluation of methods for treatment of salt waste and waste waters was completed. In thermal reactor transmutation studies, waste actinides from an LWR lattice containing mixed uranium-plutonium assemblies were recycled in separate target assemblies. (LK)

  8. Update to Assessment of Direct Disposal in Unsaturated Tuff of Spent Nuclear Fuel and High-Level Waste Owned by U.S. Department of Energy

    Energy Technology Data Exchange (ETDEWEB)

    P. D. Wheatley (INEEL POC); R. P. Rechard (SNL)

    1998-09-01

    The overall purpose of this study is to provide information and guidance to the Office of Environmental Management of the U.S. Department of Energy (DOE) about the level of characterization necessary to dispose of DOE-owned spent nuclear fuel (SNF). The disposal option modeled was codisposal of DOE SNF with defense high-level waste (DHLW). A specific goal was to demonstrate the influence of DOE SNF, expected to be minor, in a predominately commercial repository using modeling conditions similar to those currently assumed by the Yucca Mountain Project (YMP). A performance assessment (PA) was chosen as the method of analysis. The performance metric for this analysis (referred to as the 1997 PA) was dose to an individual; the time period of interest was 100,000 yr. Results indicated that cumulative releases of 99Tc and 237Np (primary contributors to human dose) from commercial SNF exceed those of DOE SNF both on a per MTHM and per package basis. Thus, if commercial SNF can meet regulatory performance criteria for dose to an individual, then the DOE SNF can also meet the criteria. This result is due in large part to lower burnup of the DOE SNF (less time for irradiation) and to the DOE SNF's small percentage of the total activity (1.5%) and mass (3.8%) of waste in the potential repository. Consistent with the analyses performed for the YMP, the 1997 PA assumed all cladding as failed, which also contributed to the relatively poor performance of commercial SNF compared to DOE SNF.

  9. Fabrication and characterization of MCC approved testing material - ATM-12 glass

    Energy Technology Data Exchange (ETDEWEB)

    Wald, J.W.

    1985-10-01

    The Materials Characterization Center (MCC) Approved Testing Material ATM-12 is a borosilicate glass that incorporates elements typical of high-level waste (HLW) resulting from the reprocessing of commercial nuclear reactor fuels. The composition has been adjusted to match that predicted for HLW type 76-68 glass at an age of 300 y. Radioactive constituents contained in this glass include depleted uranium, {sup 99}Tc, {sup 237}Np, {sup 239}Pu, and {sup 241}Am. The glass was produced by the MCC at the Pacific Northwest Laboratory (PNL). ATM-12 glass ws produced from July to November of 1984 at the request of the Nevada Nuclear Waste Site Investigations (NNWSI) Program and is the third in a series of glasses produced for NNWSI. Most of the glass produced was in the form of cast bars; special castings and crushed material were also produced. Three kilograms of ATM-12 glass were produced from a feedstock melted in a nitrogen-atmosphere glove box at 1150{sup 0}C in a platinum crucible, and formed into stress-annealed rectangular bars and the special casting shapes requested by NNWSI. Bars of ATM-12 were nominally 1.9 x 1.9 x 10 cm, with an average mass of 111 g each. Nineteen bars and 37 special castings were made. ATM-12 glass has been provided to the NNWSI Program, in the form of bars, crushed powder and special castings. As of August 1985 approximately 590 g of ATM-12 is available for distribution. Requests for materials or services related to this glass should be directed to the Materials Characterization Center Program Office, PNL.

  10. Measurements of {beta} or {alpha} emitter long lived radionuclides using inductively coupled plasma mass spectrometry; Dosage a tres bas niveau de radionucleides a longue periode emetteurs {beta} ou {alpha} par spectrometrie de masse a couplage plasma inductif

    Energy Technology Data Exchange (ETDEWEB)

    Provitina, O.

    1993-10-18

    The measurement of long-lived radionuclides is highly important for characterizing nuclear wastes for their later storage. The main techniques are {alpha} spectrometry, {beta} counting and {gamma} spectrometry. The large period of these isotopes leads to low specific activity needing time consuming measurements. Moreover, the radiometric techniques are often limited by problems of interferences involving several steps of pretreatments. Among these steps, the specific extraction with crown ethers is highly selective for the separation of {sup 99}Tc, {sup 129}I and {sup 135}Cs. The radiometric techniques are here replaced by inductively coupled plasma mass spectroscopy (ICP-MS) the advantages of which are: few interferences, sensitivity which does not depend on the radiologic period as compared to radiochemistry. ICP-MS can then measure {sup 237}Np in enriched uranium matrix and reduce by a factor of 4 the sample pretreatment and the duration of the analysis usually performed by {alpha} spectrometry. Another technique, electrothermal vaporization (ETV), is consequently used. Crown ether extraction-ETV-ICP-MS is employed for measuring the long lived radionuclides {sup 99}Tc and {sup 129}I. The conditions of the extraction and the parameters of the ETV and the ICP-MS are studied and optimized. The methods optimized (extraction, electrothermal vaporization) are validated in the case of {sup 99}Tc, in real samples. The spike method is required to quantify technetium, the quantification with calibration leading to bad results. The results obtained are in good agreement with the expected values. Extraction of technetium on anionic resin and its measurement by the spike method with pneumatic nebulization-ICP-MS is also performed on other samples. Measured values are also in agreement with expected values, but the method of extraction is more time consuming (half a day) than the extraction with crown ether (one hour). (author). 54 figs., 38 tabs.

  11. TANGRA-Setup for the Investigation of Nuclear Fission Induced by 14.1 MeV Neutrons

    Science.gov (United States)

    Ruskov, I. N.; Kopatch, Yu. N.; Bystritsky, V. M.; Skoy, V. R.; Shvetsov, V. N.; Hambsch, F.-J.; Oberstedt, S.; Noy, R. Capote; Sedyshev, P. V.; Grozdanov, D. N.; Ivanov, I. Zh.; Aleksakhin, V. Yu.; Bogolubov, E. P.; Barmakov, Yu. N.; Khabarov, S. V.; Krasnoperov, A. V.; Krylov, A. R.; Obhođaš, J.; Pikelner, L. B.; Rapatskiy, V. L.; Rogachev, A. V.; Rogov, Yu. N.; Ryzhkov, V. I.; Sadovsky, A. B.; Salmin, R. A.; Sapozhnikov, M. G.; Slepnev, V. M.; Sudac, D.; Tarasov, O. G.; Valković, V.; Yurkov, D. I.; Zamyatin, N. I.; Zeynalov, Sh. S.; Zontikov, A. O.; Zubarev, E. V.

    The new experimental setup TANGRA (Tagged Neutrons & Gamma Rays), for the investigation of neutron induced nuclear reactions, e.g. (n,xn'), (n,xn'γ), (n,γ), (n,f), on a number of important isotopes for nuclear science and engineering (235,238U, 237Np, 239Pu, 244,245,248Cm) is under construction and being tested at the Frank Laboratory of Neutron Physics (FLNP) of the Joint Institute for Nuclear Research (JINR) in Dubna. The TANGRA setup consists of: a portable neutron generator ING-27, with a 64-pixel Si charge-particle detector incorporated into its vacuum chamber for registering of α-particles formed in the T(d, n)4He reaction, as a source of 14.1 MeV steady-state neutrons radiation with an intensity of ∼5x107n/s; a combined iron (Fe), borated polyethylene (BPE) and lead (Pb) compact shielding-collimator; a reconfigurable multi-detector (neutron plus gamma ray detecting system); a fast computer with 2 (x16 channels) PCI-E 100 MHz ADC cards for data acquisition and hard disk storage; Linux ROOT data acquisition, visualization and analysis software. The signals from the α-particle detector are used to 'tag' the neutrons with the coincident α-particles. Counting the coincidences between the α-particle and the reaction-product detectors in a 20ns time-interval improves the effect/background-ratio by a factor of ∼200 as well as the accuracy in the neutron flux determination, which decreases noticeably the overall experimental data uncertainty.

  12. Fission neutron spectra measurements at LANSCE - status and plans

    Energy Technology Data Exchange (ETDEWEB)

    Haight, Robert C [Los Alamos National Laboratory; Noda, Shusaku [Los Alamos National Laboratory; Nelson, Ronald O [Los Alamos National Laboratory; O' Donnell, John M [Los Alamos National Laboratory; Devlin, Matt [Los Alamos National Laboratory; Chatillon, Audrey [CEA-FRANCE; Granier, Thierry [CEA-FRANCE; Taieb, Julien [CEA-FRANCE; Laurent, Benoit [CEA-FRANCE; Belier, Gilbert [CEA-FRANCE; Becker, John A [LLNL; Wu, Ching - Yen [LLNL

    2009-01-01

    A program to measure fission neutron spectra from neutron-induced fission of actinides is underway at the Los Alamos Neutron Science Center (LANSCE) in a collaboration among the CEA laboratory at Bruyeres-le-Chatel, Lawrence Livermore National Laboratory and Los Alamos National Laboratory. The spallation source of fast neutrons at LANSCE is used to provide incident neutron energies from less than 1 MeV to 100 MeV or higher. The fission events take place in a gas-ionization fission chamber, and the time of flight from the neutron source to that chamber gives the energy of the incident neutron. Outgoing neutrons are detected by an array of organic liquid scintillator neutron detectors, and their energies are deduced from the time of flight from the fission chamber to the neutron detector. Measurements have been made of the fission neutrons from fission of {sup 235}U, {sup 238}U, {sup 237}Np and {sup 239}Pu. The range of outgoing energies measured so far is from 1 MeV to approximately 8 MeV. These partial spectra and average fission neutron energies are compared with evaluated data and with models of fission neutron emission. Results to date will be presented and a discussion of uncertainties will be given in this presentation. Future plans are to make significant improvements in the fission chambers, neutron detectors, signal processing, data acquisition and the experimental environment to provide high fidelity data including mea urements of fission neutrons below 1 MeV and improvements in the data above 8 MeV.

  13. Hazards analysis for the E.O. Lawrence Berkeley National Laboratory x-ray absorption experiments to be performed at Stanford Synchrotron Radiation Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Edelstein, N.M.; Shuh, D.K.; Bucher, J.B. [Lawrence Berkeley National Lab., CA (United States). Chemical Sciences Div.

    1995-04-01

    The objective of this experiment is to determine the oxidation state(s) of neptunium (Np) in mouse skeleton and in soft tissue by X-ray Absorption Near Edge Structure (XANES). If Np is present in sufficient concentration, X-ray Absorption Fine Structure (XAFS) data will be obtained in order to further identify the Np species present. These data will be crucial in understanding the metabolic pathway of Np in mammals which will help in the design of reagents which can eliminate Np from mammals in the event of accidental exposure. It is proposed to run these experiments at the Standard Synchrotron Radiation Laboratory (SSRL). This laboratory is a DOE national user facility located at the Stanford Linear Accelerator Center (SLAC). The {sup 237}Np nucleus decays by the emission of an alpha particle and this particle emission is the principal hazard in handling Np samples. This hazard is mitigated by physical containment of the sample which stops the alpha particles within the containment. The total amount of Np material that will be shipped to and be at SSRL at any one time will be less than 1 gram. This limit on the amount of Np will ensure that SLAC remains a low hazard, non-nuclear facility. The Np samples will be solids or Np ions in aqueous solution. The Np samples will be shipped to SSRL/SLAC OHP. SLAC OHP will inventory the samples and swipe the containers holding the triply contained samples, and then bring them to the SSRL Actinide trailer located outside building 131. The QA counting records from the samples, as measured at LBNL, will be provided to SSRL and SLAC OHP prior to the arrival of the samples at SLAC OHP. In addition, strict monitoring of the storage and experimental areas will be performed in accordance with SLAC/OHP radiation protection procedures to ensure against the release of contamination.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2004-12-01

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

  15. OSMOSE program : statistical review of oscillation measurements in the MINERVE reactor R1-UO2 configuration.

    Energy Technology Data Exchange (ETDEWEB)

    Stoven, G.; Klann, R.; Zhong, Z.; Nuclear Engineering Division

    2007-08-28

    The OSMOSE program is a collaboration on reactor physics experiments between the United States Department of Energy and the France Commissariat Energie Atomique. At the working level, it is a collaborative effort between the Argonne National Laboratory and the CEA Cadarache Research Center. The objective of this program is to measure very accurate integral reaction rates in representative spectra for the actinides important to future nuclear system designs, and to provide the experimental data for improving the basic nuclear data files. The main outcome of the OSMOSE measurement program will be an experimental database of reactivity-worth measurements in different neutron spectra for the heavy nuclides. This database can then be used as a benchmark to verify and validate reactor analysis codes. The OSMOSE program (Oscillation in Minerve of isotopes in Eupraxic Spectra) aims at improving neutronic predictions of advanced nuclear fuels through oscillation measurements in the MINERVE facility on samples containing the following separated actinides: {sup 232}Th, {sup 233}U, {sup 234}U, {sup 235}U, {sup 236}U, {sup 238}U, {sup 237}Np, {sup 238}Pu, {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu, {sup 241}Am, {sup 243}Am, {sup 244}Cm, and {sup 245}Cm. The first part of this report provides an overview of the experimental protocol and the typical processing of a series of experimental results which is currently performed at CEA-Cadarache. In the second part of the report, improvements to this technique are presented, as well as the program that was created to process oscillation measurement results from the MINERVE facility in the future.

  16. Probabilistic assessment of the influence of lake properties in long-term radiation doses to humans.

    Science.gov (United States)

    Pohjola, Jari; Turunen, Jari; Lipping, Tarmo; Ikonen, Ari T K

    2016-11-01

    The assessment processes concerning the safety of nuclear waste repositories include the modelling of radionuclide transport in biosphere and the evaluation of the doses to the most affected humans. In this paper, a scenario, in which a contaminated lake is the water source for drinking water, irrigation water and watering of livestock, is presented. The objective of the paper is to probabilistically study the influence of lake properties as parameters in the assessment scenario. The properties of the lake are a result of previously conducted probabilistic studies, where the land uplift of the terrain surrounding the repositories and the formation of water bodies were studied in a 10,000-year time span using Monte Carlo simulation. The lake is formed at 3000 years from present day and the changing properties of the lake have been used in the study. The studied radionuclides (36)Cl, (135)Cs, (129)I, (237)Np, (90)Sr, (99)Tc and (238)U enter the lake with a rate of 1 Bq/year. The transport process from the lake water to humans is described and the doses (dose conversion factors) to adult humans are evaluated based on a study on average food consumption. Sensitivity analysis is used for identifying the parameters having the most influence on the outcome of the dose. Based on the results from the sensitivity analysis, the volumetric outflow rate of the lake and the volume of the lake were taken into closer consideration. The results show the influence of probabilistically derived geomorphic lake input parameters on the dose. Copyright © 2016 Elsevier Ltd. All rights reserved.

  17. Validation of minor actinides fission neutron cross-sections

    Directory of Open Access Journals (Sweden)

    Pešić Milan P.

    2015-01-01

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

  18. Cumulative fission yields of short-lived isotopes under natural-abundance-boron-carbide-moderated neutron spectrum

    Energy Technology Data Exchange (ETDEWEB)

    Finn, Erin C.; Metz, Lori A.; Greenwood, Lawrence R.; Pierson, Bruce; Wittman, Richard S.; Friese, Judah I.; Kephart, Rosara F.

    2015-04-09

    The availability of gamma spectroscopy data on samples containing mixed fission products at short times after irradiation is limited. Due to this limitation, data interpretation methods for gamma spectra of mixed fission product samples, where the individual fission products have not been chemically isolated from interferences, are not well-developed. The limitation is particularly pronounced for fast pooled neutron spectra because of the lack of available fast reactors in the United States. Samples containing the actinide isotopes 233, 235, 238U, 237Np, and 239Pu individually were subjected to a 2$ pulse in the Washington State University 1 MW TRIGA reactor. To achieve a fission-energy neutron spectrum, the spectrum was tailored using a natural abundance boron carbide capsule to absorb neutrons in the thermal and epithermal region of the spectrum. Our tailored neutron spectrum is unique to the WSU reactor facility, consisting of a soft fission spectrum that contains some measurable flux in the resonance region. This results in a neutron spectrum at greater than 0.1 keV with an average energy of 70 keV, similar to fast reactor spectra and approaching that of 235U fission. Unique fission product gamma spectra were collected from 4 minutes to 1 week after fission using single-crystal high purity germanium detectors. Cumulative fission product yields measured in the current work generally agree with published fast pooled fission product yield values from ENDF/B-VII, though a bias was noted for 239Pu. The present work contributes to the compilation of energy-resolved fission product yield nuclear data for nuclear forensic purposes.

  19. Partitioning of the rare earths and actinides between R7T7 nuclear glass alteration products and solution according to disposal conditions; Partage des terres rares et des actinides entre solution et produits d`alteration du verre nucleaire type R7T7 en fonction des conditions de stockage

    Energy Technology Data Exchange (ETDEWEB)

    Menard, O.

    1995-10-25

    The alteration of nuclear glass by water is liable to release radionuclides into the environment. Determining the release kinetics of these elements and their aqueous chemical forms are therefore essential steps in establishing the safety of a geological repository site. Leach tests were conducted with a nonradioactive specimen of the French ``R7T7`` light water containment glass spiked with U and Th, and with two R7T7 specimens spiked with {sup 237}Np and {sup 239}Pu, respectively. The alteration solution compositions were representative of deep groundwater and contained carbonate, sulfate, phosphate, fluorine and chlorine ions. The release of U, Th, Np and Pu, as well as of the rare earths La, Ce and Nd were monitored by ICP mass spectrometry and by {alpha} spectrometry. Scanning and transmission electron microscopic examination of the nonradioactive altered glass surfaces was also performed to assess the partitioning balance for the rare earths, U and Th between the glass alteration products and solution. The mobility of these elements depends on two competing mechanisms. The rare earths and thorium are incorporated in the alteration products (gel); the retention process is assumed to involve chemisorption or coprecipitation, enhanced in the gel layer by the presence of phosphate ions in particular. Conversely, the aqueous species in the alteration solutions (mainly anions) form complexes with the actinides and rare earths; this phenomenon is particularly evident with U and Np. The presence of carbonate ions favors this mobility. Plutonium differs from U and Np in that it is adsorbed mainly on colloids formed by glass dissolution, the principal factors governing its chemical evolution in solution. (author). refs., 122 figs., 185 tabs.

  20. Radionuclide reactions with groundwater and basalts from Columbia River basalt formations

    Energy Technology Data Exchange (ETDEWEB)

    Barney, G.S.

    1981-06-01

    Chemical reactions of radionuclides with geologic materials found in Columbia River basalt formations were studied. The objective was to determine the ability of these formations to retard radionuclide migration from a radioactive waste repository located in deep basalt. Reactions that can influence migration are precipitation, ion-exchange, complexation, and oxidation-reduction. These reactions were studied by measuring the effects of groundwater composition and redox potential (Eh) on radionuclide sorption on fresh basalt surfaces, a naturally altered basalt, and a sample of secondary minerals associated with a Columbia River basalt flow. In addition, radionuclide sorption isotherms were measured for these materials and reaction kinetics were determined. The radionuclides studied were /sup 137/Cs, /sup 85/Sr, /sup 75/Se, /sup 95m/Tc, /sup 237/Np, /sup 241/Am, /sup 226/Ra and /sup 237/Pu. The Freundlich equation accurately describes the isotherms when precipitation of radionuclides does not occur. In general, sorption increased in the order: basalt < altered basalt < secondary minerals. This increase in sorption corresponds to increasing surface area and cation exchange capacity. The Eh of the system had a large effect on technetium, plutonium, and neptunium sorption. Technetium(VII), Pu(VI), and Np(V) are reduced to Tc(IV), Pu(IV), and Np(IV), respectively, under Eh conditions expected in deep basalt formations. The kinetics of radionuclide sorption and basalt-groundwater reactions were observed over a period of 18 weeks. Most sorption reactions stabilized after about four weeks. Groundwater composition changed the least in contact with altered basalt. Contact with secondary minerals greatly increased Ca, K, and Mg concentrations in the groundwater.

  1. Set up of an innovative methodology to measure on-line the incineration potential of minor actinides under very high neutron sources in the frame of the future prospects of the nuclear waste transmutation; Mise au point d'une methodologie innovante pour la mesure du potentiel d'incineration d'actinides mineurs sous des sources tres intenses de neutrons, dans la perspective de transmutation des dechets nucleaires

    Energy Technology Data Exchange (ETDEWEB)

    Fadil, M

    2003-03-01

    This work deals generally with the problem of nuclear waste management and especially with the transmutation of it to reduce considerably its radiotoxicity potential. The principal objective of this thesis is to show the feasibility to measure on-line the incineration potential of minor actinides irradiated under very high neutron flux. To realize this goal, we have developed fission micro-chambers able to operate, for the first time in the world, in saturation regime under a severe neutron flux. These new chambers use {sup 235}U as an active deposit. They were irradiated in the high flux reactor at Laue-Langevin Institute in Grenoble. The measurement of the saturation current delivered by these chambers during their irradiation for 26 days allowed to evaluate the burn-up of {sup 235}U. We have determined the neutron flux intensity of 1,6 10{sup 15} n.cm{sup -2}.s{sup -1} in the bottom of the irradiation tube called 'V4'. The relative uncertainty of this value is less than 4 %. This is for the first time that such high neutron flux is measured with a fission chamber. To confirm this result, we have also performed independent measurements using gamma spectroscopy of irradiated Nb and Co samples. Both results are in agreement within error bars. Simple Deposit Fission Chambers (SDFC) as above were the reference of the new generation of fission chambers that we have developed in the framework of this thesis: Double Deposit Fission Chambers (DDFC). The reference active deposit was {sup 235}U. The other deposit was the actinide that we wanted to study (e.g. {sup 237}Np and {sup 241}Am). At the end of the thesis, we present some suggestions to ameliorate the operation of the DDFC to be exploited in other transmutation applications in the future. (author)

  2. Water Sorption and Radiolysis Studies for Neptunium Oxides

    Energy Technology Data Exchange (ETDEWEB)

    Icenhour, A.S.

    2004-02-03

    Plans are to convert the {sup 237}Np that is currently stored as a nitrate solution at the Savannah River Site to NpO{sub 2} and then ship it to the Y-12 National Security Complex in Oak Ridge for interim storage. This material will serve as feedstock for the {sup 238}Pu production program, and some will be periodically shipped to the Oak Ridge National Laboratory (ORNL) for fabrication into targets. The safe storage of this material requires an understanding of the radiolysis of moisture that is sorbed on the oxides, which, in turn, provides a basis for storage criteria (namely, moisture content). A two-component experimental program has been undertaken at ORNL to evaluate the radiolytic effects on NpO{sub 2}: (1) moisture uptake experiments and (2) radiolysis experiments using both gamma and alpha radiation. These experiments have produced two key results. First, the water uptake experiments demonstrated that the 0.5 wt % moisture limit that has been typically established for similar materials (e.g., uranium and plutonium oxides) cannot be obtained in a practical environment. In fact, the uptake in a typical environment can be expected to be at least an order of magnitude lower than the limit. The second key result is the establishment of steady-state pressure plateaus as a result of the radiolysis of sorbed moisture. These plateaus are the result of back reactions that limit the overall pressure increase and H{sub 2} production. These results clearly demonstrate that 0.5 wt % H{sub 2}O on NpO{sub 2} is safe for long-term storage--if such a moisture content could even be practically reached.

  3. Annual progress report on nuclear data 1992

    Energy Technology Data Exchange (ETDEWEB)

    Hansen, H.H. [ed.

    1993-06-01

    This is the 1992 annual report on nuclear data from the Central Bureau for Nuclear Measurements, Geel (Belgium). Work on standard neutron cross sections included {sup 235}U(n,f)/H(n,n) with Frisch gridded ionization chambers and using octacosanol samples. Mass, energy, and angular distribution of fission fragments for {sup 237}Np(n,f) from 0.5 to 5.5 MeV neutron energy. Alpha decay probabilities of {sup 239}Pu. In the area of nuclear data for fission technology, a measurement on the normalization of the {sup 239}Pu fission cross sections was performed. Parameters for 384 resonances in {sup 58}Ni and 350 resonances in {sup 60}Ni have been analyzed up to 1 MeV and 800 KeV, respectively. In the field of nuclear data for fusion technology, double differential neutron emission cross sections for {sup 9}Be(n,2n) for incident neutron energies between 0. 6 and 11.1 MeV have been reported. Extensive measurements of the neutron decay cross sections of {sup 207}Pb have been made. In the radionuclide metrology subproject contributions were made by the preparation of low energy x-ray standard sources, measurements of K- shell fluorescence yields, standardization of a {sup 152}Eu solution, evaluation of the second EUROMET intercomparison of {sup 192}Ir brachytherapy sources, and low level measurements on volcanic rock, archeological ceramics, soil and river sediments. Work was also reported in neutron metrology, major facilities upgrades, radiation physics, and support for a number of PhD projects.

  4. ENHANCING ADVANCED CANDU PROLIFERATION RESISTANCE FUEL WITH MINOR ACTINIDES

    Energy Technology Data Exchange (ETDEWEB)

    Gray S. Chang

    2010-05-01

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

  5. Simultaneous photon and neutron interrogation using an electron accelerator in order to quantify actinides in encapsulated radioactive wastes; Double interrogation simultanee neutrons et photons utilisant un accelerateur d'electrons pour la caracterisation separee des actinides dans les dechets radioactifs enrobes

    Energy Technology Data Exchange (ETDEWEB)

    Jallu, F

    1999-09-24

    Measuring out alpha emitters, such as ({sup 234,235,236,238}U {sup 238,239,240,242,}2{sup 44P}u, {sup 237}Np {sup 241,243}Am...), in solid radioactive waste, allows us to quantify the alpha activity in a drum and then to classify it. The SIMPHONIE (SIMultaneous PHOton and Neutron Interrogation Experiment) method, developed in this Ph.D. work, combines both the Active Neutron Interrogation and the Induced Photofission Interrogation techniques simultaneously. Its purpose is to quantify in only one measurement, fissile ({sup 235}U, {sup 239,241}Pu...) and fertile ({sup 236,238}U, {sup 238,240}Pu...) elements separately. In the first chapter of this Ph.D. report, we present the principle of the Radioactive Waste Management in France. The second chapter deals with the physical properties of neutron fission and of photofission. These two nuclear reactions are the basis of the SIMPHONIE method. Moreover, one of our purposes was to develop the ELEPHANT (ELEctron PHoton And Neutron Transport) code in view to simulate the electron, photon and neutron transport, including the ({gamma}, n), ({gamma}, 2n) and ({gamma}, f) photonuclear reactions that are not taken into account in the MCNP4 (Monte Carlo N-Particle) code. The simulation codes developed and used in this work are detailed in the third chapter. Finally, the fourth chapter gives the experimental results of SIMPHONIE obtained by using the DGA/ETCA electron linear accelerators located at Arcueil, France. Fissile ({sup 235}U, {sup 239}Pu) and fertile ({sup 238}U) samples were studied. Furthermore, comparisons between experimental results and calculated data of photoneutron production in tungsten, copper, praseodymium and beryllium by using an electron LINear Accelerator (LINAC) are given. This allows us to evaluate the validity degree of the ELEPHANT code, and finally the feasibility of the SIMPHONIE method. (author)

  6. Study of calculated and measured time dependent delayed neutron yields. [TX, for calculating delayed neutron yields; MATINV, for matrix inversion; in FORTRAN for LSI-II minicomputer

    Energy Technology Data Exchange (ETDEWEB)

    Waldo, R.W.

    1980-05-01

    Time-dependent delayed neutron emission is of interest in reactor design, reactor dynamics, and nuclear physics studies. The delayed neutrons from neutron-induced fission of /sup 232/U, /sup 237/Np, /sup 238/Pu, /sup 241/Am, /sup 242m/Am, /sup 245/Cm, and /sup 249/Cf were studied for the first time. The delayed neutron emission from /sup 232/Th, /sup 233/U, /sup 235/U, /sup 238/U, /sup 239/Pu, /sup 241/Pu, and /sup 242/Pu were measured as well. The data were used to develop an empirical expression for the total delayed neutron yield. The expression gives accurate results for a large variety of nuclides from /sup 232/Th to /sup 252/Cf. The data measuring the decay of delayed neutrons with time were used to derive another empirical expression predicting the delayed neutron emission with time. It was found that nuclides with similar mass-to-charge ratios have similar decay patterns. Thus the relative decay pattern of one nuclide can be established by any measured nuclide with a similar mass-to-charge ratio. A simple fission product yield model was developed and applied to delayed neutron precursors. It accurately predicts observed yield and decay characteristics. In conclusion, it is possible to not only estimate the total delayed neutron yield for a given nuclide but the time-dependent nature of the delayed neutrons as well. Reactors utilizing recycled fuel or burning actinides are likely to have inventories of fissioning nuclides that have not been studied until now. The delayed neutrons from these nuclides can now be incorporated so that their influence on the stability and control of reactors can be delineated. 8 figures, 39 tables.

  7. Novel insights into Fukushima nuclear accident from isotopic evidence of plutonium spread along coastal rivers.

    Science.gov (United States)

    Evrard, Olivier; Pointurier, Fabien; Onda, Yuichi; Chartin, Caroline; Hubert, Amélie; Lepage, Hugo; Pottin, Anne-Claire; Lefèvre, Irène; Bonté, Philippe; Laceby, J Patrick; Ayrault, Sophie

    2014-08-19

    The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurements of Pu isotopic atom and activity ratios are required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we used a double-focusing sector field ICP-MS to measure Pu atom and activity ratios in recently deposited sediment along rivers draining the most contaminated part of the inland radioactive plume. Results showed that plutonium isotopes (i.e., (239)Pu, (240)Pu, (241)Pu, and (242)Pu) were detected in all samples, although in extremely low concentrations. The (241)Pu/(239)Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113 ± 0.00008 on average for the Northern Hemisphere between 31°-71° N: Kelley, J. M.; Bond, L. A.; Beasley, T. M. Global distribution of Pu isotopes and (237)Np. Sci. Total. Env. 1999, 237/238, 483-500). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout that represented up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (∼45 km) from FDNPP and been deposited in rivers representing a potential source of Pu to the ocean. In future, the high (241)Pu/(239)Pu atom ratio of the Fukushima accident sourced-Pu should be measured to quantify the supply of continental-originating material from Fukushima Prefecture to the Pacific Ocean.

  8. New Insights Into the Discoveries of Elements 113, 115 and 117

    Science.gov (United States)

    Oganessian, Yuri; Abdullin, Farid; Dmitriev, Sergey; Itkis, Mikhail; Polyakov, Alexandr; Sagaidak, Roman; Shirokovsky, Igor; Subbotin, Vladimir; Sukhov, Alexandr; Tsyganov, Yuri; Utyonkov, Vladimir; Voinov, Alexey; Vostokin, Grigory; Gostic, Julie; Henderson, Roger; Moody, Kenton; Shaughnessy, Dawn; Stoyer, Mark; Stoyer, Nancy; Hamilton, Joseph; Ramayya, Akunuri; Roberto, James; Rykaczewski, Krzysztof

    2013-06-01

    The discovery of new higher Z elements and the determination of their decay properties provide important insights into our understandings of the behaviour of nuclear matter under extreme conditions of high Z and important tests of the prediction of an island of stability around N=184 and high Z (114 or even 120-126). The synthesis of odd-Z superheavy nuclei provides more detailed information than even-Z nuclei about the nuclear structure of these nuclides because of their longer decay chains as a result of strong fission hindrance caused by the unpaired nucleons. For the first time the Z=115 nuclei and their odd-Z decay products including Z=113 isotopes were observed in 2003 [1,2]. Three decay chains of 288115 284113 280Rg ...268Db and one decay chain of 287115 283113 279Rg ...267Db were discovered in the 243Am(48Ca,3-4n) complete-fusion reaction. In 2006 two decay chains of the lighter isotope 282113 were synthesized in the 237Np(48Ca,3n) reaction [3]. The discovery of element 117 [4,5] has been reported using the 249Bk+48Ca reaction; five decay chains of 293117 289115 ...281Rg and one chain of the heaviest isotope 294117 290115 ...270Db were observed in 2009-2010. A relatively high stability of all these odd-Z activities is caused by the influence of presumably spherical nuclear shells at Z=114-126 and N=184. The sequential a decays of the isotopes 282113, 287,288115 and 294117 lead to 266-270Db (N=161-165) that are already located in the vicinity of deformed nuclear shells at Z=108 and N=162...

  9. PRELIMINARY CROSS SECTION AND NU-BAR COVARIANCES FOR WPEC SUBGROUP 26

    Energy Technology Data Exchange (ETDEWEB)

    ROCHMAN,D.

    2007-01-31

    We report preliminary cross section covariances developed for the WPEC Subgroup 26 for 45 out of 52 requested materials. The covariances were produced in 15- and 187-group representations as follows: (1) 36 isotopes ({sup 16}O, {sup 19}F, {sup 23}Na, {sup 27}Al, {sup 28}Si, {sup 52}Cr, {sup 56,56}Fe, {sup 58}Ni, {sup 90,91,92,94}Zr, {sup 166,167,168,170}Er, {sup 206,207,208}Pb, {sup 209}Bi, {sup 233,234,236}U, {sup 237}Np, {sup 238,240,241,242}Pu, {sup 241,242m,243}Am, {sup 242,243,244,245}Cm) were evaluated using the BNL-LANL methodology. For the thermal region and the resolved and unresolved resonance regions, the methodology has been based on the Atlas-Kalman approach, in the fast neutron region the Empire-Kalman method has been used; (2) 6 isotopes ({sup 155,156,157,158,160}Gd and {sup 232}Th) were taken from ENDF/B-VII.0; and (3) 3 isotopes ({sup 1}H, {sup 238}U and {sup 239}Pu) were taken from JENDL-3.3. For 6 light nuclei ({sup 4}He, {sup 6,7}Li, {sup 9}Be, {sup 10}B, {sup 12}C), only partial cross section covariance results were obtained, additional work is needed and they do not report the results here. Likewise, the cross section covariances for {sup 235}U, which they recommend to take from JENDL-3.3, will be included once the multigroup processing is successfully completed. Covariances for the average number of neutrons per fission, total {nu}-bar, are provided for 10 actinides identified as priority by SG26. Further work is needed to resolve some of the issues and to produce covariances for the full set of 52 materials.

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

    Science.gov (United States)

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

    2016-07-01

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

  11. Closed fuel cycle with increased fuel burn-up and economy applying of thorium resources

    Science.gov (United States)

    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

  12. On the role of fusion neutron source with thorium blanket in forming the nuclide composition of the nuclear fuel cycle of the Russian Federation

    Science.gov (United States)

    Shmelev, A. N.; Kulikov, G. G.

    2016-12-01

    The possible role of available thorium resources of the Russian Federation in utilization of thorium in the closed (U-Pu)-fuel cycle of nuclear power is considered. The efficiency of application of fusion neutron sources with thorium blanket for economical use of available thorium resources is demonstrated. The objective of this study is the search for a solution of such major tasks of nuclear power as reduction of the amount of front-end operations in the nuclear fuel cycle and enhancement of its protection against uncontrolled proliferation of fissile materials with the smallest possible alterations in the fuel cycle. The earlier results are analyzed, new information on the amount of thorium resources of the Russian Federation is used, and additional estimates are made. The following basic results obtained on the basis of the assumption of involving fusion reactors with Th-blanket in future nuclear power for generation of the light uranium fraction 232+233+234U and 231Pa are formulated. (1) The fuel cycle would 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 fuel component, and being mixed with regenerated uranium, it would become reduced-enrichment uranium fuel, which would relieve the problem of nonproliferation of the fissile material. (3) The addition of 231Pa into the fuel would stabilize its neutron-multiplying properties, thus making it possible to implement a long fuel residence time and, as a consequence, increase the export potential of the whole nuclear power technology. (4) The available thorium resource in the vicinity of Krasnoufimsk is sufficient for operation of the large-scale nuclear power industry of the Russian Federation with an electric power of 70 GW for more than one quarter of a century. The general conclusion is that involvement of a small number of fusion reactors with Th-blanket in the future nuclear power industry of the Russian

  13. Boundary processes traced by neodymium isotopes

    Science.gov (United States)

    Jeandel, C.; Lacan, F.

    2003-04-01

    Continental margins have been identified as preferential sites for removing of reactive elements from the ocean, on the base of U-series measurements (more specifically 231Pa/230Th). This process is called boundary scavenging (Bacon, 1988). Five years of neodymium isotopes data in water masses along the ocean margins (Indonesia, Papua New Guinea, Greenland-Scotland ridge and Labrador Sea) suggests that Nd is transferred from the sediments to the ocean but the reverse also occurs via the so-called boundary scavenging. These processes are only detectable by isotopic ratio measurements because they affect the isotopic signature of the water mass coming in contact with the margin, without changing its concentration. They can involve much higher fluxes than net input processes: for example, the modification of the AAIW signature along the Papua New Guinea slope involves exchange processes only (Lacan and Jeandel, 2001). Since we suspect that such processes not only affect the Nd oceanic chemistry but also the chemical fate of other reactive elements in the ocean, we suggest that the concept of boundary scavenging should be extended to "boundary exchange".

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

    Science.gov (United States)

    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.

  15. A test of uranium-series dating of fossil tooth enamel: results from Tournal Cave, France

    Science.gov (United States)

    Bischoff, J.L.; Rosenbauer, R.J.; Tavoso, A.; de Lumley, Henry

    1988-01-01

    A series of well preserved mammal bones and horse teeth was analyzed from archaeological levels of Tournal Cave (Magdalenian, Aurignacian, and Mousterain) to test the hypothesis that well-crystallized enamel behaves more as a closed system than does whole bone. The isotopic composition of bones and tooth enamels from this deposit meet criteria for confidence, and gave no reasons to suspect contamination or open-system behavior. Two samples for which 231Pa could be analyzed showed internal concordance with the respective 230Th ages. In spite of the favourable isotopic criteria, however, comparison of the U-series ages of the bones and the tooth enamel with stratigraphic position and 14C control indicated the dates were not meaningful. In general, both bones and tooth enamels gave ages too young, although some were clearly too old. Neither group showed any systematic increase of age with stratigraphic depth. Tooth enamel, therefore, shows no advantage over bone for U-series dating for this site. In Tournal cave both bones and enamel are apparently open to U, which is probably cycling as a consequences of post-depositional groundwater movement. ?? 1988.

  16. LAFARA: a new underground laboratory in the French Pyrénées for ultra low-level gamma-ray spectrometry.

    Science.gov (United States)

    van Beek, P; Souhaut, M; Lansard, B; Bourquin, M; Reyss, J-L; von Ballmoos, P; Jean, P

    2013-02-01

    We describe a new underground laboratory, namely LAFARA (for "LAboratoire de mesure des FAibles RAdioactivités"), that was recently created in the French Pyrénées. This laboratory is primarily designed to analyze environmental samples that display low radioactivity levels using gamma-ray spectrometry. Two high-purity germanium detectors were placed under 85 m of rock (ca. 215 m water equivalent) in the tunnel of Ferrières (Ariège, France). The background is thus reduced by a factor of ∼20 in comparison to above-ground laboratories. Both detectors are fully equipped so that the samples can be analyzed in an automatic mode without requiring permanent presence of a technician in the laboratory. Auto-samplers (twenty positions) and systems to fill liquid nitrogen automatically provide one month of autonomy to the spectrometers. The LAFARA facility allows us to develop new applications in the field of environmental sciences based on the use of natural radionuclides present at low levels in the environment. As an illustration, we present two of these applications: i) dating of marine sediments using the decay of (226)Ra in sedimentary barite (BaSO(4)), ii) determination of (227)Ac ((231)Pa) activities in marine sediment cores.

  17. ORELA contribution to thorium-cycle nuclear data

    Energy Technology Data Exchange (ETDEWEB)

    Olsen, D.K.

    1982-01-01

    The measurements of direct importance to the /sup 232/Th//sup 233/U fuel cycle using neutrons from the Oak Ridge Linear Accelerator Facility are gathered together and discussed. These measurements were done in response to specific data discrepancies, as part of generic programs, and for basic fission physics studies. In particular, completed transmission and capture work on /sup 232/Th has yielded the most accurate parameters for the first four s-wave resonances; the largest average capture width, 25.2 MeV; and the largest s-wave strength function of recent measurements. These results allow improved agreement between differential and integral capture rates. Moreover, the ORNL /sup 252/Cf anti nu measurement of unprecedented accuracy and /sup 233/U anti nu ratio measurement give a /sup 233/U prompt anti nu (thermal) of 2.490 +- 0.009 neutron/fission. This result allows a much more satisfactory understanding of the /sup 233/U 2200 m/s constants. In addition, a /sup 232/Th ..gamma..-ray production measurement provides needed cross sections for shielding, and important data for both application and fission physics were obtained from /sup 232/Th fission and both /sup 231/Pa and /sup 234/U fission and total cross section measurements. Data requirements and discrepancies suggested from this work are discussed.

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

    Directory of Open Access Journals (Sweden)

    Wiedeking M.

    2012-02-01

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

  19. Direct determination of the timing of sea level change during termination II.

    Science.gov (United States)

    Gallup, Christina D; Cheng, H; Taylor, F W; Edwards, R L

    2002-01-11

    An outcrop within the last interglacial terrace on Barbados contains corals that grew during the penultimate deglaciation, or Termination II. We used combined 230Th and 231Pa dating to determine that they grew 135.8 +/- 0.8 thousand years ago, indicating that sea level was 18 +/- 3 meters below present sea level at the time. This suggests that sea level had risen to within 20% of its peak last-interglacial value by 136 thousand years ago, in conflict with Milankovitch theory predictions. Orbital forcing may have played a role in the deglaciation, as may have isostatic adjustments due to large ice sheets. Other corals in the same outcrop grew during oxygen isotope (delta18O) substage 6e, indicating that sea level was 38 +/- 5 meters below present sea level, about 168.0 thousand years ago. When compared to the delta18O signal in the benthic V19-30/V19-28 record at that time, the coral data extend to the previous glacial cycle the conclusion that deep-water temperatures were colder during glacial periods.

  20. Phytoremediation: role of terrestrial plants and aquatic macrophytes in the remediation of radionuclides and heavy metal contaminated soil and water.

    Science.gov (United States)

    Sharma, Sunita; Singh, Bikram; Manchanda, V K

    2015-01-01

    Nuclear power reactors are operating in 31 countries around the world. Along with reactor operations, activities like mining, fuel fabrication, fuel reprocessing and military operations are the major contributors to the nuclear waste. The presence of a large number of fission products along with multiple oxidation state long-lived radionuclides such as neptunium ((237)Np), plutonium ((239)Pu), americium ((241/243)Am) and curium ((245)Cm) make the waste streams a potential radiological threat to the environment. Commonly high concentrations of cesium ((137)Cs) and strontium ((90)Sr) are found in a nuclear waste. These radionuclides are capable enough to produce potential health threat due to their long half-lives and effortless translocation into the human body. Besides the radionuclides, heavy metal contamination is also a serious issue. Heavy metals occur naturally in the earth crust and in low concentration, are also essential for the metabolism of living beings. Bioaccumulation of these heavy metals causes hazardous effects. These pollutants enter the human body directly via contaminated drinking water or through the food chain. This issue has drawn the attention of scientists throughout the world to device eco-friendly treatments to remediate the soil and water resources. Various physical and chemical treatments are being applied to clean the waste, but these techniques are quite expensive, complicated and comprise various side effects. One of the promising techniques, which has been pursued vigorously to overcome these demerits, is phytoremediation. The process is very effective, eco-friendly, easy and affordable. This technique utilizes the plants and its associated microbes to decontaminate the low and moderately contaminated sites efficiently. Many plant species are successfully used for remediation of contaminated soil and water systems. Remediation of these systems turns into a serious problem due to various anthropogenic activities that have

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

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.; Jones, V.

    2009-05-27

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

  2. Neutron-induced fission cross sections of 242Pu from 0.3 MeV to 3 MeV

    Science.gov (United States)

    Salvador-Castiñeira, P.; Bryś, T.; Eykens, R.; Hambsch, F.-J.; Göök, A.; Moens, A.; Oberstedt, S.; Sibbens, G.; Vanleeuw, D.; Vidali, M.; Pretel, C.

    2015-10-01

    The majority of the next generation of nuclear power plants (GEN-IV) will work in the fast-neutron-energy region, as opposed to present day thermal reactors. This leads to new and more accurate nuclear-data needs for some minor actinides and structural materials. Following those upcoming demands, the Organisation for Economic Cooperation and Development Nuclear Energy Agency performed a sensitivity study. Based on the latter, an improvement in accuracy from the present 20% to 5% is required for the 242Pu(n ,f ) cross section. Within the same project both the 240Pu(n ,f ) cross section and the 242Pu(n ,f ) cross section were measured at the Van de Graaff accelerator of the Joint Research Centre at the Institute for Reference Materials and Measurements, where quasimonoenergetic neutrons were produced in an energy range from 0.3 MeV up to 3 MeV. A twin Frisch-grid ionization chamber has been used in a back-to-back configuration as fission-fragment detector. The 242Pu(n ,f ) cross section has been normalized to three different isotopes: 237Np(n ,f ) , 235U(n ,f ) , and 238U(n ,f ) . A comprehensive study of the corrections applied to the data and the uncertainties associated is given. The results obtained are in agreement with previous experimental data at the threshold region up to 0.8 MeV. The resonance-like structure at 0.8 to 1.1 MeV, visible in the evaluations and in most previous experimental values, was not reproduced with the same intensity in this experiment. For neutron energies higher than 1.1 MeV, the results of this experiment are slightly lower than the Evaluated Nuclear Data File/B-VII.1 evaluation but in agreement with the experiment of Tovesson et al. (2009) as well as Staples and Morley (1998). Finally, for energies above 1.5 MeV, the results show consistency with the present evaluations.

  3. Speciation of neptunium during migration in clay rock; Speziation von Neptunium bei der Migration in Tongestein

    Energy Technology Data Exchange (ETDEWEB)

    Froehlich, Daniel

    2011-12-15

    The present work was performed within a fellowship of the interdisciplinary research training group 826 ''trace analysis of elemental species: method development and application'' funded by the German Research Foundation (DFG) and the federal state Rheinland-Pfalz. Aim of this work was to gain new knowledge of the interaction between neptunium and natural clay rock with respect to the disposal of high-level nuclear waste in deep geological formations. The isotope {sup 237}Np with its long half-life of more than two million years will be one of main contributors to the radiotoxicity of the radioactive waste material after storage times of more than 1000 years. In aqueous solution under environmental relevant conditions Np can exist in the oxidation states +IV and +V. Due to its high solubility and higher mobility Np(V) is the much more hazardous species compared to Np(IV). Opalinus Clay (OPA) from Mont Terri, Switzerland, was used as a natural reference material in the migration studies. The focus of this work was on speciation of Np on the mineral surface by synchrotron based X-ray absorption spectroscopy (EXAFS/XANES). The interaction between Np(V) and OPA was studied in batch sorption and diffusion experiments in dependence of various experimental parameters (e.g. pH, temperature, background electrolyte, effect of humic acid, concurrence with U(VI), aerobic/anaerobic conditions). The investigation of Np speciation was performed on two types of samples. Powder samples from batch experiments were prepared under aerobic and anaerobic conditions and measured by EXAFS spectroscopy. Diffusion samples and OPA thin sections contacted with Np(V) were analyzed by locally resolved μ-XANES measurements on enrichments of Np. A combination with μ-XRF (X-ray fluorescence) mapping and μ-XRD (X-ray diffraction) measurements provided further information about the spatial distribution of Np and other elements contained in OPA as well as crystalline mineral

  4. Structure and Bonding in Some Gd(Ⅲ) Metal Complexes Studied by Three-Dimensional X-Ray Analysis and 155Gd M(o)ssbauer Spectroscopy

    Institute of Scientific and Technical Information of China (English)

    2007-01-01

    Some functional lanthanide metal complexes, such as acetylacetonato complexes, ethylenediaminetetraacetato complexes, were successfully applied for diagnostic technique.The authors are interested in investigating the structure and bonding in lanthanide and actinide metal complexes using 166Er, 155Gd, and 237Np M(o)ssbauer spectroscopies in connection with single-crystal and/or powder X-ray diffraction, making clear the differences on their structures as well as the differences in the participation of 4f and 5f orbitals in the chemical bonds.In this article, the crystal structures of two novel Gd(Ⅲ) acetylacetonato complexes, Gd(pta)3·2H2O (pta=1,1,1-trifluoro-5,5-dimethyl-2,4-hexanedione) and Gd(bfa)3·2H2O (bfa=1, 1, 1-trifluoro-4-phenyl-2-4-butanedione) were reported.Though both of them were dihydrate and had distorted square antiprismatical structure, Gd(pta)3·2H2O crystallizes in the P 21/ n (#14) monoclinic space group and its lattice parameters are a =1.4141(6) nm, b =1.0708(3) nm, c =2.2344(4) nm, β=95.24(2)°, and Gd(bfa)3·2H2O crystallizes in P 212121 orthorhombic space group and its lattice parameters were a=1.322(1) nm, b =2.295(1) nm, c =1.0786(8) nm.In the meantime, the authors had finished a systematic investigation on the 155Gd M(o)ssbauer isomer shift (δ) of various Gd(Ⅲ) metal complexes having a different coordination number (C.N.) and different ratios coordinating oxygen to nitrogen.A tendency for the δ value to decrease with an increase in the C.N, and the number of the nitrogen atom coordinating to Gd was confirmed.This indicated that the Gd-O and/or Gd-N bond in the investigated Gd(Ⅲ) metal complexes had a small covalent contribution, which was possible to be deduced from the O and/or N atoms of the ligands donating electrons to 6s, 5d, and 4f orbitals of Gd.

  5. Concordant plutonium-241-americium-241 dating of environmental samples: results from forest fire ash

    Energy Technology Data Exchange (ETDEWEB)

    Goldstein, Steven J [Los Alamos National Laboratory; Oldham, Warren J [Los Alamos National Laboratory; Murrell, Michael T [Los Alamos National Laboratory; Katzman, Danny [Los Alamos National Laboratory

    2010-12-07

    We have measured the Pu, {sup 237}Np, {sup 241}Am, and {sup 151}Sm isotopic systematics for a set of forest fire ash samples from various locations in the western U.S. including Montana, Wyoming, Idaho, and New Mexico. The goal of this study is to develop a concordant {sup 241}Pu (t{sub 1/2} = 14.4 y)-{sup 241}Am dating method for environmental collections. Environmental samples often contain mixtures of components including global fallout. There are a number of approaches for subtracting the global fallout component for such samples. One approach is to use {sup 242}/{sup 239}Pu as a normalizing isotope ratio in a three-isotope plot, where this ratio for the nonglobal fallout component can be estimated or assumed to be small. This study investigates a new, complementary method of normalization using the long-lived fission product, {sup 151}Sm (t{sub 1/2} = 90 y). We find that forest fire ash concentrates actinides and fission products with {approx}1E10 atoms {sup 239}Pu/g and {approx}1E8 atoms {sup 151}Sm/g, allowing us to measure these nuclides by mass spectrometric (MIC-TIMS) and radiometric (liquid scintillation counting) methods. The forest fire ash samples are characterized by a western U.S. regional isotopic signature representing varying mixtures of global fallout with a local component from atmospheric testing of nuclear weapons at the Nevada Test Site (NTS). Our results also show that {sup 151}Sm is well correlated with the Pu nuclides in the forest fire ash, suggesting that these nuclides have similar geochemical behavior in the environment. Results of this correlation indicate that the {sup 151}Sm/{sup 239}Pu atom ratio for global fallout is {approx}0.164, in agreement with an independent estimate of 0.165 based on {sup 137}Cs fission yields for atmospheric weapons tests at the NTS. {sup 241}Pu-{sup 241}Am dating of the non-global fallout component in the forest fire ash samples yield ages in the late 1950's-early 1960's, consistent with a peak

  6. Characterization of Supernate Samples from HLW Tanks 13H, 30H, 37H, 39H, 45F, 46F, and 49H

    Energy Technology Data Exchange (ETDEWEB)

    STALLINGS, MARY

    2004-07-02

    This document presents work conducted in support of technical needs expressed, in part, by the Engineering, Procurement, and Construction Contractor for the Salt Waste Processing Facility (SWPF). The Department of Energy (DOE) requested that Savannah River National Laboratory (SRNL) analyze and characterize supernate waste from seven selected High Level Waste (HLW) tanks to allow classification of feed to be sent to the SWPF, verification that SWPF processes will be able to meet Saltstone Waste Acceptance Criteria (WAC), and updating of the Waste Characterization System (WCS) database. This document provides characterization data of samples obtained from Tanks 13H, 30H, 37H, 39H, 45F, 46F, and 49H and discusses results.Characterization of the waste tank samples involved several treatments and analysis at various stages of sample processing. These analytical stages included as-received liquid, post-dilution to 6.44 M sodium (target), post-acid digestion, post-filtration (at 3 filtration pore sizes), and after cesium removal using ammonium molybdophosphate (AMP). Results and observations obtained from testing include the following. All tanks will require cesium removal as well as treatment with Monosodium Titanate (MST) for 90Sr (Strontium) decontamination. A small filtration effect for 90Sr was observed for five of the seven tank wastes. No filtration effects were observed for Pu (Plutonium), Np (Neptunium), U (Uranium), or Tc (Technetium). 137Cs (Cesium) concentration is approximately E+09 pCi/mL for all the tank wastes. Tank 37H is significantly higher in 90Sr than the other six tanks. 237Np in the F-Area tanks(45F and 46F) are at least 1 order of magnitude less than the H-Area tank wastes. The data indicate a constant ratio of 99Tc to Cs in the seven tank wastes. This indicates the Tc remains largely soluble in Savannah River Site (SRS) waste and partition similarly with Cs. 241Am (Americium) concentration was low in the seven tank wastes. The majority of data

  7. Characterization Of Supernate Samples From High Level Waste Tanks 13H, 30H, 37H, 39H, 45F, 46F and 49H

    Energy Technology Data Exchange (ETDEWEB)

    Stallings, M. E.; Barnes, M. J.; Peters, T. B.; Diprete, D. P.; Hobbs, D. T.; Fink, S. D.

    2005-06-15

    This document presents work conducted in support of technical needs expressed, in part, by the Engineering, Procurement, and Construction Contractor for the Salt Waste Processing Facility (SWPF). The Department of Energy (DOE) requested that Savannah River National Laboratory (SRNL) analyze and characterize supernate waste from seven selected High Level Waste (HLW) tanks to allow: classification of feed to be sent to the SWPF; verification that SWPF processes will be able to meet Saltstone Waste Acceptance Criteria (WAC); and updating of the Waste Characterization System (WCS) database. This document provides characterization data of samples obtained from Tanks 13H, 30H, 37H, 39H, 45F, 46F, and 49H and discusses results. Characterization of the waste tank samples involved several treatments and analysis at various stages of sample processing. These analytical stages included as-received liquid, post-dilution to 6.44 M sodium (target), post-acid digestion, post-filtration (at 3 filtration pore sizes), and after cesium removal using ammonium molybdophosphate (AMP). All tanks will require cesium removal as well as treatment with Monosodium Titanate (MST) for {sup 90}Sr (Strontium) decontamination. A small filtration effect for 90Sr was observed for six of the seven tank wastes. No filtration effects were observed for Pu (Plutonium), Np (Neptunium), U (Uranium), or Tc (Technetium); {sup 137}Cs (Cesium) concentration is ~E+09 pCi/mL for all the tank wastes. Tank 37H is significantly higher in {sup 90}Sr than the other six tanks. {sup 237}Np in the F-area tanks (45F and 46F) are at least 1 order of magnitude less than the H-Area tank wastes. The data indicate a constant ratio of {sup 99}Tc to Cs in the seven tank wastes. This indicates the Tc remains largely soluble in Savannah River Site (SRS) waste and partitions similarly with Cs. {sup 241}Am (Americium) concentration was low in the seven tank wastes. The majority of data were detection limit values, the largest being

  8. Concordant 241Pu-241Am Dating of Environmental Samples: Results from Forest Fire Ash

    Science.gov (United States)

    Goldstein, S. J.; Oldham, W. J.; Murrell, M. T.; Katzman, D.

    2010-12-01

    We have measured the Pu, 237Np, 241Am, and 151Sm isotopic systematics for a set of forest fire ash samples from various locations in the western U.S. including Montana, Wyoming, Idaho, and New Mexico. The goal of this study is to develop a concordant 241Pu (t1/2 = 14.4 y)-241Am dating method for environmental collections. Environmental samples often contain mixtures of components including global fallout. There are a number of approaches for subtracting the global fallout component for such samples. One approach is to use 242Pu/239Pu as a normalizing isotope ratio in a three-isotope plot, where this ratio for the non-global fallout component can be estimated or assumed to be small. This study investigates a new, complementary method of normalization using the long-lived fission product, 151Sm (t1/2 = 90 y). We find that forest fire ash concentrates actinides and fission products with ~1E10 atoms 239Pu/g and ~1E8 atoms 151Sm/g, allowing us to measure these nuclides by mass spectrometric (MIC-TIMS) and radiometric (liquid scintillation counting) methods. The forest fire ash samples are characterized by a western U.S. regional isotopic signature representing varying mixtures of global fallout with a local component from atmospheric testing of nuclear weapons at the Nevada Test Site (NTS). Our results also show that 151Sm is well correlated with the Pu nuclides in the forest fire ash, suggesting that these nuclides have similar geochemical behavior in the environment. Results of this correlation indicate that the 151Sm/239Pu atom ratio for global fallout is ~0.164, in agreement with an independent estimate of 0.165 based on 137Cs fission yields for atmospheric weapons tests at the NTS. 241Pu-241Am dating of the non-global fallout component in the forest fire ash samples yield ages in the late 1950’s-early 1960’s, consistent with a peak in NTS weapons testing at that time. The age results for this component are in agreement using both 242Pu and 151Sm normalizations

  9. Radionuclide studies in the North Atlantic as a contribution to a better understanding of particle dynamics in the water column. Final report; Radionukliduntersuchungen im Nordatlantik als Beitrag zum Verstaendnis der Partikeldynamik in der Wassersaeule. Endbericht

    Energy Technology Data Exchange (ETDEWEB)

    Scholten, J.C.; Vogler, S.; Fietzke, J.; Mangini, A.; Stoffers, P.

    1997-12-31

    As part of the German Joint Global Ocean Flux Study (JGOFS) the distribution of natural radionuclides in the water column and in sediment traps have been investigated. The main objective was to estimate the trapping efficiency of sediment traps deployed at three locations in the eastern North Atlantic (L1: 33 N, L2: 47 N; L3: 54 N; all situated at about 20 W) and to obtain information about particle exchange processes in the water column. In the upper water column the {sup 230}Th concentrations are similar at all locations investigated and a reversible scavenging model was able to describe the {sup 230}Th distribution. In the deep water-column at L2 and L3, however, the {sup 230}Th concentrations were significantly lower than predicted from the reversible scavenging model. The {sup 230}Th concentrations here could be described by a scavenging-mixing model which assumes an advection of {sup 230}Th depleted water masses and a rapid ventilation between 3 and 25 years. Seasonal variations in the radionuclide fluxes were observed in the sediment traps. The {sup 228}Th/{sup 230}Th ratios in the traps indicate particle exchange rates (aggregation/disaggregation) to be higher during the spring blooms. Based on the {sup 230}Th and {sup 231}Pa distribution in the water column and in the sediment traps, trapping efficiencies were calculated to be between 15% and 181%. Overtrapping was observed in a trap deployed near the seafloor. The lowest efficiencies (15%-26%) were determined in the 500 m and 1000 m traps. No direct relation between water currents and trapping biases were observed in this study. (orig.) [Deutsch] Im Rahmen der Deutschen JOINT GLOBAL OCEAN FLUX STUDY wurde die Verteilung natuerlicher Radionuklide in der Wassersaeule und in Sinkstoffallen an drei Lokationen (L1: 34 N, L2: 47 N, L3: 54 N; alle bei 20 W) im oestlichen Nordatlantik untersucht. Wesentliche Ziele des Projektes waren, die Fangeffizienz von Sinkstoffallen und die Partikeldynamik (Partikel

  10. REIMEP-22 inter-laboratory comparison. ''U Age Dating - determination of the production date of a uranium certified test sample''

    Energy Technology Data Exchange (ETDEWEB)

    Venchiarutti, Celia; Richter, Stephan; Jakopic, Rozle; Aregbe, Yetunde [European Commission, Joint Research Centre (JRC), Geel (Belgium). Institute for Reference Materials and Measurements (IRMM); Varga, Zsolt; Mayer, Klaus [European Commission, Joint Research Centre (JRC), Karlsruhe (Germany). Institute for Transuranium Elements (ITU)

    2015-07-01

    The REIMEP-22 inter-laboratory comparison aimed at determining the production date of a uranium certified test sample (i.e. the last chemical separation date of the material). Participants in REIMEP-22 on ''U Age Dating - Determination of the production date of a uranium certified test sample'' received one low-enriched 20 mg uranium sample for mass spectrometry measurements and/or one 50 mg uranium sample for a-spectrometry measurements, with an undisclosed value for the production date. They were asked to report the isotope amount ratios n({sup 230}Th)/n({sup 234}U) for the 20 mg uranium sample and/or the activity ratios A({sup 230}Th)/A({sup 234}U) for the 50 mg uranium sample in addition to the calculated production date of the certified test samples with its uncertainty. Reporting of the {sup 231}Pa/{sup 235}U ratio and the respective calculated production date was optional. Eleven laboratories reported results in REIMEP-22. Two of them reported results for both the 20 mg and 50 mg uranium certified test samples. The measurement capability of the participants was assessed against the independent REIMEP-22 reference value by means of z- and zeta-scores in compliance with ISO 13528:2005. Furthermore a performance assessment criterion for acceptable uncertainty was applied to evaluate the participants' results. In general, the REIMEP-22 participants' results were satisfactory. This confirms the analytical capabilities of laboratories to determine accurately the age of uranium materials with low amount of ingrown thorium (young certified test sample). The Joint Research Centre of the European Commission (EC-JRC) organised REIMEP-22 in parallel to the preparation and certification of a uranium reference material certified for the production date (IRMM-1000a and IRMM-1000b).

  11. Origin of elements of the Uranium-235 family observed in the Ellez river near the EL-4 experimental nuclear reactor in dismantling (Monts d'Arree- Finistere department); Origine des elements de la famille de l'uranium-235 observes dans la riviere Ellez a proximite du reacteur nucleaire experimental EL4 en cours de demantelement (Mont d'Arree - departement du Finistere). Resultats et premiers constats annee 2006

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2006-07-01

    In a previous study which concerned the catchment basin of the harbour of Brest, the A.C.R.O. put in evidence a marking by artificial radioelements around the power plant of Brennilis which can be imputed without ambiguities to the nuclear installation. It also put in evidence abnormalities concerning the natural radioactivity which justifies this new study. In the area of the Monts d'Arree, actinium 227 ({sup 227}Ac), non born by its ascendents which are {sup 235}U and {sup 231}Pa is observed. This phenomenon is characterized by mass activities superior to these ones of {sup 235}U and able to reach these ones of {sup 238}U. Its presence corresponds with the drainage of the Ellez river since the former channel of radioactive effluents releases from the nuclear power plant EL-4 up to the reservoir Saint-Herblot situated 6 km downstream. The strongest values of radioactivity are registered near the disused power plant, at this place a relationship exists between the level of actinium 227 and this one of the artificial radioactivity as it exists a relationship with the decay products of radon exhaled from the subsoil ({sup 210}Pb). But its presence is not limited to a part of the Ellez river, it is equally observed in terrestrial medium, in places in priori not influenced by the direct liquid effluents of the power plant. This place is situated at more than 4 km and without any connection with the Ellez waters. At this stage of the study, it is not possible to answer with certainty the question of the origin of this phenomenon. A new reorientation is considered indispensable to clarify definitively the origin of this unknown phenomenon in the scientific publications and the environmental monitoring. (N.C.)

  12. DISSOLVED CONCENTRATION LIMITS OF RADIOACTIVE ELEMENTS

    Energy Technology Data Exchange (ETDEWEB)

    P. Bernot

    2005-07-13

    The purpose of this study is to evaluate dissolved concentration limits (also referred to as solubility limits) of elements with radioactive isotopes under probable repository conditions, based on geochemical modeling calculations using geochemical modeling tools, thermodynamic databases, field measurements, and laboratory experiments. The scope of this activity is to predict dissolved concentrations or solubility limits for elements with radioactive isotopes (actinium, americium, carbon, cesium, iodine, lead, neptunium, plutonium, protactinium, radium, strontium, technetium, thorium, and uranium) relevant to calculated dose. Model outputs for uranium, plutonium, neptunium, thorium, americium, and protactinium are provided in the form of tabulated functions with pH and log fCO{sub 2} as independent variables, plus one or more uncertainty terms. The solubility limits for the remaining elements are either in the form of distributions or single values. Even though selection of an appropriate set of radionuclides documented in Radionuclide Screening (BSC 2002 [DIRS 160059]) includes actinium, transport of Ac is not modeled in the total system performance assessment for the license application (TSPA-LA) model because of its extremely short half-life. Actinium dose is calculated in the TSPA-LA by assuming secular equilibrium with {sup 231}Pa (Section 6.10); therefore, Ac is not analyzed in this report. The output data from this report are fundamental inputs for TSPA-LA used to determine the estimated release of these elements from waste packages and the engineered barrier system. Consistent modeling approaches and environmental conditions were used to develop solubility models for the actinides discussed in this report. These models cover broad ranges of environmental conditions so they are applicable to both waste packages and the invert. Uncertainties from thermodynamic data, water chemistry, temperature variation, and activity coefficients have been quantified or

  13. Geologic evidence for age of deposits at Hueyatlaco archeological site, Vasequillo, Mexico

    Science.gov (United States)

    Steen-McIntyre, Virginia; Fryxell, Roald; Malde, Harold E.

    1981-07-01

    Direct tracing of beds during excavation in May 1973, confirmed that the artifact-bearing layers at Hueyatlaco underlie 10 m of fine-grained, water-laid deposits that constitute part of the wide-spread Valsequillo gravels. Dissection of these deposits by the adjacent Río Atoyac has reached a depth of 50 m. The stratigraphic section at Hueyatlaco includes four distinctive tephra units. The oldest one occupies a small channel in a series of cut-and-fill stream deposits that have yielded bifacial tools. It lies more than a meter above flat-lying, fine-grained beds from which edge-retouched tools have been recovered. The three other tephra units occur higher in the section. Fission-track ages on zircon phenocrysts from two of the younger tephra layers (370,000 ± 200,000 and 600,000 ± 340,000 yr, 2σ) agree with concordant uranium-series dates for a camel pelvis that was found associated with bifacial tools at Hueyatlaco (245,000 ± 40,000 yr by 230Th and > 180,000 yr by 231Pa). These dates are compatible with the depth of burial and subsequent dissection of the Hueyatlaco deposits, as well as with the degree of hydration of volcanic glass shards and with the extent of etching of heavy-mineral phenocrysts from within the tephra layers. These findings suggest to us that further search for archaeological remains in deposits as old as those at Hueyatlaco would be warranted.

  14. Strong and deep Atlantic meridional overturning circulation during the last glacial cycle.

    Science.gov (United States)

    Böhm, E; Lippold, J; Gutjahr, M; Frank, M; Blaser, P; Antz, B; Fohlmeister, J; Frank, N; Andersen, M B; Deininger, M

    2015-01-01

    Extreme, abrupt Northern Hemisphere climate oscillations during the last glacial cycle (140,000 years ago to present) were modulated by changes in ocean circulation and atmospheric forcing. However, the variability of the Atlantic meridional overturning circulation (AMOC), which has a role in controlling heat transport from low to high latitudes and in ocean CO2 storage, is still poorly constrained beyond the Last Glacial Maximum. Here we show that a deep and vigorous overturning circulation mode has persisted for most of the last glacial cycle, dominating ocean circulation in the Atlantic, whereas a shallower glacial mode with southern-sourced waters filling the deep western North Atlantic prevailed during glacial maxima. Our results are based on a reconstruction of both the strength and the direction of the AMOC during the last glacial cycle from a highly resolved marine sedimentary record in the deep western North Atlantic. Parallel measurements of two independent chemical water tracers (the isotope ratios of (231)Pa/(230)Th and (143)Nd/(144)Nd), which are not directly affected by changes in the global cycle, reveal consistent responses of the AMOC during the last two glacial terminations. Any significant deviations from this configuration, resulting in slowdowns of the AMOC, were restricted to centennial-scale excursions during catastrophic iceberg discharges of the Heinrich stadials. Severe and multicentennial weakening of North Atlantic Deep Water formation occurred only during Heinrich stadials close to glacial maxima with increased ice coverage, probably as a result of increased fresh-water input. In contrast, the AMOC was relatively insensitive to submillennial meltwater pulses during warmer climate states, and an active AMOC prevailed during Dansgaard-Oeschger interstadials (Greenland warm periods).

  15. Prompt Fission Neutron Spectra of Actinides

    Energy Technology Data Exchange (ETDEWEB)

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

    2016-01-01

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

  16. Gamma-Ray Library and Uncertainty Analysis: Passively Emitted Gamma Rays Used in Safeguards Technology

    Energy Technology Data Exchange (ETDEWEB)

    Parker, W

    2009-09-18

    streams can be especially challenging to identify. The super cooled detectors have a marked improvement in energy resolution, allowing the possibility of deconvolution of mixtures of gamma rays that was unavailable with high purity germanium detectors. Isotopic analysis codes require libraries of gamma rays. In certain situations, isotope identification can be made in the field, sometimes with a short turnaround time, depending on the choice of detector and software analysis package. Sodium iodide and high purity germanium detectors have been successfully used in field scenarios. The newer super cooled detectors offer dramatically increased resolution, but they have lower efficiency and so can require longer collection times. The different peak shapes require software development for the specific detector type and field application. Libraries can be tailored to specific scenarios; by eliminating isotopes that are certainly not present, the analysis time may be shortened and the accuracy may be increased. The intent of this project was to create one accurate library of gamma rays emitted from isotopes of interest to be used as a reliable reference in safeguards work. All simulation and spectroscopy analysis codes can draw upon this best library to improve accuracy and cross-code consistency. Modeling codes may include MCNP and COG. Gamma-ray spectroscopy analysis codes may include MGA, MGAU, U235 and FRAM. The intent is to give developers and users the tools to use in nuclear energy safeguards work. In this project, the library created was limited to a selection of actinide isotopes of immediate interest to reactor technology. These isotopes included {sup 234-238}U, {sup 237}Np, {sup 238-242}Pu, {sup 241,243}Am and {sup 244}Cm. These isotopes were examined, and the best of gamma-ray data, including line energies and relative strengths were selected.

  17. Distilling Complex Model Results into Simple Models for use in Assessing Compliance with Performance Standards for Low Level Waste Disposal Facilities

    Energy Technology Data Exchange (ETDEWEB)

    Arthur S. Rood

    2007-02-01

    Assessing the long term performance of waste disposal facility requires numerical simulation of saturated and unsaturated groundwater flow and contaminant transport. Complex numerical models have been developed to try to realistically simulate subsurface flow and transport processes. These models provide important information about system behavior and identify important processes, but may not be practical for demonstrating compliance with performance standards because of excessively long computer simulation times and input requirements. Two approaches to distilling the behavior of a complex model into simpler formulations that are practical for demonstrating compliance with performance objectives are examined in this paper. The first approach uses the information obtained from the complex model to develop a simple model that mimics the complex model behavior for stated performance objectives. The simple model may need to include essential processes that are important to assessing performance, such as time-variable infiltration and waste emplacement rates, subsurface heterogeneity, sorption, decay, and radioactive ingrowth. The approach was applied to a Low-Level Waste disposal site at the Idaho National Laboratory where a complex three dimensional vadose zone model was developed first to understand system behavior and important processes. The complex model was distilled down to a relatively simple one-dimensional vadose zone model and three-dimensional aquifer transport model. Comparisons between the simple model and complex model of vadose zone fluxes and groundwater concentrations showed relatively good agreement between the models for both fission and activation products (129I, 36Cl, 99Tc) and actinides (238U, 239Pu, 237Np). Application of the simple model allowed for Monte Carlo uncertainty analysis and simulations of numerous disposal and release scenarios. The second approach investigated was the response surface model. In the response surface model approach

  18. Speciation of neptunium after diffusion in Opalinus Clay

    Energy Technology Data Exchange (ETDEWEB)

    Reich, Tobias; Amayri, Samer; Drebert, Jakob; Froehlich, Daniel R.; Grolimund, Daniel; Rosemann, Jonathan [Mainz Univ. (Germany). Inst. of Nuclear Chemistry; Kaplan, Ugras [Paul Scherrer Institut, Villigen (Switzerland). Swiss Light Source

    2015-07-01

    Argillaceous rock formations are under consideration as a potential host rock for the construction of high-level nuclear waste repositories. Under environmental conditions the most stable oxidation states of {sup 237}Np (t{sub 1/2}=2.1 x 10{sup 6} a) are Np(IV) and Np(V). We have investigated the sorption and diffusion of the more mobile Np(V) in Opalinus Clay (OPA, Mont Terri, Switzerland) (Wu et al. 2009, Froehlich et al. 2011 and 2012 a). OPA, which is present in Switzerland and southern Germany, possesses a micro-scale heterogeneity and is composed of several types of clay minerals, but also of calcite, quartz and iron(II)-bearing minerals. In our previous diffusion (Wu et al. 2009) and anaerobic sorption experiments (Froehlich et al. 2011), we observed higher distribution coefficients, K{sub d}, than expected from batch experiments performed in air, indicating that a partial reduction of Np(V) to Np(IV) had occurred. To test this hypothesis, different sorption and diffusion samples with Np(V) were prepared at pH 7.6 for spatially resolved molecular-level investigations at the microXAS beamline at the Swiss Light Source (PSI, Villigen, Switzerland) (Froehlich et al. 2012 b). Elemental distributions of Ca, Fe and Np have been determined by μ-XRF mapping. Regions of high Np concentration were subsequently investigated by Np L{sub III}-edge μ-XANES. In most samples Np spots with considerable amounts of tetravalent Np could be found, even when the experiments were performed under ambient-air conditions. In some cases, almost pure Np(IV) L{sub III}-edge XANES spectra were recorded. In case of the anaerobic sorption sample, a clear correlation between Np and Fe was observed by μ-XRF, indicating that iron(II)-bearing minerals could be responsible for the reduction of Np(V). μ-XRD measurements of this sample showed that pyrite is at least one of the redox-active phases determining the speciation of Np in OPA. In this case, Np was accumulated on pyrite, indicating

  19. No iron fertilization in the equatorial Pacific Ocean during the last ice age

    Science.gov (United States)

    Costa, K. M.; McManus, J. F.; Anderson, R. F.; Ren, H.; Sigman, D. M.; Winckler, G.; Fleisher, M. Q.; Marcantonio, F.; Ravelo, A. C.

    2016-01-01

    The equatorial Pacific Ocean is one of the major high-nutrient, low-chlorophyll regions in the global ocean. In such regions, the consumption of the available macro-nutrients such as nitrate and phosphate is thought to be limited in part by the low abundance of the critical micro-nutrient iron. Greater atmospheric dust deposition could have fertilized the equatorial Pacific with iron during the last ice age—the Last Glacial Period (LGP)—but the effect of increased ice-age dust fluxes on primary productivity in the equatorial Pacific remains uncertain. Here we present meridional transects of dust (derived from the 232Th proxy), phytoplankton productivity (using opal, 231Pa/230Th and excess Ba), and the degree of nitrate consumption (using foraminifera-bound δ15N) from six cores in the central equatorial Pacific for the Holocene (0-10,000 years ago) and the LGP (17,000-27,000 years ago). We find that, although dust deposition in the central equatorial Pacific was two to three times greater in the LGP than in the Holocene, productivity was the same or lower, and the degree of nitrate consumption was the same. These biogeochemical findings suggest that the relatively greater ice-age dust fluxes were not large enough to provide substantial iron fertilization to the central equatorial Pacific. This may have been because the absolute rate of dust deposition in the LGP (although greater than the Holocene rate) was very low. The lower productivity coupled with unchanged nitrate consumption suggests that the subsurface major nutrient concentrations were lower in the central equatorial Pacific during the LGP. As these nutrients are today dominantly sourced from the Subantarctic Zone of the Southern Ocean, we propose that the central equatorial Pacific data are consistent with more nutrient consumption in the Subantarctic Zone, possibly owing to iron fertilization as a result of higher absolute dust fluxes in this region. Thus, ice-age iron fertilization in the

  20. Thermodynamic and structural properties in complexing media; Comportement chimique du protactinium (V) en presence d'ions sulfate

    Energy Technology Data Exchange (ETDEWEB)

    Di Giandomenico, M.V

    2007-10-15

    Protactinium is experiencing a renewal of interest in the frame of long-term energy production. Modelling the behaviour of this element in the geosphere requires thermodynamic and structural data relevant to environmental conditions. Now deep clayey formation are considered for the disposal of radioactive waste and high values of natural sulphate contents have been determined in pore water in equilibrium with clay surface. Because of its tendency to polymerisation, hydrolysis and sorption on all solid supports, the equilibria constants relative to monomer species were determined at tracer scale (ca. 10 - 12 M) with {sup 233}Pa. The complexation constants of Pa(V) and sulphate ions were calculated starting from a systematic study of the apparent distribution coefficient D in the system TTA/Toluene/H{sub 2}O/Na{sub 2}SO{sub 4}/HClO{sub 4}/NaClO{sub 4} and as a function of ionic strength, temperature, free sulphate, protons and chelatant concentration. First of all, the interaction between free species H{sup +}, SO{sub 4}{sup -}, Na{sup +} leads to the formation of HSO{sub 4}{sup -} and NaSO{sub 4}{sup -}, for which concentrations depend upon the related thermodynamic constants. For this purpose a computer code was developed in order to determine all free species concentration. This iterative code takes into account the influence of temperature and ionic strength (SIT modelling) on thermodynamic constants. The direct measure of Pa(V) in the organic and aqueous phase by g-spectrometry had conducted to estimate the apparent distribution coefficient D as function of free sulphate ions. Complexation constants have been determined after a mathematical treatment of D. The extrapolation of these constants at zero ionic strength have been realized by SIT modelling at different temperatures. Besides, enthalpy and entropy values were calculated. Parallelly, the structural study of Pa(V) was performed using 231 Pa. XANES and EXAFS spectra show unambiguously the absence of the

  1. A Record of Uranium-Series Transport in Fractured, Unsaturated Tuff at Nopal I, Sierra Peña Blanca, Chihuahua, Mexico

    Science.gov (United States)

    Denton, J.; Goldstein, S. J.; Paviet, P.; Nunn, A. J.; Amato, R. S.; Hinrichs, K. A.

    2015-12-01

    In this study we utilize U-series disequilibria measurements to investigate mineral fluid interactions and the role fractures play in the geochemical evolution of an analogue for a high level nuclear waste repository, the Nopal I uranium ore deposit. Samples of fracture-fill materials have been collected from a vertical drill core and surface fractures. High uranium concentrations in these materials (12-7700 ppm) indicate U mobility and transport from the deposit in the past. U concentrations generally decrease with horizontal distance away from the ore deposit but show no trend with depth. Isotopic activity ratios indicate a complicated geochemical evolution in terms of the timing and extent of actinide mobility, possibly due to changing environmental (redox) conditions over the history of the deposit. 234U/238U activity ratios are generally distinct from secular equilibrium and indicate some degree of open system U behavior during the past 1.2 Ma. However, calculated closed system 238U-234U-230Th model ages are generally >313 ka and >183 ka for the surface fracture and drill core samples respectively, suggesting closed system behavior for U and Th over this most recent time period. Whole rock isochrons drawn for the drill core samples show that at two of three depths fractures have remained closed with respect to U and Th mobility for >200 ka. However, open system behavior for U in the last 350 ka is suggested at 67 m depth. 231Pa/235U activity ratios within error of unity suggest closed system behavior for U and Pa for at least the past 185 ka. 226Ra/230Th activity ratios are typically <1 (0.7-1.2), suggesting recent (<8 ka) radium loss and mobility due to ongoing fluid flow in the fractures. Overall, the mainly closed system behavior of U-Th-Pa over the past ~200 ka provides one indicator of the geochemical immobility of these actinides over long time-scales for potential nuclear waste repositories sited in fractured, unsaturated tuff.

  2. A Nd Isotopic Composition Modeling Approach of the Oceanic Thermohaline Circulation Change During LGM

    Science.gov (United States)

    Arsouze, T.; Dutay, J.; Lacan, F.; Jeandel, C.; Alkama, R.; Kageyama, M.; Piotrowski, A.

    2006-12-01

    The role of thermohaline circulation in climate change has been a matter of debate for a long time. Proxies of past ocean circulation such as δ13C or 231Pa/230Th suggest a relationship between North Atlantic Deep Water (NADW) strength and rapid climate change. Neodymium isotopic composition (Nd IC) is a quasi conservative geochemical tracer of water masses in the ocean interior and thus can be used as a proxy for NADW. Seawater Nd IC being recorded in marine sediments, this proxy is used to infer paleo-circulations on various time scales. Recent studies of Nd IC records, in the ferromanganese oxide components of a South Atlantic core, confirm the close relation between thermohaline circulation and North Atlantic climate changes through the last deglaciation (Piotrowski et al., 2004). Our purpose here is to model the Nd IC during the LGM and the Holocene with the Ocean Global Circulation Model NEMO, in the ORCA2 (2°) configuration. The explicit simulation of this proxy in the model allows to investigate and quantify the circulation change that corresponds to the Nd isotopic composition variation recorded in the sediments. We consider that the main source of Nd into the ocean is the interaction between water masses and continental margins (Boundary Exchange process; (Lacan and Jeandel, 2005). Boundary exchange is parameterized using a relaxing term (Arsouze et al., 2006). Simulated Nd IC distributions are evaluated by comparison with available records for the LGM and Holocene. References: Arsouze, T., Dutay, J.-C., Lacan, F. and Jeandel, C., 2006. Modeling the neodymium isotopic composition with a global ocean circulation model Chemical Geology, in press. Lacan, F. and Jeandel, C., 2005. Neodymium isotopes as a new tool for quantifying exchange fluxes at the continent - ocean interface. Earth and Planetary Science Letters, 232(3-4): 245-257. Piotrowski, A.M., Goldstein, S.L., Hemming, S.R. and Fairbanks, R.G., 2004. Intensification and variability of ocean

  3. No iron fertilization in the equatorial Pacific Ocean during the last ice age.

    Science.gov (United States)

    Costa, K M; McManus, J F; Anderson, R F; Ren, H; Sigman, D M; Winckler, G; Fleisher, M Q; Marcantonio, F; Ravelo, A C

    2016-01-28

    The equatorial Pacific Ocean is one of the major high-nutrient, low-chlorophyll regions in the global ocean. In such regions, the consumption of the available macro-nutrients such as nitrate and phosphate is thought to be limited in part by the low abundance of the critical micro-nutrient iron. Greater atmospheric dust deposition could have fertilized the equatorial Pacific with iron during the last ice age--the Last Glacial Period (LGP)--but the effect of increased ice-age dust fluxes on primary productivity in the equatorial Pacific remains uncertain. Here we present meridional transects of dust (derived from the (232)Th proxy), phytoplankton productivity (using opal, (231)Pa/(230)Th and excess Ba), and the degree of nitrate consumption (using foraminifera-bound δ(15)N) from six cores in the central equatorial Pacific for the Holocene (0-10,000 years ago) and the LGP (17,000-27,000 years ago). We find that, although dust deposition in the central equatorial Pacific was two to three times greater in the LGP than in the Holocene, productivity was the same or lower, and the degree of nitrate consumption was the same. These biogeochemical findings suggest that the relatively greater ice-age dust fluxes were not large enough to provide substantial iron fertilization to the central equatorial Pacific. This may have been because the absolute rate of dust deposition in the LGP (although greater than the Holocene rate) was very low. The lower productivity coupled with unchanged nitrate consumption suggests that the subsurface major nutrient concentrations were lower in the central equatorial Pacific during the LGP. As these nutrients are today dominantly sourced from the Subantarctic Zone of the Southern Ocean, we propose that the central equatorial Pacific data are consistent with more nutrient consumption in the Subantarctic Zone, possibly owing to iron fertilization as a result of higher absolute dust fluxes in this region. Thus, ice-age iron fertilization in the

  4. Compressive Test and Simulation of Cassava Stems Based on ANSYS%基于ANSYS的木薯茎秆静力学仿真研究

    Institute of Scientific and Technical Information of China (English)

    薛忠; 张衍林; 张劲; 陈实

    2016-01-01

    In this paper , on the basis of cassava stalk mechanical test , application of computer simulation to simulate and analyze the mechanics of cassava stalk in the failure limit state .During the dissertation , analysed composite structure of cassava stalk , gave the relationship of various types of material between the flexible matrix and the engineering constants ,and assumed material types of cassava stalk .Result show:( 1 ) The shear stress of the XY direction on phloem fiber is in the range of -0.002 195~-0.000 231Pa,the shear stress of the XY direction on xylem is in the range of -0.000 231~0.000 014Pa, the maximum shear stress of the XY direction is at the junction of the xylem and phloem fiber which value is -0.002 195Pa, the minimum shear stress of the XY direction is on the xylem which value is 0.000 14Pa;shear stress of YZ direction and XZ direction has the symmetry , the shear stress of stalk at direction of YZ and XZ are concentrated on -3.07E-10~-4.58E-11Pa,the maximum shear stress of YZ or XZ direction is -2.42E-9Pa,the minimum shear stress of YZ or XZ direction is 4.59E-11Pa.(2) The shear stress of XY、YZ、XZ direction present their different laws when pressure model on the lateral , but they all distribute symmetrically .The maximum shear stress of the XY direction is ±1.746 49Pa,the minimum shear stress is ±0.194 054Pa;the maximum shear stress of the YZ direction is ±0.456 2Pa, the minimum shear stress is ±0.005 063Pa, the maximum shear stress of the XZ direction is ±0.260 701Pa, the minimum shear stress is ±0.028 967Pa.%以木薯茎秆力学试验为基础,应用计算机仿真手段模拟分析了木薯茎秆在失效极限状态下的力学状况. 使用万能试验机对木薯茎秆的主要力学成分(木质部、韧皮纤维)进行拉压试验,分别测定了木质部和韧皮纤维的多组弹性模量数据. 研究表明:①韧皮纤维处的 XY 方向切应力在-0 .002 195 ~-0 .000 231 Pa 范围内,

  5. Using U-series and beryllium isotopes to reveal the occurrence and relative timing of crustal and mantle processes in the Southern Volcanic Zone of Chile

    Science.gov (United States)

    Cooper, L. B.; Reubi, O.; Dungan, M. A.; Bourdon, B.; Langmuir, C. H.; Turner, S. J.; Schaefer, J. M.

    2012-12-01

    the main edifice have been mixed with magma compositions similar to those at surrounding minor eruptive centers (Hickey-Vargas et al., 2002). The latter appear to be decompression melts of enriched mantle which manifest moderate U-Th-Ra disequilibrium and substantial 231Pa-excesses, whereas melts from Villarrica have substantial U- and Ra-excesses. Magmas from Osorno reflect a greater influence of sediments originating from the incoming slab. After discounting assimilated samples, all primary melts have uniformly high Pa-excesses (1.7-2.2) coincident with large variations in 238U-230Th disequilibria. Fluid addition-aging-melting successions at Antuco and Chillán may have led to compositions near U-Th equilibrium or with Th-excesses, respectively. Primary Ra-deficits at Chillán, Lonquimay, and Osorno are under investigation and potentially reflect melting of a cumulate body. Forthcoming 10Be data for select U-series samples will enable further clarification of the regional trend. Preliminary analyses of nine Llaima samples erupted between 1850 and 2009 confirm the successful elimination of a meteoric 10Be component and produce a data array consistent with assimilation. The invocation of radioactive decay to produce U-Th equilibrium (duration of at least 380 ky) could also explain the low 10Be/9Be compositions (half-life of 10Be=1,390 ky). Our comprehensive dataset may shed new light on melting processes in subduction zone systems.

  6. Rates of carbonate soil evolution from carbon, U- and Th-series isotope studies: Example of the Astian sands (SE France)

    Science.gov (United States)

    Barbecot, Florent; Ghaleb, Bassam; Hillaire-Marcel, Claude

    2015-04-01

    In carbonate rich soils, C-isotopes (14C, 13C) and carbonate mass budget may inform on centennial to millennial time scale dissolution/precipitation processes and weathering rates, whereas disequilibria between in the U- and Th-decay series provide tools to document high- (228Ra-228Th-210Pb) to low- (234U, 230Th, 231Pa, 226Ra) geochemical processes rate, covering annual to ~ 1Ma time scales, governing both carbonate and silicate soil fractions. Because lithology constitutes a boundary condition, we intend to illustrate the behavior of such isotopes in soils developed over Astian sands formation (up to ~ 30% carbonate) from the Béziers area (SE France). A >20 m thick unsaturated zone was sampled firstly along a naturally exposed section, then in a cored sequence. Geochemical and mineralogical analyses, including stable isotopes and 14C-measurements, were complemented with 228U, 234U, 230Th, 226Ra, 210Pb and 228Th, 232Th measurements. Whereas the upper 7 m depict geochemical and isotopic features forced by dissolution/precipitation processes leading to variable radioactive disequilibria, but overall deficits in more soluble elements of the decay series, the lower part of the sequence shows strong excesses in 234U and 230Th over parent isotopes (i.e., 238U and 234U, respectively). These features might have been interpreted as the result of successive phases of U-loss and gains. However, 226Ra and 230Th are in near-equilibrium, thus leading to conclude at a more likely slow enrichment process in both 234Th(234U) and 230Th, which we link to dissolved U-decay during groundwater recharge events. In addition, 210Pb deficits (vs parent 226Ra) are observed down to 12 m along the natural outcropping section and below the top-soil 210Pb-excess in the cored sequence, due to gaseous 222Rn-diffusion over the cliff outcrop. Based on C-isotope and chemical analysis, reaction rates at 14C-time scale are distinct from those estimates at the short- or long-lived U-series isotopes

  7. 40Ar/39Ar ages of the older eruptive units of Somma-Vesuvius volcano, Italy

    Science.gov (United States)

    Lanphere, M. A.; Calvert, A. T.; Scarpati, C.; Melluso, L.; Morra, V.; Perrotta, A.; Thornber, C.; Cioni, R.; Champion, D. E.

    2008-12-01

    others, 1971, 1973, 1974, and 1978, University of Rome Carbon-14 Dates IX: Radiocarbon, v. 13, 15, 16, and 20. Chiu, T.C., Fairbanks, R.G., Cal, L., and Mortlock, R.A., 2007, Analysis of the atmospheric 14C record spanning the past 50,000 years derived from high-precision 230Th/234U/238U, 231Pa/235U, and 14C dates on corals: Quaternary Science Reviews, 26:18-36. Delibrias, G., DiPaola, G.M., Rosi, M., and Santacroce, R., 1979, La Storia Eruttiva Del Complesso Volcanico Somma Vesuvio Ricostruita Dalle Successioni Piroclastiche Del Monte Somma; Rendiconti Societa Italiana di Mineralogia e Petrologia, 35:411-438. Reimer, P.J.and others, 2004, IntCal04 Terrestrial Radiocarbon Age Calibration, 0-26 Kyr BP: Radiocarbon, 46:1029-1058. Sigurdsson, H., Carey, S., Cornell, W., and Pesdatore, T., 1985, The Eruption of Vesuvius in A.D. 79, 1985: National Geographic Research, 1:332-387.

  8. 一种用于铀同位素比值α能谱分析的磷化膜制源新技术%A New Source-preparation Technique of Phosphate Conversion Coating Used in the Determination of Uranium Isotope Ratio by Alpha Spectrometry

    Institute of Scientific and Technical Information of China (English)

    王哲; 王玉学; 郭冬发; 付琳; 黄秋红; 孙伟; 陈春军

    2016-01-01

    A new source-preparation technique of uranium phosphate conversion coating was developed for the determination of uranium isotope ratio by alpha spectrometry. It was found experimentally that under the conditions of 3.14 cm2 Ni-foil,0.5 mol/L HCl,2.5 mol/L NaCl ,0.08 mol/L KH 2 PO 4 ,20 g/L ascorbic acid ,25 mL initial solution,90℃ constant experiment temperature,1 60 r/min vibration frequency ,20 mm vibration amplitude,and 70min deposition time ,uranium less than 200 μg can be quantitatively and spontaneously converted into phosphorization film on Ni-foil. Compared to the tradi-tional source-preparation technique of electro-deposition,the technique of uranium phosphate conversion coating has the advantage of simple in electro-deposition device, easy in operation, high working-efficiency ,no interference in measuring lots of coexisting radionuclides such as 2 3 2 Th ,2 30 Th,22 6 Ra,2 3 1 Pa and so on in phosphating solution. The total spike recovery rate of uranium reaches 100% nearly,and the spectrum resolution is good in determing uranium isotope ratio by alpha spectrometry.%研发了一种用于铀同位素比值α能谱分析的磷化膜制源新技术.试验发现,当镍镀片面积为3.14 cm2,盐酸浓度为0.5 mol/L ,氯化钠浓度为2.5 mol/L ,磷酸二氢钾浓度为0.08 mol/L,抗坏血酸浓度为20 g/L,溶液体积为25 mL,恒温90℃,振荡速率为160次/min,振程20 mm 时,磷化膜制源70 min,200μg 以下的铀可在镍箔上定量转化为磷化膜.与传统的电沉积制源技术相比较,应用磷化膜制源技术进行测量源制备时无需电沉积装置,制源过程简单快速,工效高,大量共存的232 Th 、230 Th、226 Ra、231 Pa 等核素均不产生干扰,铀的全程回收率接近100%,α能谱峰分辨率较好.

  9. Fission and Properties of Neutron-Rich Nuclei - Proceedings of the Second International Conference

    Science.gov (United States)

    Hamilton, J. H.; Phillips, W. R.; Carter, H. K.

    Long Range Alpha Emission Probabilities in the Thermal and Resonance for 239Pu * Spectroscopy of Selected Fission Fragments * Gamma-Ray Spectra of Individual Fission Products * Gamma Spectroscopy of the Transfermium Nucleus Nobelium-254 * Summary of the Yield Values from Fast Fission of 233U Measured of Studsvik * Decay Studies of Neutron-Rich Isotopes Produced in Proton-Induced Fission of Actinides * Understanding of the Fission Process From the Deformation Properties of Fissioning Nuclei * Heavy Clusterization in 252Cf: An Application of the U(3) Selection Rule * Synthesis of Superheavy Elements with Three-Dimensional Fluctuation-Dissipation Dynamical Model * Asymmetric Fission Along Nuclear Lattice Planes * Experimental Study of Correlations Between Fission Neutron Multiplicity, Mass and Kinetic Energy of Fission Fragments From Spontaneous Fission of 252Cf, 244Cm and 248Cm * Super- and Hyper-Deformed Isomeric States and Long-Lived Superheavy Elements * Systematic Investigation of the Neutron Induced Fission Reaction 235, 238U and 237Np below 6 MeV * Studying Iso-chains with RNBs * Cold Fission Studies with Large Detector Arrays * Single-Particle States in Transcurium Nuclei * Shell Effects and Fission of Superheavy Nuclei at Low Excitation Energies * Experiments on the Synthesis of Superheavy Nuclei in 48Ca-Induced Reactions * GSI Experiments on the Synthesis of Superheavy Elements - Results and Plans for the Future * Spectroscopy of Refractory Fission Products at IGISOL * Ternary Fission Induced by Polarized Neutrons * Neutron Decay of Ternary Particles in Spontaneous Fission of 252Cf * New Fission Modes * Alpha Clustering and Ternary Fission * Interplay of Fusion and Fission Dynamics * Applications of the Hartree Bogoliubov Model to Nuclei with Large Isospin Values * Structure of Neutron-Rich Pd Isotopes * Systematic Studies of Fission Saddle-Point Shapes and Their Relation to the Maxima of the Fission-Fragment Mass and Kinetic-Energy Distributions * Limits of

  10. Transmutation of radioactive nuclear waste

    Energy Technology Data Exchange (ETDEWEB)

    Toor, A; Buck, R

    2000-03-15

    Lack of a safe disposal method for radioactive nuclear waste (RNW) is a problem of staggering proportion and impact. A typical LWR fission reactor will produce the following RNW in one year: minor actinides (i.e. {sup 237}Np, {sup 242-243}Am, {sup 243-245}Cm) {approx}40 kg, long-lived fission products (i.e, {sup 99}Tc, {sup 93}Zr, {sup 129}I, {sup 135}Cs) {approx}80 kg, short lived fission products (e.g. {sup 137}Cs, {sup 90}Sr) {approx}50kg and plutonium {approx}280 kg. The total RNW produced by France and Canada amounts to hundreds of metric tonnes per year. Obtaining a uniform policy dealing with RNW has been blocked by the desire on one hand to harvest the energy stored in plutonium to benefit society and on the other hand the need to assure that the stockpile of plutonium will not be channeled into future nuclear weapons. In the meantime, the quantity and handling of these materials represents a potential health hazard to the world's population and particularly to people in the vicinity of temporary storage facilities. In the U.S., societal awareness of the hazards associated with RNW has effectively delayed development of U.S. nuclear fission reactors during the past decade. As a result the U.S. does not benefit from the large investment of resources in this industry. Reluctance to employ nuclear energy has compelled our society to rely increasingly on non-reusable alternative energy sources; coal, oil, and natural gas. That decision has compounded other unresolved global problems such as air pollution, acid rain, and global warming. Relying on these energy sources to meet our increasing energy demands has led the U.S. to increase its reliance on foreign oil; a policy that is disadvantageous to our economy and our national security. RNW can be simplistically thought of as being composed of two principal components: (1) actinides with half lives up to 10{sup 6} years and (2) the broad class of fission fragments with typical half lives of a few hundred

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

    Energy Technology Data Exchange (ETDEWEB)

    Rudisill, T.; Kyser, E.

    2010-09-02

    -vis spectroscopy demonstrated that Np(V) and Pu(III) were the predominate valences in the lactic acid/DTPA solution for the better part of a day following solution preparation. Based on these results, we chose to initially add HAN to the actinide tracer solution prepared for the distribution coefficient measurements (to produce Pu(III)) prior to combining with lactic acid and DTPA. The distribution coefficient measurements were expected to be complete in 2-3 h; therefore, Np(V) and Pu(III) valences would predominate in the solution during this time. Prior to adding the HAN to the actinide tracers, we added sufficient Am(III) activity to allow the measurement of distribution coefficients during the extraction experiments. Protactinium (V) distribution coefficients were also measured using the activity which was in secular equilibrium with the {sup 237}Np. The actinide distribution coefficients were measured at pH 2.8 and 3.5 and covered a range of temperatures from nominally 20 to 60 C.