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Sample records for calculating actinide isotope

  1. Calculated Atomic Volumes of the Actinide Metals

    DEFF Research Database (Denmark)

    Skriver, H.; Andersen, O. K.; Johansson, B.

    1979-01-01

    The equilibrium atomic volume is calculated for the actinide metals. It is possible to account for the localization of the 5f electrons taking place in americium.......The equilibrium atomic volume is calculated for the actinide metals. It is possible to account for the localization of the 5f electrons taking place in americium....

  2. Production of actinide isotopes in simulated PWR fuel and their influence on inherent neutron emission

    International Nuclear Information System (INIS)

    This report describes calculations that examine the sensitivity of actinide isotopes to various reactor parameters. The impact of actinide isotope build-up, depletion, and decay on the neutron source rate in a spent-fuel assembly is determined, and correlations between neutron source rates and spent-fuel characteristics such as exposure, fissile content, and plutonium content are established. The application of calculations for evaluating experimental results is discussed

  3. Calculated Bulk Properties of the Actinide Metals

    DEFF Research Database (Denmark)

    Skriver, Hans Lomholt; Andersen, O. K.; Johansson, B.

    1978-01-01

    Self-consistent relativistic calculations of the electronic properties for seven actinides (Ac-Am) have been performed using the linear muffin-tin orbitals method within the atomic-sphere approximation. Exchange and correlation were included in the local spin-density scheme. The theory explains t...... the variation of the atomic volume and the bulk modulus through the 5f series in terms of an increasing 5f binding up to plutonium followed by a sudden localisation (through complete spin polarisation) in americium...

  4. Preparation of isotopes and sources of actinide elements

    International Nuclear Information System (INIS)

    As the C.E.A. possesses no isotopic separation facility, the productions of isotopes of actinide elements are performed: a) by neutron irradiation and chemical treatment of special targets, b) by milking decay products from stocks of aged actinide elements, c) by chemical treatment of alpha active wastes. These productions concern the following isotopes: 233U, 238Pu, 242Pu, 243Cm, 242Cm, 244Cm (a); 228Th, 229Th, 234U, 237U, 239Np, 240Pu, 241Am, 248Cm (b); 237Np, 241Am (c). These isotopes are produced to satisfy French and international needs and are sent to users in various forms: solutions, metals, oxides, fluorides, or in different sources forms. The preparation of the sources represents an important field of activities divided into two parts: 1/Industrial sources: production of large series of different sources, 2/ Scientific sources: production of sources suitable for a specific scientific problem. A large overview of these activities is given

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

    International Nuclear Information System (INIS)

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

  6. Comparative analysis between measured and calculated concentrations of major actinides using destructive assay data from Ohi-2 PWR

    Directory of Open Access Journals (Sweden)

    Oettingen Mikołaj

    2015-09-01

    Full Text Available In the paper, we assess the accuracy of the Monte Carlo continuous energy burnup code (MCB in predicting final concentrations of major actinides in the spent nuclear fuel from commercial PWR. The Ohi-2 PWR irradiation experiment was chosen for the numerical reconstruction due to the availability of the final concentrations for eleven major actinides including five uranium isotopes (U-232, U-234, U-235, U-236, U-238 and six plutonium isotopes (Pu-236, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242. The main results were presented as a calculated-to-experimental ratio (C/E for measured and calculated final actinide concentrations. The good agreement in the range of ±5% was obtained for 78% C/E factors (43 out of 55. The MCB modeling shows significant improvement compared with the results of previous studies conducted on the Ohi-2 experiment, which proves the reliability and accuracy of the developed methodology.

  7. Actinides record, power calculations and activity for present isotopes in the spent fuel of a BWR; Historial de actinidos y calculos de potencia y actividad para isotopos presentes en el combustible gastado de un BWR

    Energy Technology Data Exchange (ETDEWEB)

    Enriquez C, P.; Ramirez S, J. R.; Lucatero, M. A., E-mail: pastor.enriquez@inin.gob.mx [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico)

    2012-10-15

    The administration of spent fuel is one of the more important stages of the nuclear fuel cycle, and this has become a problem of supreme importance in countries that possess nuclear reactors. Due to this in this work, the study on the actinides record and present fission products to the discharge of the irradiated fuel in a light water reactor type BWR is shown, to quantify the power and activity that emit to the discharge and during the cooling time. The analysis was realized on a fuel assembly type 10 x 10 with an enrichment average of 3.69 wt % in U-235 and the assembly simulation assumes four cycles of operation of 18 months each one and presents an exposition of 47 G Wd/Tm to the discharge. The module OrigenArp of the Scale 6 code is the computation tool used for the assembly simulation and to obtain the results on the actinides record presents to the fuel discharge. The study covers the following points: a) Obtaining of the plutonium vector used in the fuel production of mixed oxides, and b) Power calculation and activity for present actinides to the discharge. The results presented in this work, correspond at the same time immediate of discharge (0 years) and to a cooling stage in the irradiated fuel pool (5 years). (Author)

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

    Energy Technology Data Exchange (ETDEWEB)

    Perkasa, Y. S. [Department of Physics, Sunan Gunung Djati State Islamic University Bandung, Jl. A.H Nasution No. 105 Cibiru, Bandung (Indonesia); Waris, A., E-mail: awaris@fi.itb.ac.id; Kurniadi, R., E-mail: awaris@fi.itb.ac.id; Su' ud, Z., E-mail: awaris@fi.itb.ac.id [Nuclear Physics and Biophysics Research Division, Department of Physics, Faculty of Mathematics and Natural Sciences, Institut Teknologi Bandung, Jl. Ganesa No. 10 Bandung 40132 (Indonesia)

    2014-09-30

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

  9. Self-interaction corrected local spin density calculations of actinides

    DEFF Research Database (Denmark)

    Petit, Leon; Svane, Axel; Szotek, Z;

    2010-01-01

    We use the self-interaction corrected local spin-density approximation in order to describe localization-delocalization phenomena in the strongly correlated actinide materials. Based on total energy considerations, the methodology enables us to predict the ground-state valency configuration of the...

  10. Calculation of binary phase diagrams between the actinide elements, rare earth elements, and transition metal elements

    International Nuclear Information System (INIS)

    Attempts were made to apply the Kaufman method of calculating binary phase diagrams to the calculation of binary phase diagrams between the rare earths, actinides, and the refractory transition metals. Difficulties were encountered in applying the method to the rare earths and actinides, and modifications were necessary to provide accurate representation of known diagrams. To calculate the interaction parameters for rare earth-rare earth diagrams, it was necessary to use the atomic volumes for each of the phases: liquid, body-centered cubic, hexagonal close-packed, and face-centered cubic. Determination of the atomic volumes of each of these phases for each element is discussed in detail. In some cases, empirical means were necessary. Results are presented on the calculation of rare earth-rare earth, rare earth-actinide, and actinide-actinide diagrams. For rare earth-refractory transition metal diagrams and actinide-refractory transition metal diagrams, empirical means were required to develop values for the enthalpy of vaporization for rare earth elements and values for the constant (C) required when intermediate phases are present. Results of using the values determined for each element are presented

  11. A calculation for radial expectation values of helium like actinide ions (Z=89-93)

    Science.gov (United States)

    Ürer, G.; Arslan, M.; Balkaya, E.; Keçeli, A.

    2016-03-01

    Radial expectation values, , for helium like actinides (ZAc=89, ZTh=90, ZPa=91, ZU=92, and ZNp=93) are reported using the Multiconfiguration Hartree-Fock (MCHF) within the framework Breit-Pauli corrections. Atomic data as energy levels, wavelengths, weighted oscillator strengths, and transition probabilities for allowed and forbidden transitions need these calculations. The obtained results are compared available works.

  12. Results of coupled channels calculations for the neutrons cross sections of a set of actinide nuclei

    International Nuclear Information System (INIS)

    This report gathers recents results of neutrons interactions with the following actinide nuclei: 230Th, 232Th, 234U, 238U, 242Pu, 246Cm and 252Cf from the use of the coupled channels optical model. Tabulations of the following quantities are given in Annexe: total, direct elastic and inelastic scattering (integrated and differential), and compound nucleus formation cross sections; ground state generalized transmission coefficients needed to calculate the cross sections of partial compound nucleus processes. This work was carried out within the framework of the IAEA-NDS Coordinated Research Programme on the Intercomparison of Actinide Neutron Cross Section Evaluations

  13. Fast neutron capture in actinide isotopes: recent results from Karlsruhe

    International Nuclear Information System (INIS)

    Capture gamma-ray spectra of 241Am, 240Pu, 242Pu 238U and 197Au were calculated in the framework of the spherical optical model and the statistical model. These spectra were used to correct experimental data for the capture cross sections of 240242Pu and 241Am from relative measurements using a Moxon Rae-detector with graphite converter and 197Au as well as 238U as standards. This correction is required to take into account that the detector efficiency is not exactly proportional to gamma-ray energy. The resulting correction factors proved to be negligible for measurements relative to 238U, whereas they are approx. 3% if gold is used as a standard. The capture cross section of 243Am has been measured in the energy range 10 to 250 keV using kinematically collimated neutrons from the 7Li(p,n) and T(p,n) reaction. The samples are positioned at flight paths of 5 to 7 cm and gold was used as a standard. Capture events were detected by two Moxon-Rae detectors with graphite and bismuth-graphite converters shielded by 0.5 to 2 cm of lead. Fission events were detected by a NE213 liquid scintillator. The present status of the experiment and some preliminary results will be presented

  14. Isopiestic density law of actinide nitrates applied to criticality calculations

    International Nuclear Information System (INIS)

    Up to now, criticality safety experts used density laws fitted on experimental data and applied them in and outside the measurement range. Depending on the case, such an approach could be wrong for nitrate solutions. Seven components are concerned: UO2(NO3)2, U(NO3)4, Pu(NO3)4, Pu(NO3)3, Th(NO3)4, Am(NO3)3 and HNO3. To get rid of this problem, a new methodology based on the thermodynamic concept of binary electrolytes solutions mixtures at constant water activity, so called 'isopiestic' solutions, has been developed by IRSN to calculate the nitrate solutions density. This article shortly presents the theoretical aspects of the method, its qualification using benchmarks and its implementation in IRSN graphical user interface. (author)

  15. Calculation of cross sections for heavy isotopes

    International Nuclear Information System (INIS)

    In the present work an integrated system of codes for basic neutron data evaluation were assembled and built. Complete evaluations for the isotopes 240Pu, 241Pu, 242Pu and 238Pu were performed. The following cross sections: total, elastic, radiative capture, fission, total inelastic, partial inelastic, (n,2n), (n,3n) and differential elastic were evaluated as well as the average number of neutrons per neutron-induced fission and the average elastic scattering cosine in the lab system.The data for the plutonium isotopes were incorporated into the German KEDAK file. A method was developed for calculating the energy distributions of the second and third secondary neutrons from the A(n,2n) and (n,3n) reactions in the framework of the compound nucleus theory, and utilizing the nuclear data of the nuclei A, A-1, A-2. This method was used to generate the 238U secondary neutron energy distributions in the incident neutron energy range of 6 to 15 MeV. A nuclear data evaluation for 237U in the resolved inelastic scattering range (10-700 keV) was performed. The compound elastic and partial inelastic scattering cross sections were used in the 238U secondary neutron energy distribution calculations. (B.G.)

  16. Hydride interference on the determination of minor actinide isotopes by inductively coupled plasma mass spectrometry

    International Nuclear Information System (INIS)

    Hydrogen adducts of the major naturally occurring actinide isotopes 232Th and 238U were studied using an inductively coupled plasma mass spectrometer. The hydride:atomic ion ratios for both elements varied as a function of the parameters that were studied, i.e., nebulizer flow rate, solution uptake rate and desolvation conditions. When the instrument sensitivity for U and Th was optimized, 232ThH+:232Th+ was found to be (3.9±0.2) x 10-5 with pneumatic nebulization and (2.10±0.07) x 10-5 with ultrasonic nebulization. Under the same conditions, 238UH+:238U+ was found to be (3.2±0.2) x 10-5 and (1.8±0.1) x 10-5 using pneumatic and ultrasonic nebulization, respectively. Conditions that reduced hydrogen number density and/or increased plasma temperature decreased the hydride:atomic ion ratio. Such conditions are best if 233U and 239Pu are to be determined in the presence of 232Th and 238U. (Author)

  17. AMS of actinides in groundwater: development of a new procedure for trace analysis of Np, Pu, Am and Cm isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Quinto, Francesca; Lagos, Markus; Plaschke, Markus; Schaefer, Thorsten; Geckeis, Horst [Karlsruhe Institute of Technology, Institute for Nuclear Waste Disposal (KIT-INE), Hermann-von Helmholtz-Platz 1, D-76344 Eggenstein-Leopoldshafen (Germany); Steier, Peter [VERA Laboratory, Faculty of Physics, University of Vienna, Waehringer Strasse 17, A-1090 Vienna (Austria)

    2014-07-01

    In order to assess the actinides contamination in groundwater, their geochemistry is intensely studied in field and laboratory experiments focusing on speciation and ways of transport through the aquifers. A challenge lies in the analysis of actinides below ppq levels. We present a new analytical protocol suited to the measurement by accelerator mass spectrometry of Np, Pu, Am and Cm isotopes without previous chemical separation from each other. The actinides are quantitatively co-precipitated with Fe-hydroxide from the groundwater specimens. This procedure allows the pre-concentration of the actinides from the bulk elements and their incorporation into a sample matrix suited to the AMS measurements. The chemical yield of the co-precipitation is estimated measuring samples with suitable spikes by HR ICP-MS. At the AMS sytem: (a) the ionization yield of Np, Pu, Am and Cm in the given sample matrix, (b) the maximum number of nuclides per sample allowing detection limits below 0.01 ppq, and (c) the influence of the laboratory background on the results, are determined.

  18. The procedure and results of calculations of the equilibrium isotopic composition of a demonstration subcritical molten salt reactor

    Energy Technology Data Exchange (ETDEWEB)

    Nevinitsa, V. A., E-mail: Neviniza-VA@nrcki.ru; Dudnikov, A. A.; Blandinskiy, V. Yu.; Balanin, A. L.; Alekseev, P. N. [National Research Centre Kurchatov Institute (Russian Federation); Titarenko, Yu. E.; Batyaev, V. F.; Pavlov, K. V.; Titarenko, A. Yu., E-mail: yuri.titarenko@itep.ru [Institute for Theoretical and Experimental Physics (Russian Federation)

    2015-12-15

    A subcritical molten salt reactor with an external neutron source is studied computationally as a facility for incineration and transmutation of minor actinides from spent nuclear fuel of reactors of VVER-1000 type and for producing {sup 233}U from {sup 232}Th. The reactor configuration is chosen, the requirements to be imposed on the external neutron source are formulated, and the equilibrium isotopic composition of heavy nuclides and the key parameters of the fuel cycle are calculated.

  19. The procedure and results of calculations of the equilibrium isotopic composition of a demonstration subcritical molten salt reactor

    Science.gov (United States)

    Nevinitsa, V. A.; Dudnikov, A. A.; Blandinskiy, V. Yu.; Balanin, A. L.; Alekseev, P. N.; Titarenko, Yu. E.; Batyaev, V. F.; Pavlov, K. V.; Titarenko, A. Yu.

    2015-12-01

    A subcritical molten salt reactor with an external neutron source is studied computationally as a facility for incineration and transmutation of minor actinides from spent nuclear fuel of reactors of VVER-1000 type and for producing 233U from 232Th. The reactor configuration is chosen, the requirements to be imposed on the external neutron source are formulated, and the equilibrium isotopic composition of heavy nuclides and the key parameters of the fuel cycle are calculated.

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

    Directory of Open Access Journals (Sweden)

    Ishizuka Chikako

    2016-01-01

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

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

    Science.gov (United States)

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

    2016-06-01

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

  2. PC/FRAM: A code for the nondestructive measurement of the isotopic composition of actinides for safeguards applications

    Energy Technology Data Exchange (ETDEWEB)

    Sampson, T.E.; Kelley, T.A.

    1996-12-01

    The Nuclear Safeguards Program at the Los Alamos National Laboratory has developed and fielded techniques for the gamma-ray spectrometry measurement of the isotopic composition of plutonium and other actinides for over 20 years, ever since Parker and Reilly first proposed a practical method for the measurement of the arbitrary sample. Their procedures, incorporating internal (to the measured gamma-ray spectrum) or {open_quotes}intrinsic{close_quotes} self-determination of the relative efficiency function of the sample-detector measurement system, are widely applied today. The PC/FRAM code is the most recent and most highly-developed Los Alamos code developed specifically for the nuclear safeguards applications of this technique. We will describe the measurement principles that allow accurate measurements to be taken on samples of arbitrary size, shape, and measurement geometry- and of arbitrary physical and chemical composition-through the use of known nuclear decay data (half-lives and branching intensities). Subsequently, we will describe the analysis methodology, which is driven by an easily edited parameter file that frees the user from dependence on a dedicated programmer for analyses of special cases. This methodology relies on internal gamma-ray peaks from the spectrum under analysis to self-calibrate the unknown spectrum for energy and peak shape (energy dependence of full width at half maximum (FWHM) and tailing parameters). The program uses these parameters to calculate response functions that are fit to the analysis peaks requested in the parameter file. The structure of the code and its Windows 3.1 user interface allows use with equal ease by the experienced spectroscopist or operator-level personnel in a working facility.

  3. Calculation of individual isotope equilibrium constants for geochemical reactions

    Science.gov (United States)

    Thorstenson, D.C.; Parkhurst, D.L.

    2004-01-01

    Theory is derived from the work of Urey (Urey H. C. [1947] The thermodynamic properties of isotopic substances. J. Chem. Soc. 562-581) to calculate equilibrium constants commonly used in geochemical equilibrium and reaction-transport models for reactions of individual isotopic species. Urey showed that equilibrium constants of isotope exchange reactions for molecules that contain two or more atoms of the same element in equivalent positions are related to isotope fractionation factors by ?? = (Kex)1/n, where n is the number of atoms exchanged. This relation is extended to include species containing multiple isotopes, for example 13C16O18O and 1H2H18O. The equilibrium constants of the isotope exchange reactions can be expressed as ratios of individual isotope equilibrium constants for geochemical reactions. Knowledge of the equilibrium constant for the dominant isotopic species can then be used to calculate the individual isotope equilibrium constants. Individual isotope equilibrium constants are calculated for the reaction CO2g = CO2aq for all species that can be formed from 12C, 13C, 16O, and 18O; for the reaction between 12C18 O2aq and 1H218Ol; and among the various 1H, 2H, 16O, and 18O species of H2O. This is a subset of a larger number of equilibrium constants calculated elsewhere (Thorstenson D. C. and Parkhurst D. L. [2002] Calculation of individual isotope equilibrium constants for implementation in geochemical models. Water-Resources Investigation Report 02-4172. U.S. Geological Survey). Activity coefficients, activity-concentration conventions for the isotopic variants of H2O in the solvent 1H216Ol, and salt effects on isotope fractionation have been included in the derivations. The effects of nonideality are small because of the chemical similarity of different isotopic species of the same molecule or ion. The temperature dependence of the individual isotope equilibrium constants can be calculated from the temperature dependence of the fractionation

  4. Testing actinide fission yield treatment in CINDER90 for use in MCNP6 burnup calculations

    International Nuclear Information System (INIS)

    Most of the development of the MCNPX/6 burnup capability focused on features that were applied to the Boltzman transport or used to prepare coefficients for use in CINDER90, with little change to CINDER90 or the CINDER90 data. Though a scheme exists for best solving the coupled Boltzman and Bateman equations, the most significant approximation is that the employed nuclear data are correct and complete. Thus, the CINDER90 library file contains 60 different actinide fission yields encompassing 36 fissionable actinides (thermal, fast, high energy and spontaneous fission). Fission reaction data exists for more than 60 actinides and as a result, fission yield data must be approximated for actinides that do not possess fission yield information. Several types of approximations are used for estimating fission yields for actinides which do not possess explicit fission yield data. The objective of this study is to test whether or not certain approximations of fission yield selection have any impact on predictability of major actinides and fission products. Further we assess which other fission products, available in MCNP6 Tier 3, result in the largest difference in production. Because the CINDER90 library file is in ASCII format and therefore easily amendable, we assess reasons for choosing, as well as compare actinide and major fission product prediction for the H. B. Robinson benchmark for, three separate fission yield selection methods: (1) the current CINDER90 library file method (Base); (2) the element method (Element); and (3) the isobar method (Isobar). Results show that the three methods tested result in similar prediction of major actinides, Tc-99 and Cs-137; however, certain fission products resulted in significantly different production depending on the method of choice

  5. Multiconfiguration calculations of electronic isotope shift factors in Al I

    CERN Document Server

    Filippin, Livio; Ekman, Jörgen; Fritzsche, Stephan; Godefroid, Michel; Jönsson, Per

    2016-01-01

    The present work reports results from systematic multiconfiguration Dirac-Hartree-Fock calculations of electronic isotope shift factors for a set of transitions between low-lying states in neutral aluminium. These electronic quantities together with observed isotope shifts between different pairs of isotopes provide the changes in mean-square charge radii of the atomic nuclei. Two computational approaches are adopted for the estimation of the mass- and field shift factors. Within these approaches, different models for electron correlation are explored in a systematic way to determine a reliable computational strategy and estimate theoretical uncertainties of the isotope shift factors.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2012-10-30

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

  7. Report of the panel on practical problems in actinide biology

    International Nuclear Information System (INIS)

    Practical problems are classified as the need to make operational decisions, the need for regulatory assessment either of individual facilities or of generic actions, and the overt appearance of radiobiological effects in man or radioactivity in man or the environment. Topics discussed are as follows: simulated reactor accident; long term effects of low doses; effects of repeated exposures to actinides; inhaled uranium mine air contaminants; metabolism and dosimetry; environmental equilibrium models; patterns of alpha dosimetry; internal dose calculations; interfaces between actinide biology and environmental studies; removal of actinides deposited in the body; and research needs related to uranium isotopes

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

    International Nuclear Information System (INIS)

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

  9. Theoretical Calculation of Oxygen Isotopic Fractionation of Tenorite

    Institute of Scientific and Technical Information of China (English)

    方涛

    1997-01-01

    Tenorite is an oxide of cupper which has been well documented on its structure,force constants and spectrum.Based on the isotopic shifts of its spectrum calculated from the force constants of tenorite,its reduced partition function ratios were calculated,from which an oxygen isotopic fractionation curve between tenorite and water was obtained:103lnα=2.51X2-14.87X+6.31(X=103/T)Oxygen isotopic fractionation of tenorite was also calculated with the modified increment method of Zheng(1991),and another equation was obtained:103lnα=2.89X2-13.10X+3.92(X=103/T) Calculated results of the two different models were fitted and possible deviation involved in the calcuation was also discussed.

  10. Calculation of uncertainties of U-Pb isotope data

    Science.gov (United States)

    Ludwig, K. R.

    1980-01-01

    Equations are derived for the estimation of errors and error correlations for various types of U-Pb isotope data, taking into account ion-beam instabilities, run-to-run variability in mass-discrimination, uncertainties in Pb and U concentrations, and uncertainties in initial-Pb and blank-Pb amount and isotopic composition. Equations are also given for the calculation of concordia intercept errors. ?? 1980.

  11. Calculations of the actinide transmutation with HELIOS for fuels of light water reactors; Calculos de la transmutacion de actinidos con HELIOS para combustibles de reactores de agua ligera

    Energy Technology Data Exchange (ETDEWEB)

    Francois L, J.L.; Guzman A, J.R. [UNAM-FI, Laboratorio de Analisis en Ingenieria de Reactores Nucleares, Paseo Cuauhnahuac 8532, Jiutepec, Morelos (Mexico)]. e-mail: jlfl@fi-b.unam.mx

    2006-07-01

    In this work a comparison of the obtained results with the HELIOS code is made and those obtained by other similar codes, used in the international community, respect to the transmutation of smaller actinides. For this the one it is analyzed the international benchmark: 'Calculations of Different Transmutation Concepts', of the Nuclear Energy Agency. In this benchmark two cell types are analyzed: one small corresponding to a PWR standard, and another big one corresponding to a PWR highly moderated. Its are considered two types of burnt of discharge: 33 GWd/tHM and 50 GWd/tHM. The following types of results are approached: the k{sub eff} like a function of the burnt one, the atomic densities of the main isotopes of the actinides, the radioactivities in the moment in that the reactor it is off and in the times of cooling from 7 up to 50000 years, the reactivity by holes and the Doppler reactivity. The results are compared with those obtained by the following institutions: FZK (Germany), JAERI (Japan), ITEP (Russia) and IPPE (Russian Federation). In the case of the eigenvalue, the obtained results with HELIOS showed a discrepancy around 3% {delta}k/k, which was also among other participants. For the isotopic concentrations: {sup 241}Pu, {sup 242} Pu and {sup 242m} Am the results of all the institutions present a discrepancy bigger every time, as the burnt one increases. Regarding the activities, the discrepancy of results is acceptable, except in the case of the {sup 241} Pu. In the case of the Doppler coefficients the discrepancy of results is acceptable, except for the cells with high moderation; in the case of the holes coefficients, the discrepancy of results increases in agreement with the holes fraction increases, being quite high to 95% of holes. In general, the results are consistent and in good agreement with those obtained by all the participants in the benchmark. The results are inside of the established limits by the work group on Plutonium Fuels

  12. Calculation of prompt neutron spectra for curium isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Ohsawa, Takaaki [Kinki Univ., Higashi-Osaka, Osaka (Japan). Atomic Energy Research Inst.

    1997-03-01

    With the aim of checking the existing evaluations contained in JENDL-3.2 and providing new evaluations based on a methodology proposed by the author, a series of calculations of prompt neutron spectra have been undertaken for curium isotopes. Some of the evaluations in JENDL-3.2 was found to be unphysically hard and should be revised. (author)

  13. Production of heavy actinides in incomplete fusion reactions

    Science.gov (United States)

    Antonenko, N. V.; Cherepanov, E. A.; Iljinov, A. S.; Mebel, M. V.

    1994-10-01

    We present preliminary results of calculations by the phenomenological model of the estimated yield of some heavy actinide isotopes. It is assumed that these isotopes are produced as a result of multinucleon transfers followed by neutrons and charged particle emission A.S. Iljinov and E.A. Cherepanov (1980). The yield P(sub Z, N)(E*) of primary excited actinides is found using the model of N.V. Antonenko and R.V. Jolos (1991). Absolute cross-sections for different binary reaction channels are obtained by summing the cross-sections for all subchannels with an appreciable yield according to J. Wilczynski et al. (1980).

  14. Accelerating quantum instanton calculations of the kinetic isotope effects.

    Science.gov (United States)

    Karandashev, Konstantin; Vaníček, Jiří

    2015-11-21

    Path integral implementation of the quantum instanton approximation currently belongs among the most accurate methods for computing quantum rate constants and kinetic isotope effects, but its use has been limited due to the rather high computational cost. Here, we demonstrate that the efficiency of quantum instanton calculations of the kinetic isotope effects can be increased by orders of magnitude by combining two approaches: The convergence to the quantum limit is accelerated by employing high-order path integral factorizations of the Boltzmann operator, while the statistical convergence is improved by implementing virial estimators for relevant quantities. After deriving several new virial estimators for the high-order factorization and evaluating the resulting increase in efficiency, using ⋅Hα + HβHγ → HαHβ + ⋅ Hγ reaction as an example, we apply the proposed method to obtain several kinetic isotope effects on CH4 + ⋅ H ⇌ ⋅ CH3 + H2 forward and backward reactions. PMID:26590524

  15. Microscopic calculations of quadrupole moments in Li and B isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Radhi, R.A.; Dakhil, Z.A.; Manie, N.S. [University of Baghdad, Department of Physics, College of Science, Baghdad (Iraq)

    2014-07-15

    Quadrupole moments and effective charges are calculated for Li (A = 7, 8, 9, 11) and B (A = 8, 10, 11, 12, 13, 14, 15) isotopes based on the shell model with p and large basis spsdpf-shell model spaces. Excitations out of major shell space are taken into account through a microscopic theory which allows particle-hole excitations from the core and model space orbits to all higher orbits with 6ℎω excitations. Effective charges are obtained for the neutron-rich Li and B isotopes which are smaller than the standard values for the stable p- and sd-shell nuclei. Our calculated Q moments agree very well with the experimentally observed trends of the recent experimental data. (orig.)

  16. Microscopic Shell Model Calculations for the Fluorine Isotopes

    Science.gov (United States)

    Barrett, Bruce R.; Dikmen, Erdal; Maris, Pieter; Vary, James P.; Shirokov, Andrey M.

    2015-10-01

    Using a formalism based on the No Core Shell Model (NCSM), we have determined miscroscopically the core and single-particle energies and the effective two-body interactions that are the input to standard shell model (SSM) calculations. The basic idea is to perform a succession of a Okubo-Lee-Suzuki (OLS) transformation, a NCSM calculation, and a second OLS transformation to a further reduced space, such as the sd-shell, which allows the separation of the many-body matrix elements into an ``inert'' core part plus a few valence-nucleons calculation. In the present investigation we use this technique to calculate the properties of the nuclides in the Fluorine isotopic chain, using the JISP16 nucleon-nucleon interaction. The obtained SSM input, along with the results of the SSM calculations for the Fluorine isotopes, will be presented. This work supported in part by TUBITAK-BIDEB, the US DOE, the US NSF, NERSC, and the Russian Ministry of Education and Science.

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

    Science.gov (United States)

    Yücel, Haluk

    2007-11-01

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

  18. A Fast Numerical Method for the Calculation of the Equilibrium Isotopic Composition of a Transmutation System in an Advanced Fuel Cycle

    Directory of Open Access Journals (Sweden)

    F. Álvarez-Velarde

    2012-01-01

    Full Text Available A fast numerical method for the calculation in a zero-dimensional approach of the equilibrium isotopic composition of an iteratively used transmutation system in an advanced fuel cycle, based on the Banach fixed point theorem, is described in this paper. The method divides the fuel cycle in successive stages: fuel fabrication, storage, irradiation inside the transmutation system, cooling, reprocessing, and incorporation of the external material into the new fresh fuel. The change of the fuel isotopic composition, represented by an isotope vector, is described in a matrix formulation. The resulting matrix equations are solved using direct methods with arbitrary precision arithmetic. The method has been successfully applied to a double-strata fuel cycle with light water reactors and accelerator-driven subcritical systems. After comparison to the results of the EVOLCODE 2.0 burn-up code, the observed differences are about a few percents in the mass estimations of the main actinides.

  19. Accelerating quantum instanton calculations of the kinetic isotope effects

    Energy Technology Data Exchange (ETDEWEB)

    Karandashev, Konstantin; Vaníček, Jiří, E-mail: jiri.vanicek@epfl.ch [Laboratory of Theoretical Physical Chemistry, Institut des Sciences et Ingénierie Chimiques, Ecole Polytechnique Fédérale de Lausanne (EPFL), Lausanne CH-1015 (Switzerland)

    2015-11-21

    Path integral implementation of the quantum instanton approximation currently belongs among the most accurate methods for computing quantum rate constants and kinetic isotope effects, but its use has been limited due to the rather high computational cost. Here, we demonstrate that the efficiency of quantum instanton calculations of the kinetic isotope effects can be increased by orders of magnitude by combining two approaches: The convergence to the quantum limit is accelerated by employing high-order path integral factorizations of the Boltzmann operator, while the statistical convergence is improved by implementing virial estimators for relevant quantities. After deriving several new virial estimators for the high-order factorization and evaluating the resulting increase in efficiency, using ⋅H{sub α} + H{sub β}H{sub γ} → H{sub α}H{sub β} + ⋅ H{sub γ} reaction as an example, we apply the proposed method to obtain several kinetic isotope effects on CH{sub 4} + ⋅ H ⇌ ⋅ CH{sub 3} + H{sub 2} forward and backward reactions.

  20. Evaluation of prompt neutron spectra for minor actinide nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Ohsawa, Takaaki [Kinki Univ., Higashi-Osaka, Osaka (Japan). Atomic Energy Research Inst.

    1997-03-01

    Measurement data on fission prompt neutron spectra of minor actinide (MA) is much little, and its accuracy is also unsufficient. Therefore, conventional evaluation value of fission spectra of MA was assumed for its nuclear temperature by using a method of determining from its systemicity owing to assumption of the Maxwell type distribution, but it can be said that this method consider fully to features of MA isotopes. In this paper, some evaluation calculation results are shown by adopting an evaluation method developed by authors and based on modified Madland Nix model and are conducted by concept of physical properties on target nuclei. As a result, by adopting the level density parameter of fission fragments, the inverse process cross section, the fission product yield distribution and the total release energy, effect of inverse process cross section, mass distribution of fission product, calculation results of Cm isotope and systemicity of fission spectra of actinide isotope were investigated. (G.K.)

  1. Calculating isotopic fractionation from atmospheric measurements at various scales

    International Nuclear Information System (INIS)

    In this paper we describe some new approaches for calculating isotopic discrimination from atmospheric measurements of CO2 and 13C. We introduce a framework that is more flexible than the traditional 'Keeling plot' two end-member mixing model, because it allows for the explicit specification of the background values of both CO2 and 13C. This approach is necessary for evaluating time series for which one can be certain that the Keeling plot requirement of stable background is violated. We also discuss a robust method for curve fitting and for estimating uncertainty of the fitting parameters. In addition to accounting for the uncertainty associated with measurements, we also account for the uncertainty associated with the appropriateness of the analytical model to the data. Our analysis suggests that uncertainty in calculated source signatures is more strongly related to the appropriateness of the model to the data than to the analytical precision of CO2 and 13C measurements. Relative to our approach, other approaches tend to underestimate the uncertainty in the fitted parameters. There can be substantial uncertainty in slopes and intercepts (two per mil or more) even if R2 is greater than 0.98. In addition, we note that fitting methods not accounting for uncertainty in both x and y result in systematic biases in the fitted parameters. Finally, we discuss the interpretation of the apparent isotopic source signature when this is a composite of several sources

  2. Calculation and analysis of neutron and radiation characteristics of lead coolants with isotopic tailoring for future nuclear power facilities

    Energy Technology Data Exchange (ETDEWEB)

    Blokhin, A.I.; Ivanov, A.P.; Korobeinikov, V.V.; Lunev, V.P.; Manokhin, V.N.; Khorasanov, G.L. [SSC RF A. I. Leypunsky Institute for Physics and Power Engineering, Obninsk, Kaluga Region (Russian Federation)

    2000-03-01

    A new type of safe fast reactor with lead coolant was proposed in Russia. The use of coolants with low moderating properties is one of the ways to get a hard neutron spectrum and an increase in the burning of Np-237, Am-243 and other miner actinides(MA) fissionable preferentially in the fast reactor. The stable lead isotope, Pb-208, is proposed as the one of such coolants. The neutron inelastic scattering cross-section of Pb-208 is 3.0-3.5 times less than the one of other lead isotopes. Calculation of the MA transmutation rates in the standard BN-type fast reactor with different coolants is performed by Monte-Carlo method using Code MMKFK. Six various models are simulated for the fast reactor blanket with different kinds of fuel and coolant. The fast reactor with natural-lead coolant practically does not differ from the reactor with sodium coolant relative to MA incineration. The use of Pb-208 as a coolant in the fast reactor results in increasing incineration of MA from 18 to 26% in comparison with a usual fast reactor. Calculation of induced radioactivity was performed using the FISPACT-3 inventory code, also. The results include total induced radioactivity and dose rate for initial material composition and selected long-lived radionuclides. The calculations show that the coolant consisting of lead isotope, Pb-206, or Pb-207, can be considered as the low-activation one because it does not practically contain long-lived toxic radionuclides. (M. Suetake)

  3. Bias estimates used in lieu of validation of fission products and minor actinides in MCNP Keff calculations for PWR burnup credit casks

    Energy Technology Data Exchange (ETDEWEB)

    Mueller, Don E. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Marshall, William J. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Wagner, John C. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Bowen, Douglas G. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2015-09-01

    The U.S. Nuclear Regulatory Commission (NRC) Division of Spent Fuel Storage and Transportation recently issued Interim Staff Guidance (ISG) 8, Revision 3. This ISG provides guidance for burnup credit (BUC) analyses supporting transport and storage of PWR pressurized water reactor (PWR) fuel in casks. Revision 3 includes guidance for addressing validation of criticality (keff) calculations crediting the presence of a limited set of fission products and minor actinides (FP&MA). Based on previous work documented in NUREG/CR-7109, recommendation 4 of ISG-8, Rev. 3, includes a recommendation to use 1.5 or 3% of the FP&MA worth to conservatively cover the bias due to the specified FP&MAs. This bias is supplementary to the bias and bias uncertainty resulting from validation of keff calculations for the major actinides in SNF and does not address extension to actinides and fission products beyond those identified herein. The work described in this report involves comparison of FP&MA worths calculated using SCALE and MCNP with ENDF/B-V, -VI, and -VII based nuclear data and supports use of the 1.5% FP&MA worth bias when either SCALE or MCNP codes are used for criticality calculations, provided the other conditions of the recommendation 4 are met. The method used in this report may also be applied to demonstrate the applicability of the 1.5% FP&MA worth bias to other codes using ENDF/B V, VI or VII based nuclear data. The method involves use of the applicant s computational method to generate FP&MA worths for a reference SNF cask model using specified spent fuel compositions. The applicant s FP&MA worths are then compared to reference values provided in this report. The applicants FP&MA worths should not exceed the reference results by more than 1.5% of the reference FP&MA worths.

  4. Actinides in irradiated graphite of RBMK-1500 reactor

    International Nuclear Information System (INIS)

    Highlights: • Activation of actinides in the graphite of the RBMK-1500 reactor was analyzed. • Numerical modeling using SCALE 6.1 and MCNPX was used for actinide calculation. • Measurements of the irradiated graphite sample were used for model validation. • Results are important for further decommissioning process of the RBMK type reactors. - Abstract: The activation of graphite in the nuclear power plants is the problem of high importance related with later graphite reprocessing or disposal. The activation of actinide impurities in graphite due to their toxicity determines a particular long term risk to waste management. In this work the activation of actinides in the graphite constructions of the RBMK-1500 reactor is determined by nuclear spectrometry measurements of the irradiated graphite sample from the Ignalina NPP Unit I and by means of numerical modeling using two independent codes SCALE 6.1 (using TRITON-VI sequence) and MCNPX (v2.7 with CINDER). Both models take into account the 3D RBMK-1500 reactor core fragment with explicit graphite construction including a stack and a sleeve but with a different simplification level concerning surrounding graphite and construction of control roads. The verification of the model has been performed by comparing calculated and measured isotope ratios of actinides. Also good prediction capabilities of the actinide activation in the irradiated graphite have been found for both calculation approaches. The initial U impurity concentration in the graphite model has been adjusted taking into account the experimental results. The specific activities of actinides in the irradiated RBMK-1500 graphite constructions have been obtained and differences between numerical simulation results, different structural parts (sleeve and stack) as well as comparison with previous results (Ancius et al., 2005) have been discussed. The obtained results are important for further decommissioning process of the Ignalina NPP and other RBMK

  5. Actinides in irradiated graphite of RBMK-1500 reactor

    Energy Technology Data Exchange (ETDEWEB)

    Plukienė, R., E-mail: rita@ar.fi.lt; Plukis, A.; Barkauskas, V.; Gudelis, A.; Gvozdaitė, R.; Duškesas, G.; Remeikis, V.

    2014-10-01

    Highlights: • Activation of actinides in the graphite of the RBMK-1500 reactor was analyzed. • Numerical modeling using SCALE 6.1 and MCNPX was used for actinide calculation. • Measurements of the irradiated graphite sample were used for model validation. • Results are important for further decommissioning process of the RBMK type reactors. - Abstract: The activation of graphite in the nuclear power plants is the problem of high importance related with later graphite reprocessing or disposal. The activation of actinide impurities in graphite due to their toxicity determines a particular long term risk to waste management. In this work the activation of actinides in the graphite constructions of the RBMK-1500 reactor is determined by nuclear spectrometry measurements of the irradiated graphite sample from the Ignalina NPP Unit I and by means of numerical modeling using two independent codes SCALE 6.1 (using TRITON-VI sequence) and MCNPX (v2.7 with CINDER). Both models take into account the 3D RBMK-1500 reactor core fragment with explicit graphite construction including a stack and a sleeve but with a different simplification level concerning surrounding graphite and construction of control roads. The verification of the model has been performed by comparing calculated and measured isotope ratios of actinides. Also good prediction capabilities of the actinide activation in the irradiated graphite have been found for both calculation approaches. The initial U impurity concentration in the graphite model has been adjusted taking into account the experimental results. The specific activities of actinides in the irradiated RBMK-1500 graphite constructions have been obtained and differences between numerical simulation results, different structural parts (sleeve and stack) as well as comparison with previous results (Ancius et al., 2005) have been discussed. The obtained results are important for further decommissioning process of the Ignalina NPP and other RBMK

  6. Actinides-1981

    International Nuclear Information System (INIS)

    Abstracts of 134 papers which were presented at the Actinides-1981 conference are presented. Approximately half of these papers deal with electronic structure of the actinides. Others deal with solid state chemistry, nuclear physic, thermodynamic properties, solution chemistry, and applied chemistry

  7. Actinides-1981

    Energy Technology Data Exchange (ETDEWEB)

    1981-09-01

    Abstracts of 134 papers which were presented at the Actinides-1981 conference are presented. Approximately half of these papers deal with electronic structure of the actinides. Others deal with solid state chemistry, nuclear physic, thermodynamic properties, solution chemistry, and applied chemistry.

  8. Calorimetric assay of minor actinides

    Energy Technology Data Exchange (ETDEWEB)

    Rudy, C.; Bracken, D.; Cremers, T.; Foster, L.A.; Ensslin, N.

    1996-12-31

    This paper reviews the principles of calorimetric assay and evaluates its potential application to the minor actinides (U-232-4, Am-241, Am- 243, Cm-245, Np-237). We conclude that calorimetry and high- resolution gamma-ray isotopic analysis can be used for the assay of minor actinides by adapting existing methodologies for Pu/Am-241 mixtures. In some cases, mixtures of special nuclear materials and minor actinides may require the development of new methodologies that involve a combination of destructive and nondestructive assay techniques.

  9. Calorimetric assay of minor actinides

    International Nuclear Information System (INIS)

    This paper reviews the principles of calorimetric assay and evaluates its potential application to the minor actinides (U-232-4, Am-241, Am- 243, Cm-245, Np-237). We conclude that calorimetry and high- resolution gamma-ray isotopic analysis can be used for the assay of minor actinides by adapting existing methodologies for Pu/Am-241 mixtures. In some cases, mixtures of special nuclear materials and minor actinides may require the development of new methodologies that involve a combination of destructive and nondestructive assay techniques

  10. RIS3: A program for relativistic isotope shift calculations

    Science.gov (United States)

    Nazé, C.; Gaidamauskas, E.; Gaigalas, G.; Godefroid, M.; Jönsson, P.

    2013-09-01

    An atomic spectral line is characteristic of the element producing the spectrum. The line also depends on the isotope. The program RIS3 (Relativistic Isotope Shift) calculates the electron density at the origin and the normal and specific mass shift parameters. Combining these electronic quantities with available nuclear data, isotope-dependent energy level shifts are determined. Program summaryProgram title:RIS3 Catalogue identifier: ADEK_v2_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/ADEK_v2_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.html No. of lines in distributed program, including test data, etc.: 5147 No. of bytes in distributed program, including test data, etc.: 32869 Distribution format: tar.gz Programming language: Fortran 77. Computer: HP ProLiant BL465c G7 CTO. Operating system: Centos 5.5, which is a Linux distribution compatible with Red Hat Enterprise Advanced Server. Classification: 2.1. Catalogue identifier of previous version: ADEK_v1_0 Journal reference of previous version: Comput. Phys. Comm. 100 (1997) 81 Subprograms used: Cat Id Title Reference ADZL_v1_1 GRASP2K VERSION 1_1 to be published. Does the new version supersede the previous version?: Yes Nature of problem: Prediction of level and transition isotope shifts in atoms using four-component relativistic wave functions. Solution method: The nuclear motion and volume effects are treated in first order perturbation theory. Taking the zero-order wave function in terms of a configuration state expansion |Ψ>=∑μcμ|Φ(γμPJMj)>, where P, J and MJ are, respectively, the parity and angular quantum numbers, the electron density at the nucleus and the normal and specific mass shift parameters may generally be expressed as ∑cμcν where V is the relevant operator. The matrix elements, in turn, can be expressed as sums over radial integrals multiplied

  11. Calculation of isotope shifts and relativistic shifts in CI, CII, CIII and CIV

    OpenAIRE

    Berengut, J. C.; Flambaum, V. V.; Kozlov, M. G.

    2005-01-01

    We present an accurate ab initio method of calculating isotope shifts and relativistic shifts in atomic spectra. We test the method on neutral carbon and three carbon ions. The relativistic shift of carbon lines may allow them to be included in analyses of quasar absorption spectra that seek to measure possible variations in the fine structure constant, alpha, over the lifetime of the Universe. Carbon isotope shifts can be used to measure isotope abundances in gas clouds: isotope abundances a...

  12. Experimental control of burn-up calculations for high temperature reactor fuel by introduction of a special alpha spectrometric method for the determination of transuranium content. An attempt to establish isotopic correlations

    International Nuclear Information System (INIS)

    In the field of high-temperature-reactor (HTR) fuel investigation there is a great interest in the experimental and calculational determination of heavy metal content under the aspects of burn-up physics and for the prediction of reliable data for reprocessing and waste management. Using a laser-micro-boring preparation method, high resolution alpha-spectroscopy and sophisticated computer decomposition programs we identify qualitatively and quantitatively most of the important actinide isotopes in irradiated HTR-fuel. Additionally we use data, delivered by gamma- and mass-spectroscopy of the same fuel samples. The evaluated results are compared with calculational results from the burn-up code ORIGEN, using a special generated HTR-neutron-cross-section library. In a first step we determine new cross sections for the uranium and plutonium isotopes depending on the irradiation conditions. In a second step we calculate correlations between the heavy metal isotopes and the burn-up or the fission products

  13. Research needs in metabolism and dosimetry of the actinides

    International Nuclear Information System (INIS)

    The following topics are discussed: uranium mine and mill tailings; environmental standards; recommendations of NCRP and ICRP; metabolic models and health effects; life-time exposures to actinides and other alpha emitters; high-specific-activity actinide isotopes versus naturally occurring isotopic mixtures of uranium isotopes; adequacy of the n factor; and metabolism and dosimetry;

  14. Isotope Production Facility Conceptual Thermal-Hydraulic Design Review and Scoping Calculations

    Energy Technology Data Exchange (ETDEWEB)

    Pasamehmetoglu, K.O.; Shelton, J.D.

    1998-08-01

    The thermal-hydraulic design of the target for the Isotope Production Facility (IPF) is reviewed. In support of the technical review, scoping calculations are performed. The results of the review and scoping calculations are presented in this report.

  15. Usage of burnt fuel isotopic compositions from engineering codes in Monte-Carlo code calculations

    Energy Technology Data Exchange (ETDEWEB)

    Aleshin, Sergey S.; Gorodkov, Sergey S.; Shcherenko, Anna I. [Nuclear Research Centre ' ' Kurchatov Institute' ' , Moscow (Russian Federation)

    2015-09-15

    A burn-up calculation of VVER's cores by Monte-Carlo code is complex process and requires large computational costs. This fact makes Monte-Carlo codes usage complicated for project and operating calculations. Previously prepared isotopic compositions are proposed to use for the Monte-Carlo code (MCU) calculations of different states of VVER's core with burnt fuel. Isotopic compositions are proposed to calculate by an approximation method. The approximation method is based on usage of a spectral functionality and reference isotopic compositions, that are calculated by engineering codes (TVS-M, PERMAK-A). The multiplication factors and power distributions of FA and VVER with infinite height are calculated in this work by the Monte-Carlo code MCU using earlier prepared isotopic compositions. The MCU calculation data were compared with the data which were obtained by engineering codes.

  16. Research on the chemical speciation of actinides

    International Nuclear Information System (INIS)

    A demand for the safe and effective management of spent nuclear fuel and radioactive waste generated from nuclear power plant draws increasing attention with the growth of nuclear power industry. The objective of this project is to establish the basis of research on the actinide chemistry by using advanced laser-based highly sensitive spectroscopic systems. Researches on the chemical speciation of actinides are prerequisite for the development of technologies related to nuclear fuel cycles, especially, such as the safe management of high level radioactive wastes and the chemical examination of irradiated nuclear fuels. For supporting these technologies, laser-based spectroscopies have been performed for the chemical speciation of actinide in an aqueous solutions and the quantitative analysis of actinide isotopes in spent nuclear fuels. In this report, results on the following subjects have been summarized. (1) Development of TRLFS technology for chemical speciation of actinides, (2) Development of LIBD technology for measuring solubility of actinides, (3) Chemical speciation of plutonium complexes by using a LWCC system, (4) Development of LIBS technology for the quantitative analysis of actinides, (5) Development of technology for the chemical speciation of actinides by CE, (6) Evaluation on the chemical reactions between actinides and humic substances, (7) Chemical speciation of actinides adsorbed on metal oxides surfaces, (8) Determination of actinide source terms of spent nuclear fuel

  17. Nuclear data needs for the analysis of generation and burn-up of actinide isotopes in nuclear reactors

    International Nuclear Information System (INIS)

    A reliable prediction of the in-pile and out-of-pile physics characteristics of nuclear fuel is one of the objectives of present-day reactor physics. The paper describes the main production paths of important actinides for light water and fast breeder reactors. The accuracy of recent nuclear data is examined by comparisons of theoretical predictions with the results from post-irradiation analysis of nuclear fuel from power reactors, and partly with results obtained in zero-power facilities. A world-wide comparison of nuclear data to be used in large fast power reactor burn-up and long term considerations is presented. The needs for further improvement of nuclear data are discussed. (orig.)

  18. Nuclear data for plutonium and minor actinides

    International Nuclear Information System (INIS)

    Some experience in the usage of different evaluations of neutron constants for plutonium isotopes and minor actinides (MA) is described. That experience was obtained under designing the ABBN-93 group data set which nowadays is used widely for neutronics calculations of different cores with different spectrum and shielding. Under testing of the ABBN-93 data set through different integral and macroscopic experiments the main attention was paid to fuel nuclides and cross sections for MA practically did not verify. That gave an opportunity to change MA nuclear data for more modern without verification of the hole system. This desire appeared with new data libraries JENDL-3.2, JEF-2.2 and ENDF/B-6.2, which was not accessible under designing the ABBN-93. At the same time with the reevaluation of the basic MA nuclear data the ABBN-93 and the library FOND-2 of evaluated nuclear data files, which used as the basis for retrieving of the ABBN-93 data, were added with not very important MA data. So the FOND-2 library nowadays contents nuclear data files for all actinides with the half-life time more 1 day and also those MA which produce long-life actinides

  19. Isotopic selectivity calculations for multi-step photoionization of calcium atoms using narrow-band lasers

    International Nuclear Information System (INIS)

    Isotopic selectivity calculations are carried out for minor calcium isotopes against the major isotope 40Ca for the single-resonance two-step and double-resonance three-step photoionization schemes with narrow-band lasers by using spectral simulation (SS) and modified spectrum (MS) approaches. The results of these calculations are compared with the density matrix (DM) results reported in the literature. It is noted that the values of isotopic selectivity from the SS approach do not agree with those from the DM approach whereas the MS approach, considering hole burning in the Doppler-broadened atomic spectrum, predicts selectivity values which are in good agreement with the DM results. It is argued that one can adequately use the simple MS approach rather than the complex DM approach for the calculation of isotopic selectivity of multi-step photoionization with single-frequency lasers. (author)

  20. Ab Initio Nuclear Structure and Reaction Calculations for Rare Isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Draayer, Jerry P. [Louisiana State Univ., Baton Rouge, LA (United States)

    2014-09-28

    We have developed a novel ab initio symmetry-adapted no-core shell model (SA-NCSM), which has opened the intermediate-mass region for ab initio investigations, thereby providing an opportunity for first-principle symmetry-guided applications to nuclear structure and reactions for nuclear isotopes from the lightest p-shell systems to intermediate-mass nuclei. This includes short-lived proton-rich nuclei on the path of X-ray burst nucleosynthesis and rare neutron-rich isotopes to be produced by the Facility for Rare Isotope Beams (FRIB). We have provided ab initio descriptions of high accuracy for low-lying (including collectivity-driven) states of isotopes of Li, He, Be, C, O, Ne, Mg, Al, and Si, and studied related strong- and weak-interaction driven reactions that are important, in astrophysics, for further understanding stellar evolution, X-ray bursts and triggering of s, p, and rp processes, and in applied physics, for electron and neutrino-nucleus scattering experiments as well as for fusion ignition at the National Ignition Facility (NIF).

  1. Calculation of isotopic mass and energy production by a matrix operator method

    International Nuclear Information System (INIS)

    The Volterra method of the multiplicative integral is used to determine the isotopic density, mass, and energy production in linear systems. The solution method, assumptions, and limitations are discussed. The method allows a rapid accurate calculation of the change in isotopic density, mass, and energy production independent of the magnitude of the time steps, production or decay rates, or flux levels

  2. Isotopic analyses and calculation by use of JENDL-3.2 for high burn-up UO{sub 2} and MOX spent fuels

    Energy Technology Data Exchange (ETDEWEB)

    Sasahara, Akihiro; Matsumura, Tetsuo [Central Research Inst. of Electric Power Industry, Komae, Tokyo (Japan). Komae Research Lab.; Nicolaou, G.; Betti, M.; Walker, C.T.

    1997-03-01

    The post irradiation examinations (PIE) were carried out for high burn-up UO{sub 2} spent fuel (3.8%U235, average burn-up:60GWd/t) and mixed oxide (MOX) spent fuel (5.07%Pu, average burn-up:45GWd/t). The PIE includes, (a) isotopic analysis, (b) electron probe microanalysis (EPMA) in pellet cross section and so on. The results of isotopic analyses and EPMA were compared with ORIGEN2/82 and VIM-BURN calculation results. In VIM-BURN calculation, the nuclear data of actinides were proceeded from new data file, JENDL-3.2. The sensitivities of power history and moderator density to nuclides composition were investigated by VIM-BURN calculation and consequently power history mainly effected on Am241 and Am242m and moderator density effected on fissile nuclides. From EPMA results of U and Pu distribution in pellet, VIM-BURN calculation showed reasonable distribution in pellet cross section. (author)

  3. Sector field inductively coupled plasma mass spectrometry in the elemental and isotopic analysis of lanthanides and actinides

    International Nuclear Information System (INIS)

    Plutonium is one element which is indispensable in identifying the source and for estimating the hazardous effects of rad. The isotopic ratios of plutonium (240Pu/239Pu) and its total concentration in environmental samples were also precisely estimated by high resolution inductively coupled plasma mass spectrometry

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

    Energy Technology Data Exchange (ETDEWEB)

    Wasserburg, G.J.

    1999-02-01

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

  5. Isoscaling and fission modes in the yields of the Kr and Xe isotopes from photofission of actinides

    Science.gov (United States)

    Drnoyan, J.; Zhemenik, V. I.; Mishinsky, G. V.

    2016-05-01

    Yields of Kr and Xe isotopes in photofission of 232Th, 238U, 237Np, 244Pu, 243Am, and 248Cm were tested for isoscaling dependence. Isoscaling for Kr is revealed. For Xe, isoscaling is found to be affected by the STI and STII fission modes governed by the N = 82 and N = 88 neutron shells. The work was performed at the Flerov Laboratory of Nuclear Reactions, Joint Institute for Nuclear Research (JINR).

  6. Enzymatic Kinetic Isotope Effects from First-Principles Path Sampling Calculations.

    Science.gov (United States)

    Varga, Matthew J; Schwartz, Steven D

    2016-04-12

    In this study, we develop and test a method to determine the rate of particle transfer and kinetic isotope effects in enzymatic reactions, specifically yeast alcohol dehydrogenase (YADH), from first-principles. Transition path sampling (TPS) and normal mode centroid dynamics (CMD) are used to simulate these enzymatic reactions without knowledge of their reaction coordinates and with the inclusion of quantum effects, such as zero-point energy and tunneling, on the transferring particle. Though previous studies have used TPS to calculate reaction rate constants in various model and real systems, it has not been applied to a system as large as YADH. The calculated primary H/D kinetic isotope effect agrees with previously reported experimental results, within experimental error. The kinetic isotope effects calculated with this method correspond to the kinetic isotope effect of the transfer event itself. The results reported here show that the kinetic isotope effects calculated from first-principles, purely for barrier passage, can be used to predict experimental kinetic isotope effects in enzymatic systems.

  7. Relativistic calculations of the isotope shifts in highly charged Li-like ions

    CERN Document Server

    Zubova, N A; Shabaev, V M; Tupitsyn, I I; Volotka, A V; Plunien, G; Brandau, C; Stöhlker, Th

    2014-01-01

    Relativistic calculations of the isotope shifts of energy levels in highly charged Li-like ions are performed. The nuclear recoil (mass shift) contributions are calculated by merging the perturbative and large-scale configuration-interaction Dirac-Fock-Sturm (CI-DFS) methods. The nuclear size (field shift) contributions are evaluated by the CI-DFS method including the electron-correlation, Breit, and QED corrections. The nuclear deformation and nuclear polarization corrections to the isotope shifts in Li-like neodymium, thorium, and uranium are also considered. The results of the calculations are compared with the theoretical values obtained with other methods.

  8. 5 f -Shell correlation effects in dioxides of light actinides studied by O 1s x-ray absorption and emission spectroscopies and first-principles calculations

    International Nuclear Information System (INIS)

    Soft x-ray emission and absorption spectroscopic data are reported for the O 1s region of a single crystal of UO2, a polycrystalline NpO2 sample, and a single crystal of PuO2. The experimental data are interpreted using first-principles correlated-electron calculations within the framework of the density functional theory with added Coulomb U interaction (DFT+U). A detailed analysis regarding the origin of different structures in the x-ray emission and x-ray absorption spectra is given and the effect of varying the intra-atomic Coulomb interaction-U for the 5 f electrons is investigated. Our data indicate that O 1s x-ray absorption and emission spectroscopies can, in combination with DFT+U calculations, successfully be used to study 5 f -shell Coulomb correlation effects in dioxides of light actinides. The values for the Coulomb U parameter in these dioxides are derived to be in the range of 4–5 eV. (paper)

  9. Calculation of Energy Spectrum of 12C Isotope by Relativistic Cluster model

    CERN Document Server

    Roshanbakht, Nafiseh

    2016-01-01

    In this paper, we have calculated the energy spectrum of 12C isotope by cluster model. The experimental results show that the "Hoyle" state at 7.65 MeV in 12C isotope has a well-developed three-alpha structure. Hence, we select a three-body system and for interaction between the clusters we use modified Yukawa potential plus coulomb potential. Then, we solve the relativistic Klein-Gordon equation using Nikiforov-Uvarov method to calculate the energy spectrum. Finally, the calculated results are compared with the experimental data. The results show that the isotope 12C should be considered as consisting of three-alpha cluster and the modified Yukawa potential is adaptable for cluster interactions.

  10. Identifying Stereoisomers by ab-initio Calculation of Secondary Isotope Shifts on NMR Chemical Shieldings

    Directory of Open Access Journals (Sweden)

    Karl-Heinz Böhm

    2014-04-01

    Full Text Available We present ab-initio calculations of secondary isotope effects on NMR chemical shieldings. The change of the NMR chemical shift of a certain nucleus that is observed if another nucleus is replaced by a different isotope can be calculated by computing vibrational corrections on the NMR parameters using electronic structure methods. We demonstrate that the accuracy of the computational results is sufficient to even distinguish different conformers. For this purpose, benchmark calculations for fluoro(2-2Hethane in gauche and antiperiplanar conformation are carried out at the HF, MP2 and CCSD(T level of theory using basis sets ranging from double- to quadruple-zeta quality. The methodology is applied to the secondary isotope shifts for 2-fluoronorbornane in order to resolve an ambiguity in the literature on the assignment of endo- and exo-2-fluoronorbornanes with deuterium substituents in endo-3 and exo-3 positions, also yielding insight into mechanistic details of the corresponding synthesis.

  11. Actinides recycling assessment in a thermal reactor

    International Nuclear Information System (INIS)

    Highlights: • Actinides recycling is assessed using BWR fuel assemblies. • Four fuel rods are substituted by minor actinides rods in a UO2 and in a MOX fuel assembly. • Performance of standard fuel assemblies and the ones with the substitution is compared. • Reduction of actinides is measured for the fuel assemblies containing minor actinides rods. • Thermal reactors can be used for actinides recycling. - Abstract: Actinides recycling have the potential to reduce the geological repository burden of the high-level radioactive waste that is produced in a nuclear power reactor. The core of a standard light water reactor is composed only by fuel assemblies and there are no specific positions to allocate any actinides blanket, in this assessment it is proposed to replace several fuel rods by actinides blankets inside some of the reactor core fuel assemblies. In the first part of this study, a single uranium standard fuel assembly is modeled and the amount of actinides generated during irradiation is quantified for use it as reference. Later, in the same fuel assembly four rods containing 6 w/o of minor actinides and using depleted uranium as matrix were replaced and depletion was simulated to obtain the net reduction of minor actinides. Other calculations were performed using MOX fuel lattices instead of uranium standard fuel to find out how much reduction is possible to obtain. Results show that a reduction of minor actinides is possible using thermal reactors and a higher reduction is obtained when the minor actinides are embedded in uranium fuel assemblies instead of MOX fuel assemblies

  12. Ab Initio Calculations of Deuterium Isotope Effects on Chemical Shifts of Salt-Bridged Lysines

    DEFF Research Database (Denmark)

    Ullah, Saif; Ishimoto, Takayoshi; Williamson, Mike P.;

    2011-01-01

    Deuterium isotope effects measure the change in chemical shift on substitution of a proton by deuterium. They have been calculated by direct treatment of the H/D nuclear quantum effect using a multicomponent ab initio molecular orbital method based on a non-Born−Oppenheimer approximation. This me......Deuterium isotope effects measure the change in chemical shift on substitution of a proton by deuterium. They have been calculated by direct treatment of the H/D nuclear quantum effect using a multicomponent ab initio molecular orbital method based on a non-Born−Oppenheimer approximation...

  13. Calculations of the vibrational frequency and isotopic shift of UF6 and U2F6

    Institute of Scientific and Technical Information of China (English)

    Zhang Yun-Guang; Zha Xin-Wei

    2012-01-01

    Molecular structure,vibrational frequency and infrared intensity of UF6 are investigated by using the revised Perdew-Burke-Enzerhof function with the triple-zeta polarized basis set.The calculation results are in good agreement with the experimental values and indicate the existence of a stable U2F6 molecule with a multiple bonded U2 unit.The calculation results also predict that the D3d symmetry of U2F6 is more stable than D3h.The optimized geometries,vibrational frequencies,and infrared intensities are also reported for U2F6 molecules in D3d symmetry.In addition,the isotopic shift of vibrational frequencies of the two molecules under isotopic substitution of uranium atom are also investigated with the same method.The U2F6 molecule is predicted to be better than UF6 for laser uranic isotope separation.

  14. Core correlation effects in multiconfiguration calculations of isotope shifts in Mg I

    CERN Document Server

    Filippin, Livio; Ekman, Jörgen; Jönsson, Per

    2016-01-01

    The present work reports results from systematic multiconfiguration Dirac-Hartree-Fock calculations of isotope shifts for several well-known transitions in neutral magnesium. Relativistic normal and specific mass shift factors as well as the electronic probability density at the origin are calculated. Combining these electronic quantities with available nuclear data, energy and transition level shifts are determined for the $^{26}$Mg$-^{24}$Mg pair of isotopes. Different models for electron correlation are adopted. It is shown that although valence and core-valence models provide accurate values for the isotope shifts, the inclusion of core-core excitations in the computational strategy significantly improves the accuracy of the transition energies and normal mass shift factors.

  15. Criticality analysis of aggregations of actinides from commerical nuclear waste in geological storage

    International Nuclear Information System (INIS)

    An underground nuclear-waste terminal-storage facility for either spent fuel elements or high level waste from a reprocessing plant will contain large amounts of fissionable actinides. Such a facility must be designed to preclude the concentration of these isotopes into a critical mass. Information on the critical masses of the various isotopes present in spent fuel or high level waste is required as part of such a design effort. This study provides this information. The results of this study will be used, in conjunction with geologic transport rates of the actinide compounds, to estimate mass formation probabilities in waste repositories. A computational model was developed as part of the study to perform criticality calculations rapidly and efficiently and to produce tables and plots of actinide concentration in geologic material versus critical mass. The criticality model uses a discrete ordinates approximation to neutron transport theory and treats six energy groups and spherical geometry. Neutron cross sections were obtained from ENDF/B-IV or ENDF/B-V cross section libraries. Critical masses calculated with the computational model were checked against experimental values and against more detailed calculational values and were found to be from 30 percent less to 10 percent greater. Critical mass calculations were made for five waste types, five waste ages, five actinide elements, and four geologic compositions. Minimum critical masses were calculated for over 400 combinations of the above variables. The relative importance for criticality of the various actinides and waste types is presented in terms of the number of possible critical masses per waste container

  16. Calculation and Analysis of B/T (Burning and/or Transmutation Rate of Minor Actinides and Plutonium Performed by Fast B/T Reactor

    Directory of Open Access Journals (Sweden)

    Marsodi

    2006-01-01

    Full Text Available Calculation and analysis of B/T (Burning and/or Transmutation rate of MA (minor actinides and Pu (Plutonium has been performed in fast B/T reactor. The study was based on the assumption that the spectrum shift of neutron flux to higher side of neutron energy had a potential significance for designing the fast B/T reactor and a remarkable effect for increasing the B/T rate of MA and/or Pu. The spectrum shifts of neutron have been performed by change MOX to metallic fuel. Blending fraction of MA and or Pu in B/T fuel and the volume ratio of fuel to coolant in the reactor core were also considered. Here, the performance of fast B/T reactor was evaluated theoretically based on the calculation results of the neutronics and burn-up analysis. In this study, the B/T rate of MA and/or Pu increased by increasing the blending fraction of MA and or Pu and by changing the F/C ratio. According to the results, the total B/T rate, i.e. [B/T rate]MA + [B/T rate]Pu, could be kept nearly constant under the critical condition, if the sum of the MA and Pu inventory in the core is nearly constant. The effect of loading structure was examined for inner or outer loading of concentric geometry and for homogeneous loading. Homogeneous loading of B/T fuel was the good structure for obtaining the higher B/T rate, rather than inner or outer loading

  17. A-dependence of the Spectra of the F Isotopes from ab initio Calculations

    Science.gov (United States)

    Barrett, Bruce R.; Dikmen, Erdal; Maris, Pieter; Vary, James P.; Shirokov, Andrey M.

    2016-03-01

    Using a succession of Okubo-Lee-Suzuki transformations within the No Core Shell Model (NCSM) formalism, we derive an ab initio, non-perturbative procedure for calculating the input for standard shell-model (SSM) calculations within one major shell. We have used this approach for calculating the spectra of the F isotopes from A=18 to A=25, so as to study the A-dependence of the results. In particular, we are interested in seeing if the theoretical input is weak enough, so that a single set of two-body effective interactions can be used for all of the F isotopes investigated. We will present results from SSM calculations based on input obtained with the JISP16 nucleon-nucleon interaction in an initial 4 ℏΩ NCSM basis space. This work supported in part by TUBITAK-BIDEB, the US DOE, the US NSF, NERSC, and the Russian Ministry of Education and Science.

  18. Neutronics design of transmutation of minor actinides in a fusion reactor

    International Nuclear Information System (INIS)

    A concept of transmutation of Minor Actinide (MA) nuclear waste based on the spherical torus (ST) tokamak reactor, FDTR, is put forward. A set of plasma parameter was decided suitable for the ST transmuting nuclear waste blanket. The 2-D neutron transport code TWODANT, 3-D Monte Carlo code MCNP-4B and 1-D burn-up calculation code BISON3.0 and their associated data libraries are used to calculate the transmutation rate, the energy multiplication factor and the tritium breeding rate of the transmutation blanket. The calculation results of the system parameters and the actinide series isotopes for different operation times are also given. The engineering feasibility of the center-post of FDTR is investigated. Relevant results are also given. A preliminary neutronics calculation based on ST transmutation blanket shows that proposed system has high transmuting ability for MA wastes

  19. Calculation of energy spectrum of $^{12}$C isotope with modified Yukawa potential by cluster models

    Indian Academy of Sciences (India)

    MOHAMMAD REZA SHOJAE; NAFISEH ROSHAN BAKHT

    2016-10-01

    In this paper, we have calculated the energy spectrum of 12C isotope in two-cluster models, $3\\alpha$ cluster model and $^8$Be + $\\alpha$ cluster model. We use the modified Yukawa potential for interaction between theclusters and solve the Schrödinger equation using Nikiforov–Uvarov method to calculate the energy spectrum. Then, we increase the accuracy by adding spin-orbit coupling and tensor force and solve them by perturbationtheory in both models. Finally, the calculated results for both models are compared with each other and with the experimental data. The results show that the isotope $^{12}$C should be considered as a three-$\\alpha$ cluster and themodified Yukawa potential is adaptable for cluster interactions.

  20. Results of the isotopic concentrations of VVER calculational burnup credit benchmark no. 2(cb2

    International Nuclear Information System (INIS)

    The characterization of the irradiated fuel materials is becoming more important with the Increasing use of nuclear energy in the world. The purpose of this document is to present the results of the nuclide concentrations calculated Using Calculation VVER Burnup Credit Benchmark No. 2(CB2). The calculations were Performed in The Nuclear Technology Center of Cuba. The CB2 benchmark specification as the second phase of the VVER burnup credit benchmark is Summarized in [1]. The CB2 benchmark focused on VVER burnup credit study proposed on the 97' AER Symposium [2]. It should provide a comparison of the ability of various code systems And data libraries to predict VVER-440 spent fuel isotopes (isotopic concentrations) using Depletion analysis. This phase of the benchmark calculations is still in progress. CB2 should be finished by summer 1999 and evaluated results could be presented on the next AER Symposium. The obtained results are isotopic concentrations of spent fuel as a function of the burnup and Cooling time. The depletion point ORIGEN2[3] code was used for the calculation of the spent Fuel concentration. The depletion analysis was performed using the VVER-440 irradiated fuel assemblies with in-core Irradiation time of 3 years, burnup of the 30000 mwd/TU, and an after discharge cooling Time of 0 and 1 year. This work also comprises the results obtained by other codes[4].

  1. Large-scale shell-model calculations on the spectroscopy of $N<126$ Pb isotopes

    CERN Document Server

    Qi, Chong; Fu, G J

    2016-01-01

    Large-scale shell-model calculations are carried out in the model space including neutron-hole orbitals $2p_{1/2}$, $1f_{5/2}$, $2p_{3/2}$, $0i_{13/2}$, $1f_{7/2}$ and $0h_{9/2}$ to study the structure and electromagnetic properties of neutron deficient Pb isotopes. An optimized effective interaction is used. Good agreement between full shell-model calculations and experimental data is obtained for the spherical states in isotopes $^{194-206}$Pb. The lighter isotopes are calculated with an importance-truncation approach constructed based on the monopole Hamiltonian. The full shell-model results also agree well with our generalized seniority and nucleon-pair-approximation truncation calculations. The deviations between theory and experiment concerning the excitation energies and electromagnetic properties of low-lying $0^+$ and $2^+$ excited states and isomeric states may provide a constraint on our understanding of nuclear deformation and intruder configuration in this region.

  2. Calculations of neutron and proton induced reaction cross sections for actinides in the energy region from 10MeV to 1GeV

    International Nuclear Information System (INIS)

    Several nuclear model codes were applied to calculations of nuclear data in the energy region from 10MeV to 1GeV. At energies up to 100MeV the nuclear theory code GNASH was used for nuclear data calculation for neutrons incident for on 238U, 233-236U, 238-242Pu, 237Np, 232Th, 241-243Am and 242-247Cm. At energies from 100MeV to 1GeV the intranuclear cascade exciton model including the fission process was applied to calculations of protons and neutrons with 233U, 235U, 238U, 232Th, 232Pa, 237Np, 238Np, 239Pu, 241Am, 242Am and 242-248Cm. Determination of parameter systematics was a major effort in the present work that was aimed at improving the predictive capability of the models used. An emphasis was placed upon a simultaneous analysis of data for a variety of reaction channels for the nuclei considered, as well as of data that are available for nearby nuclei or for other incident particles. Comparisons with experimental data available on multiple reaction cross sections, isotope yields, fission cross sections, particle multiplicities, secondary particle spectra, and double differential cross sections indicate that the calculations reproduce the trends, and often the details, of the measurements data. (author) 82 refs

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

    Energy Technology Data Exchange (ETDEWEB)

    Yuecel, Haluk [TAEK-Saraykoey Nuclear Research and Training Center, Atom Cad. No.27, Saray Mah, 06983 Ankara (Turkey)], E-mail: haluk.yucel@taek.gov.tr

    2007-11-15

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

  4. Memory-efficient calculation of the isotopic mass states of a molecule.

    Science.gov (United States)

    Li, Long; Karabacak, N Murat; Cobb, Jennifer S; Wang, Qi; Hong, Pengyu; Agar, Jeffrey N

    2010-09-01

    Our previous work postulated a transition concept among different isotopic mass states (i.e., isotopic species) of a molecule, and developed a hierarchical algorithm for accurately calculating their masses and abundances. A theoretical mass spectrum can be generated by convoluting a peak shape function to these discrete mass states. This approach suffers from limited memory if a level in the hierarchical structure has too many mass states. Here we present a memory efficient divide-and-recursively-combine algorithm to do the calculation, which also improves the truncation method used in the previous hierarchical algorithm. Instead of treating all of the elements in a molecule as a whole, the new algorithm first 'strips' each element one by one. For the mass states of each element, a hierarchical structure is established and kept in the memory. This process reduces the memory usage by orders of magnitude (e.g., for bovine insulin, memory can be reduced from gigabytes to kilobytes). Next, a recursive algorithm is applied to combine mass states of elements to mass states of the whole molecule. The algorithm described above has been implemented as a computer program called Isotope Calculator, which was written in C++. It is freely available under the GNU Lesser General Public License from http://www.cs.brandeis.edu/~hong/software.html or http://people.brandeis.edu/~agar.

  5. Coordination chemistry for new actinide separation processes

    International Nuclear Information System (INIS)

    The amount of wastes and the number of chemical steps can be decreased by replacing the PUREX process extractant (TBP) by, N.N- dialkylamides (RCONR'2). Large amounts of deep underground storable wastes can be stored into sub-surface disposals if the long lived actinide isotopes are removed. Spent nuclear fuels reprocessing including the partitioning of the minor actinides Np, Am, Cm and their transmutation into short half lives fission products is appealing to the public who is not favorable to the deep underground storage of large amounts of long half lived actinide isotopes. In this paper coordination chemistry problems related to improved chemical separations by solvent extraction are presented. 2 tabs.; 4 refs

  6. Spectroscopic calculations of the low-lying structure in exotic Os and W isotopes

    International Nuclear Information System (INIS)

    Structural evolution in neutron-rich Os and W isotopes is investigated in terms of the interacting boson model (IBM) Hamiltonian determined by (constrained) Hartree-Fock-Bogoliubov calculations with the Gogny-D1S energy density functional (EDF). The interaction strengths of the IBM Hamiltonian are produced by mapping the potential energy surface (PES) of the Gogny-EDF with quadrupole degrees of freedom onto the corresponding PES of the IBM system. We examine the prolate-to-oblate shape/phase transition which is predicted to take place in this region as a function of neutron number N within the considered Os and W isotopic chains. The onset of this transition is found to be more rapid compared to the neighboring Pt isotopes. The calculations also allow the prediction of spectroscopic variables (excited state energies and reduced transition probabilities) which are presented for the neutron-rich 192,194,196W nuclei, for which there is only very limited experimental data available to date.

  7. Mass-Independent Fractionation of Oxygen Isotope in Earth Wind: First Principle Calculations for Photodissociation

    Science.gov (United States)

    Yamada, A.; Nanbu, S.; Kasai, Y.; Ozima, M.

    2009-12-01

    Mass-independently fractionated oxygen isotope were reported on metal particles extracted from Apollo lunar soils [1, 2], but these origins are still unknown. Since the substantial fraction of Earth-escaping O+ flux (Earth Wind, EW hereafter), comparable to the amount of the anomalous oxygen implanted on the metal particles, could reach the lunar surface [3], Ozima et al. [4] suggested that EW may be responsible to the anomalous oxygen. The purpose is to test this EW hypothesiss, we study oxygen isotopic ratios of O+ at the upper atmosphere. From quantum chemical calculations of photo-dissociation of O2, we show the results in mass-independent isotopic fractionation of oxygen, thereby in conformity with the EW hypothesis. First principles reaction dynamics simulations were performed to compute the photolysis rate for the B3Σu- ← X3Σg- electronic transition, for Schumann-Runge band. With the assumption of the Born-Oppenheimer approximation, we performed the wave-packet dynamics for the nuclei-motion in the potential energy curves determined by the first step calculation. Quantum chemical program package [5] was used for the first step calculation, and the quantum dynamics was carried out by our own program package. Assuming the quantum yield of the corresponding photolysis is unity, the photo-absorption cross section can be correlated with the photolysis rate. Therefore, following the time dependent approach, the autocorrelation function (A(t) = ) was numerically computed by the second step calculation. Finally, the theoretical spectrum as a function of wavelength of excitation light was estimated by the Fourier transform of the autocorrelation function A(t) [6]. Calculated absorption cross sections for C16O showed similar wavelength dependence with experiment [7], although the absolute magnitude was yet to be calibrated for a quantitative comparison. Assuming Boltzmann distribution at 1200 K, we estimated enrichment factors defined as σι(λ)/σ16(λ) - 1 (i

  8. Calculation of isotopic mass and energy production by a matrix operator method. [Volterra method of the multiplicative integral

    Energy Technology Data Exchange (ETDEWEB)

    Lee, C.E.

    1976-08-01

    The Volterra method of the multiplicative integral is used to determine the isotopic density, mass, and energy production in linear systems. The solution method, assumptions, and limitations are discussed. The method allows a rapid accurate calculation of the change in isotopic density, mass, and energy production independent of the magnitude of the time steps, production or decay rates, or flux levels.

  9. Comparisons of Neutron Cross Sections and Isotopic Composition Calculations for Fission-Product Evaluations

    Science.gov (United States)

    Kim, Do Heon; Gil, Choong-Sup; Chang, Jonghwa; Lee, Yong-Deok

    2005-05-01

    The neutron absorption cross sections for 18 fission products evaluated within the framework of the KAERI (Korea Atomic Energy Research Institute)-BNL (Brookhaven National Laboratory) international collaboration have been compared with ENDF/B-VI.7. Also, the influence of the new evaluations on the isotopic composition calculations of the fission products has been estimated through the OECD/NEA burnup credit criticality benchmarks (Phase 1B) and the LWR/Pu recycling benchmarks. These calculations were performed by WIMSD-5B with the 69-group libraries prepared from three evaluated nuclear data libraries: ENDF/B-VI.7, ENDF/B-VI.8 including the new evaluations in the resonance region covering the thermal region, and the expected ENDF/B-VII including those in the upper resonance region up to 20 MeV. For Xe-131, the composition calculated with ENDF/B-VI.8 shows a maximum difference of 5.02% compared to ENDF/B-VI.7. However, the isotopic compositions of all the fission products calculated with the expected ENDF/B-VII show no differences when compared to ENDF/B-VI.7 for the thermal reactor benchmark cases.

  10. TMI-2 decay power: LASL fission-product and actinide decay power calculations for the President's Commission at Three Mile Island

    Energy Technology Data Exchange (ETDEWEB)

    England, T.R.; Wilson, W.B.

    1979-10-01

    Fission-product and actinide decay heating, gas content, curies, and detailed contributions of the most important nuclide contributors were supplied in a series of letters following requests from the Presidential Commission on the Accident at Three Mile Island. In addition, similar data assuming different irradiation (power) histories were requested for purposes of comparison. This report consolidates the tabular and graphical data supplied and explains its basis.

  11. The lanthanides and actinides

    International Nuclear Information System (INIS)

    This paper relates the chemical properties of the actinides to their position in the Mendeleev periodic system. The changes in the oxidation states of the actinides with increasing atomic number are similar to those of the 3d elements. Monovalent and divalent actinides are very similar to alkaline and alkaline earth elements; in the 3+ and 4+ oxidation states they resemble d elements in the respective oxidation states. However, in their highest oxidation states the actinides display their individual properties with only a slight resemblance to d elements. Finally, there is a profound similarity between the second half of the actinides and the first half of the lanthanides

  12. Calculation and preliminary analysis of group cross sections for gadolinium and its isotopes

    International Nuclear Information System (INIS)

    Evaluated nuclear data files ENDL 78 and ENDF/B-IV and the cross section generation code FEDGROUP-R were used to produce averaged group cross sections for group systems BNAB and THSIG for gadolinium and its isotopes. Different sets of group cross sections for gadolinium (due to different evaluated data files or different processing codes) were compared and significant differences analyzed. The group capture cross sections for the isotopes of gadolinium were compared with published data. The group cross sections data sets prepared are analyzed as to what extent they can meet the requirements of cell calculations for gadolinium-loaded fuel. Some group cross section tables and cross section plots are presented. (author)

  13. Ab initio calculations of the Fe(II) and Fe(III) isotopic effects in citrates, nicotianamine, and phytosiderophore, and new Fe isotopic measurements in higher plants

    Science.gov (United States)

    Moynier, Frédéric; Fujii, Toshiyuki; Wang, Kun; Foriel, Julien

    2013-05-01

    Iron is one of the most abundant transition metal in higher plants and variations in its isotopic compositions can be used to trace its utilization. In order to better understand the effect of plant-induced isotopic fractionation on the global Fe cycling, we have estimated by quantum chemical calculations the magnitude of the isotopic fractionation between different Fe species relevant to the transport and storage of Fe in higher plants: Fe(II)-citrate, Fe(III)-citrate, Fe(II)-nicotianamine, and Fe(III)-phytosiderophore. The ab initio calculations show firstly, that Fe(II)-nicotianamine is ˜3‰ (56Fe/54Fe) isotopically lighter than Fe(III)-phytosiderophore; secondly, even in the absence of redox changes of Fe, change in the speciation alone can create up to ˜1.5‰ isotopic fractionation. For example, Fe(III)-phytosiderophore is up to 1.5‰ heavier than Fe(III)-citrate2 and Fe(II)-nicotianamine is up to 1‰ heavier than Fe(II)-citrate. In addition, in order to better understand the Fe isotopic fractionation between different plant components, we have analyzed the iron isotopic composition of different organs (roots, seeds, germinated seeds, leaves and stems) from six species of higher plants: the dicot lentil (Lens culinaris), and the graminaceous monocots Virginia wild rye (Elymus virginicus), Johnsongrass (Sorghum halepense), Kentucky bluegrass (Poa pratensis), river oat (Uniola latifolia), and Indian goosegrass (Eleusine indica). The calculations may explain that the roots of strategy-II plants (Fe(III)-phytosiderophore) are isotopically heavier (by about 1‰ for the δ56Fe) than the upper parts of the plants (Fe transported as Fe(III)-citrate in the xylem or Fe(II)-nicotianamine in the phloem). In addition, we suggest that the isotopic variations observed between younger and older leaves could be explained by mixing of Fe received from the xylem and the phloem.

  14. Fine-grid calculations for stellar electron and positron capture rates on Fe isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Nabi, Jameel-Un, E-mail: jameel@giki.edu.pk [Ghulam Ishaq Khan Institute of Engineering Sciences and Technology, Faculty of Engineering Sciences (Pakistan); Tawfik, Abdel Nasser, E-mail: a.tawfik@eng.mti.edu.eg [MTI University, Egyptian Center for Theoretical Physics (ECTP) (Egypt)

    2013-03-15

    The acquisition of precise and reliable nuclear data is a prerequisite to success for stellar evolution and nucleosynthesis studies. Core-collapse simulators find it challenging to generate an explosion from the collapse of the core of massive stars. It is believed that a better understanding of the microphysics of core-collapse can lead to successful results. The weak interaction processes are able to trigger the collapse and control the lepton-to-baryon ratio (Y{sub e}) of the corematerial. It is suggested that the temporal variation of Y{sub e} within the core of a massive star has a pivotal role to play in the stellar evolution and a fine-tuning of this parameter at various stages of presupernova evolution is the key to generate an explosion. During the presupernova evolution of massive stars, isotopes of iron, mainly {sup 54-56}Fe, are considered to be key players in controlling Y{sub e} ratio via electron capture on these nuclides. Recently an improved microscopic calculation of weak-interaction-mediated rates for iron isotopes was introduced using the proton-neutron quasiparticle random-phase-approximation (pn-QRPA) theory. The pn-QRPA theory allows a microscopic state-by-state calculation of stellar capture rates which greatly increases the reliability of calculated rates. The results were suggestive of some fine-tuning of the Y{sub e} ratio during various phases of stellar evolution. Here we present for the first time the fine-grid calculation of the electron and positron capture rates on {sup 54-56}Fe. The sensitivity of the pn-QRPA calculated capture rates to the deformation parameter is also studied in this work. Core-collapse simulators may find this calculation suitable for interpolation purposes and for necessary incorporation in the stellar evolution codes.

  15. Isotope shifts in beryllium-, boron-, carbon-, and nitrogen-like ions from relativistic configuration interaction calculations

    Energy Technology Data Exchange (ETDEWEB)

    Nazé, C.; Verdebout, S. [Service de Chimie Quantique et Photophysique, CP160/09, Université Libre de Bruxelles, Avenue F.D. Roosevelt 50, B 1050 Brussels (Belgium); Rynkun, P.; Gaigalas, G. [Vilnius University, Institute of Theoretical Physics and Astronomy, LT-01108 Vilnius (Lithuania); Godefroid, M., E-mail: mrgodef@ulb.ac.be [Service de Chimie Quantique et Photophysique, CP160/09, Université Libre de Bruxelles, Avenue F.D. Roosevelt 50, B 1050 Brussels (Belgium); Jönsson, P. [Group for Materials Science and Applied Mathematics, Malmö University, 205-06 Malmö (Sweden)

    2014-09-15

    Energy levels, normal and specific mass shift parameters as well as electronic densities at the nucleus are reported for numerous states along the beryllium, boron, carbon, and nitrogen isoelectronic sequences. Combined with nuclear data, these electronic parameters can be used to determine values of level and transition isotope shifts. The calculation of the electronic parameters is done using first-order perturbation theory with relativistic configuration interaction wavefunctions that account for valence, core–valence, and core–core correlation effects as zero-order functions. Results are compared with experimental and other theoretical values, when available.

  16. Results of the isotopic concentrations of VVER calculational burnup credit benchmark No. 2(CB2)

    International Nuclear Information System (INIS)

    Results of the nuclide concentrations are presented of VVER Burnup Credit Benchmark No. 2(CB2) that were performed in The Nuclear Technology Center of Cuba with available codes and libraries. The CB2 benchmark specification as the second phase of the VVER burnup credit benchmark is summarized. The CB2 benchmark focused on VVER burnup credit study proposed on the 97' AER Symposium. The obtained results are isotopic concentrations of spent fuel as a function of the burnup and cooling time. The depletion point 'ORIGEN2' code and other codes were used for the calculation of the spent fuel concentration. (author)

  17. Spectroscopic calculations of the low-lying structure in exotic Os and W isotopes

    OpenAIRE

    Nomura, K.; T. Otsuka; Rodríguez-Guzmán, R.; Robledo, L M; Sarriguren, Pedro; Regan, P.H.; Stevenson, P. D.; Podolyák, Zs.

    2011-01-01

    Structural evolution in neutron-rich Os and W isotopes is investigated in terms of the interacting boson model (IBM) Hamiltonian determined by (constrained) Hartree-Fock-Bogoliubov calculations with the Gogny-D1S energy density functional (EDF). The interaction strengths of the IBM Hamiltonian are produced by mapping the potential energy surface (PES) of the Gogny-EDF with quadrupole degrees of freedom onto the corresponding PES of the IBM system. We examine the prolate-to-oblate shape/phase ...

  18. A refined method for calculating paleotemperatures from linear correlations in bamboo coral carbon and oxygen isotopes

    Science.gov (United States)

    Saenger, Casey; Watkins, James M.

    2016-06-01

    Bamboo corals represent an emerging paleoclimate archive with the potential to record variability at intermediate depths throughout much of the global ocean. Realizing this potential has been complicated by biologically mediated vital effects, which are evident in linear correlations of skeletal carbon (δ13C) and oxygen (δ18O) isotope composition. Previous efforts to develop a bamboo coral δ18O paleothermometer by accounting for such vital effects have not been completely successful as they still rely on empirical calibrations that are offset from the temperature dependence of abiogenic experiments. Here we describe an approach that better corrects for bamboo coral vital effects and allows paleotemperatures to be calculated directly from the abiogenic temperature dependence. The success of the method lies in calculating apparent equilibrium carbon and oxygen isotope fractionation at the temperature, pH, and growth rate of each coral, as well as in the use of model II regressions. Rigorous propagation of uncertainty suggests typical errors of ±2-3°C, but in select cases errors as low as ±0.65°C can be achieved for densely sampled and strongly correlated data sets. This lower limit approaches the value attributed to uncertainty in pH and growth rate estimates alone, as predicted by a series of pseudoproxy experiments. The incorporation of isotopically light metabolic CO2 appears to be negligible in most Pacific corals, but may be significant in Atlantic specimens, potentially requiring an additional correction. The success of the method therefore hinges on how well complex environmental systems and biomineralization strategies are constrained, with the most reliable temperatures occurring when calcifying fluid pH, growth rate, and incorporation of metabolic carbon into skeletal calcite are constrained using multiple geochemical proxies.

  19. Large scale shell model calculations for even-even $^{62-66}$Fe isotopes

    CERN Document Server

    Srivastava, P C

    2009-01-01

    The recently measured experimental data of Legnaro National Laboratories on neutron rich even isotopes of $^{62-66}$Fe with A=62,64,66 have been interpreted in the framework of large scale shell model. Calculations have been performed with a newly derived effective interaction GXPF1A in full $\\it{fp}$ space without truncation. The experimental data is very well explained for $^{62}$Fe, satisfactorily reproduced for $^{64}$Fe and poorly fitted for $^{66}$Fe. The increasing collectivity reflected in experimental data when approaching N=40 is not reproduced in calculated values. This indicates that whereas the considered valence space is adequate for $^{62}$Fe, inclusion of higher orbits from $\\it{sdg}$ shell is required for describing $^{66}$Fe.

  20. Performance comparison of metallic, actinide burning fuel in lead-bismuth and sodium cooled fast reactors

    Energy Technology Data Exchange (ETDEWEB)

    Weaver, K.D.; Herring, J.S.; Macdonald, P.E. [Idaho National Engineering and Environment Lab., Advanced Nuclear Energy, Idaho (United States)

    2001-07-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2001-04-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Laurinat, James E.; Askew, Neal M.; Hensel, Steve J.

    2013-03-21

    Packaging options are evaluated for compliance with safety requirements for shipment of mixed actinide oxides packaged in a 9975 Primary Containment Vessel (PCV). Radiolytic gas generation rates, PCV internal gas pressures, and shipping windows (times to reach unacceptable gas compositions or pressures after closure of the PCV) are calculated for shipment of a 9975 PCV containing a plastic bottle filled with plutonium and uranium oxides with a selected isotopic composition. G-values for radiolytic hydrogen generation from adsorbed moisture are estimated from the results of gas generation tests for plutonium oxide and uranium oxide doped with curium-244. The radiolytic generation of hydrogen from the plastic bottle is calculated using a geometric model for alpha particle deposition in the bottle wall. The temperature of the PCV during shipment is estimated from the results of finite element heat transfer analyses.

  3. Minior Actinide Doppler Coefficient Measurement Assessment

    Energy Technology Data Exchange (ETDEWEB)

    Nolan E. Hertel; Dwayne Blaylock

    2008-04-10

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

  4. Results of calculations of isotope-selective laser excitation of long-lived levels of zinc atoms

    International Nuclear Information System (INIS)

    On the basis of mathematical model of laser isotope-selective excitation of long-lived atoms numerical calculations were conducted for zinc atoms. These atoms are characterized by small shifts between lines of different isotopes (600700 MHz), while the method are particularly effective in the case of big shifts. In spite of that due to relative simplicity of the method in comparison with AVLIS it is used for zinc isotope separation. The method is effective in the case of excitation of atom long-lived level. In this case in the interval between radiation impulses at the account of chemical reaction with some molecules atoms in this state could be removed. Calculation results show efficiency of burning out of those isotopes, which lines are nearest to radiation line

  5. Actinides transmutation - a comparison of results for PWR benchmark

    Energy Technology Data Exchange (ETDEWEB)

    Claro, Luiz H. [Instituto de Estudos Avancados (IEAv/CTA), Sao Jose dos Campos, SP (Brazil)], e-mail: luizhenu@ieav.cta.br

    2009-07-01

    The physical aspects involved in the Partitioning and Transmutation (P and T) of minor actinides (MA) and fission products (FP) generated by reactors PWR are of great interest in the nuclear industry. Besides these the reduction in the storage of radioactive wastes are related with the acceptability of the nuclear electric power. From the several concepts for partitioning and transmutation suggested in literature, one of them involves PWR reactors to burn the fuel containing plutonium and minor actinides reprocessed of UO{sub 2} used in previous stages. In this work are presented the results of the calculations of a benchmark in P and T carried with WIMSD5B program using its new cross sections library generated from the ENDF-B-VII and the comparison with the results published in literature by other calculations. For comparison, was used the benchmark transmutation concept based in a typical PWR cell and the analyzed results were the k{infinity} and the atomic density of the isotopes Np-239, Pu-241, Pu-242 and Am-242m, as function of burnup considering discharge of 50 GWd/tHM. (author)

  6. Rapid determination of actinides in asphalt samples

    International Nuclear Information System (INIS)

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

  7. Scission neutrons for U, Pu, Cm, and Cf isotopes: Relative multiplicities calculated in the sudden limit

    Science.gov (United States)

    Capote, R.; Carjan, N.; Chiba, S.

    2016-02-01

    The multiplicities of scission neutrons νs c are calculated for series of U, Pu, Cm, and Cf isotopes assuming a sudden transition between two different nuclear configurations (αi→αf ): one just before the neck rupture and one immediately after the disappearance of the neck. This calculation requires only the knowledge of the corresponding two sets of neutron eigenstates. The nuclear shapes around the scission point are described in terms of Cassinian ovals with only two parameters: α (that positions the shape with respect to the zero-neck shape) and α1 (that defines the mass asymmetry). Based on these shapes, a neutron mean field of the Woods-Saxon type is constructed using two prescriptions to calculate the distance to the nuclear surface. The accent in the present work is put on the dependence of νs c on the neutron number Nf of the fissioning nucleus and on the mass asymmetry AL/AH of the primary fission fragments. The relative dependence of these multiplicities, averaged over the mass yields, , are finally compared with existing experimental data on prompt fission neutrons .

  8. Large-scale shell model calculations for structure of Ni and Cu isotopes

    Science.gov (United States)

    Tsunoda, Yusuke; Otsuka, Takaharu; Shimizu, Noritaka; Honma, Michio; Utsuno, Yutaka

    2014-09-01

    We study nuclear structure of Ni and Cu isotopes, especially neutron-rich ones in the N ~ 40 region by Monte Carlo shell model (MCSM) calculations in pfg9d5 model space (0f7 / 2 , 1p3 / 2 , 0f5 / 2 , 1p1 / 2 , 0g9 / 2 , 1d5 / 2). Effects of excitation across N = 40 and other gaps are important to describe properties such as deformation, and we include this effects by using the pfg9d5 model space. We can calculate in this large model space without any truncation, as an advantage of MCSM. In the MCSM, a wave function is represented as a linear combination of angular-momentum- and parity-projected deformed Slater determinants. We can study intrinsic shapes of nuclei by using quadrupole deformations of MCSM basis states before projection. In doubly-magic 68Ni, there are oblate and prolate deformed bands as well as the spherical ground state from the calculation. Such shape coexistence can be explained by introducing the mechanism called Type II shell evolution, driven by changes of configurations within the same nucleus mainly due to the tensor force.

  9. An emergency bioassay method for actinides in urine.

    Science.gov (United States)

    Dai, Xiongxin; Kramer-Tremblay, Sheila

    2011-08-01

    A rapid bioassay method has been developed for the sequential measurements of actinides in human urine samples. The method involves actinide separation from a urine matrix by co-precipitation with hydrous titanium oxide (HTiO), followed by anion exchange and extraction chromatography column purification, and final counting by alpha spectrometry after cerium fluoride micro-precipitation. The minimal detectable activities for the method were determined to be 20 mBq L(-1) or less for plutonium, uranium, americium and curium isotopes, with an 8-h sample turn-around time. Spike tests showed that this method would meet the requirements for actinide bioassay following a radiation emergency. PMID:21709501

  10. Theoretical calculation of oxygen equilibrium isotope fractionation factors involving various NOy molecules, radOH, and H2O and its implications for isotope variations in atmospheric nitrate

    Science.gov (United States)

    Walters, Wendell W.; Michalski, Greg

    2016-10-01

    The oxygen stable isotope composition (δ18O) of nitrogen oxides [NOx = nitric oxide (NO) + nitrogen dioxide (NO2)] and their oxidation products (NOy = NOx + nitric acid (HNO3) + particulate nitrate (p-NO3-) + nitrate radical (NO3) + dinitrogen pentoxide (N2O5) + nitrous acid (HONO) + …) have been shown to be a useful tool for inferring the proportion of NOx that is oxidized by ozone (O3). However, isotopic fractionation processes may have an influence on δ18O of various NOy molecules and other atmospheric O-bearing molecules pertinent to NOx oxidation chemistry. Here we have evaluated the impacts of O isotopic exchange involving NOy molecules, the hydroxyl radical (radOH), and water (H2O) using reduced partition function ratios (xβ) calculated by hybrid density functional theory. Assuming atmospheric isotopic equilibrium is achieved between NO and NO2 during the daytime, and NO2, NO3, and N2O5 during the nighttime, δ18O-δ15N compositions were predicted for the major atmospheric nitrate formation pathways using our calculated exchange fractionation factors and isotopic mass-balance. Our equilibrium model predicts that various atmospheric nitrate formation pathways, including NO2 + radOH → HNO3, N2O5 + H2O + surface → 2HNO3, and NO3 + R → HNO3 + Rrad will yield distinctive δ18O-δ15N compositions. Our calculated δ18O-δ15N compositions match well with previous atmospheric nitrate measurements, and will potentially help better understand the role oxidation chemistry plays on the N and O isotopic composition of atmospheric nitrate.

  11. Ground-State Properties of C, O, and Ne Isotopes in Hartree-Fock-Bogoliubov Calculation with Gogny Interaction

    Institute of Scientific and Technical Information of China (English)

    GUO Lu; ZHAO En-Guang; SAKATA Fumihiko

    2003-01-01

    Ground-state.properties of C, O, and Ne isotopes are described in the framework of Hartree-FockBogoliubov theory with density-dependent finite-range Gogny interaction D1S. We include all the contributions to the Hartree-Fock and pairing field arising from Gogny and Coulomb interaction as well as the center of mass correction in the numerical calculations. These ground-state properties of C, O, and Ne isotopes are compared with available experimental results, Hartree-Fock plus BCS, shell model and relativistic Hartree-Bogoliubov calculations. The agreement between experiments and our theoretical results is pretty well. The predicted drip-line is dependent strongly on the model and effective interaction due to their sensitivity to various theoretical details. The calculations predict no evidence for halo structure predicted for C, O, and Ne isotopes in a previous RHB study.

  12. Comparison of actinides and fission products recycling scheme with the normal plutonium recycling scheme in fast reactors

    Directory of Open Access Journals (Sweden)

    Salahuddin Asif

    2013-01-01

    Full Text Available Multiple recycling of actinides and non-volatile fission products in fast reactors through the dry re-fabrication/reprocessing atomics international reduction oxidation process has been studied as a possible way to reduce the long-term potential hazard of nuclear waste compared to that resulting from reprocessing in a wet PUREX process. Calculations have been made to compare the actinides and fission products recycling scheme with the normal plutonium recycling scheme in a fast reactor. For this purpose, the Karlsruhe version of isotope generation and depletion code, KORIGEN, has been modified accordingly. An entirely novel fission product yields library for fast reactors has been created which has replaced the old KORIGEN fission products library. For the purposes of this study, the standard 26 groups data set, KFKINR, developed at Forschungszentrum Karlsruhe, Germany, has been extended by the addition of the cross-sections of 13 important actinides and 68 most important fission products. It has been confirmed that these 68 fission products constitute about 95% of the total fission products yield and about 99.5% of the total absorption due to fission products in fast reactors. The amount of fissile material required to guarantee the criticality of the reactor during recycling schemes has also been investigated. Cumulative high active waste per ton of initial heavy metal is also calculated. Results show that the recycling of actinides and fission products in fast reactors through the atomics international reduction oxidation process results in a reduction of the potential hazard of radioactive waste.

  13. Influence of bacteria on lanthanide and actinide transfer from specific soil components (humus, soil minerals and vitrified municipal solid waste incinerator bottom ash) to corn plants: Sr-Nd isotope evidence

    International Nuclear Information System (INIS)

    Experiments have been performed to test the stability of vitrified municipal solid waste (MSW) incinerator bottom ash under the presence of bacteria (Pseudomonas aeruginosa) and plants (corn). The substratum used for the plant growth was a humus-rich soil mixed with vitrified waste. For the first time, information on the stability of waste glasses in the presence of bacteria and plants is given. Results show that inoculated plant samples contained always about two times higher lanthanide and actinide element concentrations. Bacteria support the element transfer since plants growing in inoculated environment developed a smaller root system but have higher trace element concentrations. Compared with the substratum, plants are light rare earth element (LREE) enriched. The vitrified bottom ash has to some extent been corroded by bacteria and plant activities as indicated by the presence of Nd (REE) and Sr from the vitrified waste in the plants. 87Sr/86Sr and 143Nd/144Nd isotope ratios of plants and soil components allow the identification of the corroded soil components and confirm that bacteria accelerate the assimilation of elements from the vitrified bottom ash. These findings are of importance for landfill disposal scenarios, and similar experiments should be performed in order to better constrain the processes of microbially mediated alteration of the MSW glasses in the biosphere

  14. Influence of bacteria on lanthanide and actinide transfer from specific soil components (humus, soil minerals and vitrified municipal solid waste incinerator bottom ash) to corn plants: Sr-Nd isotope evidence

    Energy Technology Data Exchange (ETDEWEB)

    Aouad, Georges [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France); Stille, Peter [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France)]. E-mail: pstille@illite.u-strasbg.fr; Crovisier, Jean-Louis [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France); Geoffroy, Valerie A. [UMR 7156 Universite Louis-Pasteur/CNRS, Genetique Moleculaire, Genomique Microbiologie, Departement Micro-organisme, Genomes, Environnement, 28 rue Goethe, 67083 Strasbourg Cedex (France); Meyer, Jean-Marie [UMR 7156 Universite Louis-Pasteur/CNRS, Genetique Moleculaire, Genomique Microbiologie, Departement Micro-organisme, Genomes, Environnement, 28 rue Goethe, 67083 Strasbourg Cedex (France); Lahd-Geagea, Majdi [Ecole et Observatoire des Sciences de la Terre, Centre de Geochimie de la Surface/CNRS UMR 7517, 1 rue Blessig, 67084 Strasbourg Cedex (France)

    2006-11-01

    Experiments have been performed to test the stability of vitrified municipal solid waste (MSW) incinerator bottom ash under the presence of bacteria (Pseudomonas aeruginosa) and plants (corn). The substratum used for the plant growth was a humus-rich soil mixed with vitrified waste. For the first time, information on the stability of waste glasses in the presence of bacteria and plants is given. Results show that inoculated plant samples contained always about two times higher lanthanide and actinide element concentrations. Bacteria support the element transfer since plants growing in inoculated environment developed a smaller root system but have higher trace element concentrations. Compared with the substratum, plants are light rare earth element (LREE) enriched. The vitrified bottom ash has to some extent been corroded by bacteria and plant activities as indicated by the presence of Nd (REE) and Sr from the vitrified waste in the plants. {sup 87}Sr/{sup 86}Sr and {sup 143}Nd/{sup 144}Nd isotope ratios of plants and soil components allow the identification of the corroded soil components and confirm that bacteria accelerate the assimilation of elements from the vitrified bottom ash. These findings are of importance for landfill disposal scenarios, and similar experiments should be performed in order to better constrain the processes of microbially mediated alteration of the MSW glasses in the biosphere.

  15. Feasibility studies of actinide recycle in LMFBRs as a waste management alternative

    International Nuclear Information System (INIS)

    A strategy of actinide burnup in LMFBRs is being investigated as a waste management alternative to long term storage of high level nuclear waste. This strategy is being evaluated because many of the actinides in the waste from spent-fuel reprocessing have half-lives of thousands of years and an alternative to geological storage may be desired. From a radiological viewpoint, the actinides and their daughters dominate the waste hazard for decay times beyond about 400 years. Actinide burnup in LMFBRs may be an attractive alternative to geological storage because the actinides can be effectively transmuted to fission products which have significantly shorter half-lives. Actinide burnup in LMFBRs rather than LWRs is preferred because the ratio of fission reaction rate to capture reaction rate for the actinides is higher in an LMFBR, and an LMFBR is not so sensitive to the addition of the actinide isotopes. An actinide target assembly recycle scheme is evaluated to determine the effects of the actinides on the LMFBR performance, including local power peaking, breeding ratio, and fissile material requirements. Several schemes are evaluated to identify any major problems associated with reprocessing and fabrication of recycle actinide-containing assemblies. The overall efficiency of actinide burnout in LMFBRs is evaluated, and equilibrium cycle conditions are determined. It is concluded that actinide recycle in LMFBRs offers an attractive alternative to long term storage of the actinides, and does not significantly affect the performance of the host LMFBR. Assuming a 0.1 percent or less actinide loss during reprocessing, a 0.1 percent loss of less during fabrication, and proper recycle schemes, virtually all of the actinides produced by a fission reactor economy could be transmuted in fast reactors

  16. Minor actinide transmutation on PWR burnable poison rods

    International Nuclear Information System (INIS)

    Highlights: • Key issues associated with MA transmutation are the appropriate loading pattern. • Commercial PWRs are the only choice to transmute MAs in large scale currently. • Considerable amount of MA can be loaded to PWR without disturbing keff markedly. • Loading MA to PWR burnable poison rods for transmutation is an optimal loading pattern. - Abstract: Minor actinides are the primary contributors to long term radiotoxicity in spent fuel. The majority of commercial reactors in operation in the world are PWRs, so to study the minor actinide transmutation characteristics in the PWRs and ultimately realize the successful minor actinide transmutation in PWRs are crucial problem in the area of the nuclear waste disposal. The key issues associated with the minor actinide transmutation are the appropriate loading patterns when introducing minor actinides to the PWR core. We study two different minor actinide transmutation materials loading patterns on the PWR burnable poison rods, one is to coat a thin layer of minor actinide in the water gap between the zircaloy cladding and the stainless steel which is filled with water, another one is that minor actinides substitute for burnable poison directly within burnable poison rods. Simulation calculation indicates that the two loading patterns can load approximately equivalent to 5–6 PWR annual minor actinide yields without disturbing the PWR keff markedly. The PWR keff can return criticality again by slightly reducing the boric acid concentration in the coolant of PWR or removing some burnable poison rods without coating the minor actinide transmutation materials from PWR core. In other words, loading minor actinide transmutation material to PWR does not consume extra neutron, minor actinide just consumes the neutrons which absorbed by the removed control poisons. Both minor actinide loading patterns are technically feasible; most importantly do not need to modify the configuration of the PWR core and

  17. PREFACE: Actinides 2009

    Science.gov (United States)

    Rao, Linfeng; Tobin, James G.; Shuh, David K.

    2010-07-01

    This volume of IOP Conference Series: Materials Science and Engineering consists of 98 papers that were presented at Actinides 2009, the 8th International Conference on Actinide Science held on 12-17 July 2009 in San Francisco, California, USA. This conference was jointly organized by Lawrence Livermore National Laboratory and Lawrence Berkeley National Laboratory. The Actinides conference series started in Baden-Baden, Germany (1975) and this first conference was followed by meetings at Asilomar, CA, USA (1981), Aix-en-Provence, France (1985), Tashkent, USSR (1989), Santa Fe, NM, USA (1993), Baden-Baden, Germany (1997), Hayama, Japan (2001), and Manchester, UK (2005). The Actinides conference series provides a regular venue for the most recent research results on the chemistry, physics, and technology of the actinides and heaviest elements. Actinides 2009 provided a forum spanning a diverse range of scientific topics, including fundamental materials science, chemistry, physics, environmental science, and nuclear fuels. Of particular importance was a focus on the key roles that basic actinide chemistry and physics research play in advancing the worldwide renaissance of nuclear energy. Editors Linfeng Rao Lawrence Berkeley National Laboratory (lrao@lbl.gov) James G Tobin Lawrence Livermore National Laboratory (tobin1@llnl.gov) David K Shuh Lawrence Berkeley National Laboratory (dkshuh@lbl.gov)

  18. Minor actinides transmutation strategies in sodium fast reactors

    International Nuclear Information System (INIS)

    In minor actinides transmutation strategies for fast spectrum reactors, different possibilities regarding the core loading are considered. We study both homogeneous patterns (HOM) with various minor actinides (MA) content values and heterogeneous schemes (HET) with higher percentages of MA (Np, Am and Cm) at the periphery of reactor. We analyze the capability of transmutation of each design and the reactivity coefficients such as the Doppler constant, void worth and the fraction of delayed neutrons. The EVOLCODE2 code is the computational tool used in this study. It is based on MCNPX and ORIGEN/ACAB codes and allows carrying out burn-up calculations to get the isotopic evolution of fuel composition. Among the three strategies studied (HOM 2.5 %, HOM 4% and HET 20 %) for a possible design of a Sodium Cooled Fast Breeder Reactor, the one with better transmutation results is the HOM 4%, which shows higher absolute and relative values (12 Kg-MA/TWe, 29% respectively). Concerning transmutation in blankets with 20% MA content, results show a very little or no transmutation values when considering Np, Am and Cm together, though a positive small value for Np and Am is obtained

  19. Ground-State Properties ,of C, O, and Ne Isotopes in Hartree--Fock-Bogoliubov Calculation with Gogny Interaction

    Institute of Scientific and Technical Information of China (English)

    GUOLu; ZHAOEn-Guang; SAKATAFumihiko

    2003-01-01

    Ground-state properties of C, O, and Ne isotopes are described in the framework of Hartree-Fock-Bogoliubov theory with density-dependent finite-range Gogny interaction D1S. We include all the contributions to the Hartree-Fock and pairing feld arising from Gogny and Coulomb interaction as well as the center of mass correction in the numerical calcu/ations. These ground-state properties of C, O, and Ne isotopes are compared with available experimental results, Hartree-Fock plus BCS, shell model and relativistic Hartree--Bogoliubov calculations. The agreement between experiments and our theoretical results is pretty well. The predicted drip-line is dependent strongly on the model and effective interaction due to their sensitivity to various theoretical details. The calculations predict no evidence for halo structure predicted for C,O, and Ne isotopes in a previous RHB study.

  20. Emergence of rotational bands in ab initio no-core configuration interaction calculations of the Be isotopes

    CERN Document Server

    Maris, P; Vary, J P

    2014-01-01

    The emergence of rotational bands is observed in no-core configuration interaction (NCCI) calculations for the Be isotopes (7<=A<=12), as evidenced by rotational patterns for excitation energies, electromagnetic moments, and electromagnetic transitions. Yrast and low-lying excited bands are found. The results indicate well-developed rotational structure in NCCI calculations, using the JISP16 realistic nucleon-nucleon interaction within finite, computationally-accessible configuration spaces.

  1. THERMODYNAMICS OF THE ACTINIDES

    Energy Technology Data Exchange (ETDEWEB)

    Cunningham, Burris B.

    1962-04-01

    Recent work on the thermodynamic properties of the transplutonium elements is presented and discussed in relation to trends in thermodynamic properties of the actinide series. Accurate values are given for room temperature lattice parameters of two crystallographic forms, (facecentred cubic) fcc and dhcp (double-hexagonal closepacked), of americium metal and for the coefficients of thermal expansion between 157 and 878 deg K (dhcp) and 295 to 633 deg K (fcc). The meiting point of the metal, and its magnetic susceptibility between 77 and 823 deg K are reported and the latter compared with theoretical values for the tripositive ion calculated from spectroscopic data. Similar data (crystallography, meiting point and magnetic susceptibility) are given for metallic curium. A value for the heat of formation of americium monoxide is reported in conjunction with crystallographic data on the monoxide and mononitride. A revision is made in the current value for the heat of formation of Am/O/sub 2/ and for the potential of the Am(III)-Am(IV) couple. The crystal structures and lattice parameters are reported for the trichloride, oxychloride and oxides of californium. (auth)

  2. Transmutation of minor actinide using thorium fueled BWR core

    International Nuclear Information System (INIS)

    One of the methods to conduct transmutation of minor actinide is the use of BWR with thorium fuel. Thorium fuel has a specific behaviour of producing a little secondary minor actinides. Transmutation of minor actinide is done by loading it in the BWR with thorium fuel through two methods, namely close recycle and accumulation recycle. The calculation of minor actinide composition produced, weigh of minor actinide transmuted, and percentage of reminder transmutation was carried SRAC. The calculations were done to equivalent cell modeling from one fuel rod of BWR. The results show that minor actinide transmutation is more effective using thorium fuel than uranium fuel, through both close recycle and accumulation recycle. Minor actinide transmutation weight show that the same value for those recycle for 5th recycle. And most of all minor actinide produced from 5 unit BWR uranium fuel can transmuted in the 6th of close recycle. And, the minimal value of excess reactivity of the core is 12,15 % Δk/k, that is possible value for core operation

  3. Subsurface Biogeochemistry of Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Kersting, Annie B. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Univ. Relations and Science Education; Zavarin, Mavrik [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Inst.

    2016-06-29

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

  4. Fine-Grid Calculations for Stellar Electron and Positron Capture Rates on Fe-Isotopes

    CERN Document Server

    Nabi, Jameel-Un

    2011-01-01

    The acquisition of precise and reliable nuclear data is a prerequisite to success for stellar evolution and nucleosynthesis studies. Core-collapse simulators find it challenging to generate an explosion from the collapse of the core of massive stars. It is believed that a better understanding of the microphysics of core-collapse can lead to successful results. The weak interaction processes are able to trigger the collapse and control the lepton-to-baryon ratio ($Y_{e}$) of the core material. It is suggested that the temporal variation of $Y_{e}$ within the core of a massive star has a pivotal role to play in the stellar evolution and a fine-tuning of this parameter at various stages of presupernova evolution is the key to generate an explosion. During the presupernova evolution of massive stars, isotopes of iron, mainly $^{54,55,56}$Fe, are considered to be key players in controlling $Y_{e}$ ratio via electron capture on these nuclide. Recently an improved microscopic calculation of weak interaction mediated...

  5. Comparison of force fields and calculation methods for vibration intervals of isotopic H+3 molecules

    International Nuclear Information System (INIS)

    This paper reports (a) improved values for low-lying vibration intervals of H+3, H2D+, D2H+, and D+3 calculated using the variational method and Simons--Parr--Finlan representations of the Carney--Porter and Dykstra--Swope ab initio H+3 potential energy surfaces, (b) quartic normal coordinate force fields for isotopic H+3 molecules, (c) comparisons of variational and second-order perturbation theory, and (d) convergence properties of the Lai--Hagstrom internal coordinate vibrational Hamiltonian. Standard deviations between experimental and ab initio fundamental vibration intervals of H+3, H2D+, D2H+, and D+3 for these potential surfaces are 6.9 (Carney--Porter) and 1.2 cm-1 (Dykstra--Swope). The standard deviations between perturbation theory and exact variational fundamentals are 5 and 10 cm-1 for the respective surfaces. The internal coordinate Hamiltonian is found to be less efficient than the previously employed ''t'' coordinate Hamiltonian for these molecules, except in the case of H2D+

  6. The effects of actinide separation on the radiological consequences of disposal of high-level radioactive waste on the ocean bed

    International Nuclear Information System (INIS)

    One option in the management of high-level radioactive wastes is to separate the actinides prior to vitrification and disposal. This option is examined in the context of disposal of high-level wastes on the deep ocean bed. The initial quantity of waste corresponds to the generation of 1000 GW(e)y of nuclear energy, and the actinide-separation process is assumed to remove 99% of all elements of atomic number greater than that of actinium. The models used to describe the dispersion of activity from a single disposal site on the bed of the Atlantic Ocean represent both local dispersion and long-term mixing. Collective doses and doses to individuals are calculated for six potential pathways: ingestion of fish, crustacea, molluscs, plankton and seaweed, and external irradiation from contaminated beach sediments. The period from 400 to 1,000,000 years after disposal is considered. The potential radiological impact from disposal of high-level waste without separation of actinides on the ocean bed arises from the actinides; isotopes of americium, neptunium and plutonium give the highest doses. Actinide separation would reduce these doses in proportion to the effectiveness of the separation process, until doses become determined by fission products rather than actinides: the achievable dose reduction would be a factor of approximately a hundred, or less for certain pathways. This reduction applies only to doses to the public from waste disposal: no account was taken of doses arising from the separation process itself or from the management of the separated actinides. The results of the assessment are contrasted with those of similar studies based on toxicity indices. Major deficiencies are identified in the use of toxicity indices as a basis for decision-making. (author)

  7. Actinide measurements by AMS using fluoride matrices

    Science.gov (United States)

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

    2015-10-01

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

  8. Electronic Structure of the Actinide Metals

    DEFF Research Database (Denmark)

    Johansson, B.; Skriver, Hans Lomholt

    1982-01-01

    itinerant to localized 5f electron behaviour calculated to take place between plutonium and americium. From experimental data it is shown that the screening of deep core-holes is due to 5f electrons for the lighter actinide elements and 6d electrons for the heavier elements. A simplified model for the full...

  9. Waste disposal aspects of actinide separation

    International Nuclear Information System (INIS)

    Two recent NRPB reports are summarized (Camplin, W.C., Grimwood, P.D. and White, I.F., The effects of actinide separation on the radiological consequences of disposal of high-level radioactive waste on the ocean bed, Harwell, National Radiological Protection Board, NRPB-R94 (1980), London, HMSO; Hill, M.D., White, I.F. and Fleishman, A.B., The effects of actinide separation on the radiological consequences of geologic disposal of high-level waste. Harwell, National Radiological Protection Board, NRPB-R95 (1980), London, HMSO). They describe preliminary environmental assessments relevant to waste arising from the reprocessing of PWR fuel. Details are given of the modelling of transport of radionuclides to man, and of the methodology for calculating effective dose equivalents in man. Emphasis has been placed on the interaction between actinide separation and the disposal options rather than comparison of disposal options. The reports show that the effects of actinide separation do depend on the disposal method. Conditions are outlined where the required substantial further research and development work on actinide separation and recycle would be justified. Toxicity indices or 'toxic potentials' can be misleading and should not be used to guide research and development. (U.K.)

  10. Density functional theory calculations of H/D isotope effects on polymer electrolyte membrane fuel cell operations

    International Nuclear Information System (INIS)

    To elucidate hydrogen isotope effects observed between fuel and exhaust hydrogen gases during polymer electrolyte membrane fuel cell operations, H-to-D reduced partition function ratios (RPFRs) for the hydrogen species in the Pt catalyst phase of the anode and the electrolyte membrane phase of the fuel cell were evaluated by density functional theory calculations on model species of the two phases. The evaluation yielded 3.2365 as the value of the equilibrium constant of the hydrogen isotope exchange reaction between the two phases at 39 C, which was close to the experimentally estimated value of 3.46-3.99 at the same temperature. It was indicated that H+ ions on the Pt catalyst surface of the anode and H species in the electrolyte membrane phase were isotopically in equilibrium with one another during fuel cell operations.

  11. The electronic structure of the lanthanides and actinides, a comparison

    International Nuclear Information System (INIS)

    Full text: Optical spectra of the two f-element series (the lanthanides and actinides) are comparable in many respects. For the trivalent ions isolated in single crystals, both series exhibit rich, narrow line spectra. These data can be analysed in terms of a parametric model based on a free-ion Hamiltonian plus the addition of a crystal field Hamiltonian. For most systems the agreement between the calculated and experimental energy levels is quite good. In the actinide series there appears to be a correlation between the magnitude of the crystal field and the inadequacy of the fits. The early actinides exhibit multiple oxidation states for which there is no precedent in the lanthanide series. The parametric model mentioned earlier has been utilized for some tetravalent actinide systems with reasonably good results. A selective survey of results describing the similarities and differences of various lanthanide and actinide systems will be given

  12. Scenarios for the transmutation of actinides in CANDU reactors

    Energy Technology Data Exchange (ETDEWEB)

    Hyland, Bronwyn, E-mail: hylandb@aecl.ca [Atomic Energy of Canada Limited, Chalk River Laboratories, Chalk River, Ontario, K0J 1J0 (Canada); Gihm, Brian, E-mail: gihmb@aecl.ca [Atomic Energy of Canada Limited, 2251 Speakman Drive, Mississauga, Ontario, L5K 1B2 (Canada)

    2011-12-15

    With world stockpiles of used nuclear fuel increasing, the need to address the long-term utilization of this resource is being studied. Many of the transuranic (TRU) actinides in nuclear spent fuel produce decay heat for long durations, resulting in significant nuclear waste management challenges. These actinides can be transmuted to shorter-lived isotopes to reduce the decay heat period or consumed as fuel in a CANDU(R) reactor. Many of the design features of the CANDU reactor make it uniquely adaptable to actinide transmutation. The small, simple fuel bundle simplifies the fabrication and handling of active fuels. Online refuelling allows precise management of core reactivity and separate insertion of the actinides and fuel bundles into the core. The high neutron economy of the CANDU reactor results in high TRU destruction to fissile-loading ratio. This paper provides a summary of actinide transmutation schemes that have been studied in CANDU reactors at AECL, including the works performed in the past. The schemes studied include homogeneous scenarios in which actinides are uniformly distributed in all fuel bundles in the reactor, as well as heterogeneous scenarios in which dedicated channels in the reactor are loaded with actinide targets and the rest of the reactor is loaded with fuel. The transmutation schemes that are presented reflect several different partitioning schemes. Separation of americium, often with curium, from the other actinides enables targeted destruction of americium, which is a main contributor to the decay heat 100-1000 years after discharge from the reactor. Another scheme is group-extracted transuranic elements, in which all of the transuranic elements, plutonium (Pu), neptunium (Np), americium (Am), and curium (Cm) are extracted together and then transmuted. This paper also addresses ways of utilizing the recycled uranium, another stream from the separation of spent nuclear fuel, in order to drive the transmutation of other actinides.

  13. Actinides and Life's Origins.

    Science.gov (United States)

    Adam, Zachary

    2007-12-01

    There are growing indications that life began in a radioactive beach environment. A geologic framework for the origin or support of life in a Hadean heavy mineral placer beach has been developed, based on the unique chemical properties of the lower-electronic actinides, which act as nuclear fissile and fertile fuels, radiolytic energy sources, oligomer catalysts, and coordinating ions (along with mineralogically associated lanthanides) for prototypical prebiotic homonuclear and dinuclear metalloenzymes. A four-factor nuclear reactor model was constructed to estimate how much uranium would have been required to initiate a sustainable fission reaction within a placer beach sand 4.3 billion years ago. It was calculated that about 1-8 weight percent of the sand would have to have been uraninite, depending on the weight percent, uranium enrichment, and quantity of neutron poisons present within the remaining placer minerals. Radiolysis experiments were conducted with various solvents with the use of uraniumand thorium-rich minerals (metatorbernite and monazite, respectively) as proxies for radioactive beach sand in contact with different carbon, hydrogen, oxygen, and nitrogen reactants. Radiation bombardment ranged in duration of exposure from 3 weeks to 6 months. Low levels of acetonitrile (estimated to be on the order of parts per billion in concentration) were conclusively identified in 2 setups and tentatively indicated in a 3(rd) by gas chromatography/mass spectrometry. These low levels have been interpreted within the context of a Hadean placer beach prebiotic framework to demonstrate the promise of investigating natural nuclear reactors as power production sites that might have assisted the origins of life on young rocky planets with a sufficiently differentiated crust/mantle structure. Future investigations are recommended to better quantify the complex relationships between energy release, radioactive grain size, fissionability, reactant phase, phosphorus

  14. Calculated activities of some isotopes in the RA reactor highly enriched fuel significant for possible environmental contamination - Operational report

    International Nuclear Information System (INIS)

    This report contains calculation basis and obtained results of activities for three groups of isotopes in the RA reactor 80% enriched fuel element. The following isotopes are included: 1) 85mKr, 87Kr, 88Kr, 131J, 132J, 133J, 134J, 135J, 133Xe, 138Xe i 138Cs, 2) 89Sr, 90Sr, 91Sr, 92Sr, 95Zr, 97Zr, 103Ru, 105Ru, 106Ru, 129mTe, 134Cs, 137Cs, 140Ba, 144Ce, kao i 3) 238Pu, 239Pu i 240Pu. It was estimated that the fuel is exposed to mean neutron flux. The periodicity of reactor operation is taken into account. Calculation results are given dependent on the time of exposure. These results are to be used as source data for Ra reactor safety analyses

  15. Statistical model calculations of pre-scission neutron multiplicity for the heavy ion induced fusion-fission reactions with actinide target 232Th

    Directory of Open Access Journals (Sweden)

    Thakur Meenu

    2015-01-01

    Full Text Available The reaction mechanism of 19F + 232Th and 28Si + 232Th systems populating the near-super-heavy compound nuclei 251Es and 260Rf respectively are investigated using neutron multiplicity as a probe. The prescission neutron multiplicities of these compound nuclei are calculated at different excitation energies using a statistical model code. These calculations are performed using the Bohr-Wheeler transition state fission width as well as the dissipative dynamical fission width based on the Kramers’ prescription. For 19F + 232Th system, the measured yield of pre-scission is compared with the statistical model calculations for the decay of a compound nucleus in the excitation energy range of 54-90 MeV. The comparison between the measured and the calculated values indicates that the Bohr-Wheeler fission width underestimates the pre-scission neutron yield and a large amount of dissipation strength is required to reproduce the experimental pre-scission neutron multiplicities. The excitation energy dependence of the fitted values of the dissipation coefficient is also discussed. In addition, exploratory statistical model calculations of pre-scission neutron multiplicity for the 28Si + 232Th system are presented in the above range of excitation energy.

  16. Calculation of proton-induced reactions on Tellurium isotopes below 60 MeV for medical radioisotope production

    International Nuclear Information System (INIS)

    The 123Te(p,n)123I, 124Te(p,n)124I and 124Te(p,2n)123I reactions, among the many reaction channels opened, are the major reactions under consideration from a diagnostic purpose because reaction residuals as the gamma emitters are used for most radiopharmaceutical applications involving radioiodine. Based on the available experimental data, the absorption cross sections and elastic scattering angular distributions of the proton-induced nuclear reaction on Te isotopes below 60 NeV are calculated using the optical model code APMNK. The transmission coefficients of neutron, proton, deuteron, trition and alpha particles are calculated by CUNF code and are fed into the GNASH code. By adjusting level density parameters and the pair correction values of some reaction channels, as well as the composite nucleus state density constants of the pre-equilibrium model, the production cross sections and energy-angle correlated spectra of the secondary light particles, as well as production cross sections and energy distributions of heavy recoils and gamma rays are calculated by the statistical plus pre-equilibrium model code GNAH. The calculated results are analysed and compared with the experimental data taken from the EXFOR. The optimized global optical model parameters give overall agreement with the experimental data over both the entire energy range and all tellurium isotopes. (author)

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

    Energy Technology Data Exchange (ETDEWEB)

    Leyba, J.D.

    1990-09-07

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

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

    International Nuclear Information System (INIS)

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

  19. Compilation of actinide neutron nuclear data

    International Nuclear Information System (INIS)

    The Swedish nuclear data committee has compiled a selected set of neutron cross section data for the 16 most important actinide isotopes. The aim of the report is to present available data in a comprehensible way to allow a comparison between different evaluated libraries and to judge about the reliability of these libraries from the experimental data. The data are given in graphical form below about 1 ev and above about 10 keV shile the 2200 m/s cross sections and resonance integrals are given in numerical form. (G.B.)

  20. Status of nuclear data for actinides

    Energy Technology Data Exchange (ETDEWEB)

    Guzhovskii, B.Y.; Gorelov, V.P.; Grebennikov, A.N. [Russia Federal Nuclear Centre, Arzamas (Russian Federation)] [and others

    1995-10-01

    Nuclear data required for transmutation problem include many actinide nuclei. In present paper the analysis of neutron fission, capture, (n,2n) and (n,3n) reaction cross sections at energy region from thermal point to 14 MeV was carried out for Th, Pa, U, Np, Pu, Am and Cm isotops using modern evaluated nuclear data libraries and handbooks of recommended nuclear data. Comparison of these data indicates on substantial discrepancies in different versions of files, that connect with quality and completeness of original experimental data.

  1. Review of Axial Burnup Distribution Considerations for Burnup Credit Calculations

    Energy Technology Data Exchange (ETDEWEB)

    Wagner, J.C.; DeHart, M.D.

    2000-03-01

    This report attempts to summarize and consolidate the existing knowledge on axial burnup distribution issues that are important to burnup credit criticality safety calculations. Recently released Nuclear Regulatory Commission (NRC) staff guidance permits limited burnup credit, and thus, has prompted resolution of the axial burnup distribution issue. The reactivity difference between the neutron multiplication factor (keff) calculated with explicit representation of the axial burnup distribution and keff calculated assuming a uniform axial burnup is referred to as the ``end effect.'' This end effect is shown to be dependent on many factors, including the axial-burnup profile, total accumulated burnup, cooling time, initial enrichment, assembly design, and the isotopics considered (i.e., actinide-only or actinides plus fission products). Axial modeling studies, efforts related to the development of axial-profile databases, and the determination of bounding axial profiles are also discussed. Finally, areas that could benefit from further efforts are identified.

  2. Review of Axial Burnup Distribution Considerations for Burnup Credit Calculations

    International Nuclear Information System (INIS)

    This report attempts to summarize and consolidate the existing knowledge on axial burnup distribution issues that are important to burnup credit criticality safety calculations. Recently released Nuclear Regulatory Commission (NRC) staff guidance permits limited burnup credit, and thus, has prompted resolution of the axial burnup distribution issue. The reactivity difference between the neutron multiplication factor (keff) calculated with explicit representation of the axial burnup distribution and keff calculated assuming a uniform axial burnup is referred to as the ''end effect.'' This end effect is shown to be dependent on many factors, including the axial-burnup profile, total accumulated burnup, cooling time, initial enrichment, assembly design, and the isotopics considered (i.e., actinide-only or actinides plus fission products). Axial modeling studies, efforts related to the development of axial-profile databases, and the determination of bounding axial profiles are also discussed. Finally, areas that could benefit from further efforts are identified

  3. Physics studies of higher actinide consumption in an LMR

    Energy Technology Data Exchange (ETDEWEB)

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

    1990-01-01

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

  4. Comparison of Self-Consistent Skyrme and Gogny Calculations for Light Hg Isotopes

    CERN Document Server

    Warda, M; Próchniak, L

    2009-01-01

    The ground-state properties of neutron-deficient Hg isotopes have been investigated by the constrained self-consistent Hartree-Fock-Bogoliubov approach with the Skyrme and Gogny effective forces. In the case of the Skyrme interaction we h ave also applied the Hartree-Fock+BCS model with the state-dependent $\\delta$-pairing interaction. Potential energy surfaces and pairing properties have been compared for the both types of forces.

  5. Device for Detecting Actinides, Method for Detecting Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Stevens, Fred J.; Wilkins-Stevens, Priscilla

    1998-10-29

    A heavy metal detector is provided comprising a first molecule and a second molecule, whereby the first and second molecules interact in a predetermined manner; a first region on the first molecule adapted to interact with an actinide; and a second region on the second molecule adapted to interact with the actinide, whereby the interactions of the actinide with the regions effect the predetermined manner of interaction between the molecules.

  6. Simulation calculations for a catalytic exchange/cryogenic distillation hydrogen isotope separation process

    International Nuclear Information System (INIS)

    Some of the aspects of the optimization and simulation calculations for the Moderator Detritiation Plant thay may be applicable to other processes are described. The FORTRAN optimization program and the CPES and PROCESS distillation calculation are covered

  7. Models for calculating the effects of isotopic exchange, radioactive decay, and of recycle in removing iodine from gas and liquid streams

    International Nuclear Information System (INIS)

    Different decontamination factors for 129I and 131I are frequently invoked in environmental impact reports concerned with nuclear fuel recycle. Selected differences, or ratios, have not been justified on the basis of mathematical models or experimental data. A description is given of the origins of these differences in terms of isotopic exchange and material balance equations for the short- and long-lived (or stable) isotopes. The ratios of decontamination factors can be calculated when there is complete attainment of isotopic exchange between gas- or liquid-phase iodine and iodine sorbed by a solid or liquid. If there is no exchange, decontamination factors are isotope-independent unless material recycle occurs within the system. Between these extremes, there can be decontamination factors whose explanation requires experimental determination of the extent of exchange. The model applies to other radioactive isotopes of iodine as well as to other elements with short- and long-lived (or stable) isotopes. (auth)

  8. Comparison of isotopic compositions in the frame of the NEA depletion calculation benchmark devoted to MOX fuel cycles

    International Nuclear Information System (INIS)

    An accurate knowledge of irradiated fuel composition is of utmost importance regarding properties such as criticality, activity or residual heat generation. These magnitudes are in turn essential to fuel transport and storage and depend on many parameters, from which of course fuel type is essential. In the frame of activities devoted to fuel cycle issues, the NEA WPRS proposed a Depletion Calculation Benchmark to compare results and trends with different codes and libraries. While Phase 1 dealt with UOX fuel, Phase 2 is devoted to MOX fuel. The present paper aims at comparing isotopic compositions for MOX fuel obtained by GRS and AREVA with different codes and libraries. (orig.)

  9. The electrochemical properties of actinide amalgams

    International Nuclear Information System (INIS)

    Standard potentials are selected for actinides (An) and their amalgams. From the obtained results, energy characteristics are calculated and analyzed for alloy formation in An-Hg systems. It is found that solutions of the f-elements in mercury are very close in properties to amalgams of the alkali and alkaline-earth metals, except that, for the active Group III metals, the ion skeletons have a greater number of realizable charged states in the condensed phase

  10. Recovering actinide values

    International Nuclear Information System (INIS)

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

  11. Actinides: why are they important biologically

    International Nuclear Information System (INIS)

    The following topics are discussed: actinide elements in energy systems; biological hazards of the actinides; radiation protection standards; and purposes of actinide biological research with regard to toxicity, metabolism, and therapeutic regimens

  12. Photoelectron spectra of actinide compounds

    International Nuclear Information System (INIS)

    A brief overview of the application of photoelectron spectroscopy is presented for the study of actinide materials. Phenomenology as well as specific materials are discussed with illustrative examples

  13. Gamma spectroscopy of neutron rich actinide nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Birkenbach, Benedikt; Geibel, Kerstin; Vogt, Andreas; Hess, Herbert; Reiter, Peter; Steinbach, Tim; Schneiders, David [Koeln Univ. (Germany). IKP; Collaboration: AGATA-Collaboration

    2013-07-01

    Excited states in neutron-rich actinide Th and U nuclei were investigated after multi nucleon transfer reactions employing the AGATA demonstrator and PRISMA setup at LNL (INFN, Italy). A primary {sup 136}Xe beam of 1 GeV hitting a {sup 238}U target was used to produce the nuclei of interest. Beam-like reaction products of Xe- and Ba isotopes after neutron transfer were selected by the PRISMA spectrometer. The recoil like particles were registered by a MCP detector inside the scattering chamber. Coincident γ-rays from excited states in beam and target like particles were measured with the position sensitive AGATA HPGe detectors. Improved Doppler correction and quality of the γ-spectra is based on the novel γ-ray tracking technique which was successfully exploited. First results on the collective properties of various Th and U isotopes are discussed.

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

    Science.gov (United States)

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

    2016-01-01

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

  15. Model calculation of A-type zeolite selectivity in adsorption of hydrogen isotope molecules. Henry region

    International Nuclear Information System (INIS)

    The available literary data on IR-spectra of two-atom molecules adsorbed on A-type zeolites have been studied to calculate and compare shift values of transition band maxima. For Na12A zeolite with its most precise roentgenographic data, calculated shifts of H2, D2, N2 bands coincide with experimental for one set of characteristics of zeolite lattice ions, using the ion characteristics obtained coefficients of H2 and D2 mixture separation, adsorption heat and Ne, Ar Henry constant are calculated. They are compared with experimental values

  16. Calculations for HFIR [High Flux Isotope Reactor] fuel plate non- bonding and fuel segregation uncertainty factors

    International Nuclear Information System (INIS)

    The effects of non-bonds and of fuel segregation on the package factors of the heat flux in the High Flux Isotope Reactor (HFIR) are examined. The effects of the two defects are examined both separately and together. It is concluded that the peaking factors that are used in the present HFIR thermal analysis code are conservative and thus no changes in the peaking factors are necessary to continue to ensure that HFIR is safe. A study was made of the effect of the non-bond spot diameter on the peaking factor. The conclusion is that the spot can have diameter more than three times the maximum value allowed by the specifications before the peaking factor is greater than the maximum value specified in the present HFIR thermal analysis code. 6 refs., 7 figs., 8 tabs

  17. Baseline identification in stable isotope studies of temperate lotic systems and implications for calculated trophic positions

    DEFF Research Database (Denmark)

    Kristensen, Peter Brinkmann; Riis, Tenna; Dylmer, Hans Erik;

    2016-01-01

    including several taxonomic groups and feeding types due to difficulties of finding ubiquitous taxonomic groups. We identified taxonomic groups which correlated well with land use in Danish lowland streams, and several of those are widely distributed in running waters in the Northern hemisphere...... of two common fish species (three-spined stickleback, Gasterosteus aculeatus, and brown trout Salmo trutta) differed markedly depending on the baseline chosen. The estimated trophic position was lowest when based on Baetidae and highest when using Simuliidae. The trophic position of Gasterosteus......) are thus apparently the best indicator of land uses, not least when the gradient of land use is large. Our results strongly support the use of these organisms as baseline in stable isotope studies of trophic webs....

  18. Isotopic clusters

    International Nuclear Information System (INIS)

    Spectra of isotopically mixed clusters (dimers of SF6) are calculated as well as transition frequencies. The result leads to speculations about the suitability of the laser-cluster fragmentation process for isotope separation. (Auth.)

  19. Factors affecting actinide solubility in a repository for spent fuel, 1

    International Nuclear Information System (INIS)

    The main tasks in the study were to get information on the chemical conditions in a repository for spent fuel and information on factors affecting releases of actinides from spent fuel and solubility of actinides in a repository for spent fuel. The work in this field started at the Reactor Laboratory of the Technical Research Centre of Finland (VTT) in 1982. This is a report on the effects on the main parameters, Eh, pH, carbonate, organic compounds, colloids, microbes and radiation on the actinide solubility in the nearfield of the repository. Another task has been to identify available models and reported experience from actinide solubility calculations with different codes. 167 refs

  20. Utilization of Minor Actinides (Np, Am, Cm) in Nuclear Power Reactor

    Science.gov (United States)

    Gerasimov, A.; Bergelson, B.; Tikhomirov, G.

    2014-06-01

    Calculation research of the utilization process of minor actinides (transmutation with use of power released) is performed for specialized power reactor of the VVER type operating on the level of electric power of 1000 MW. Five subsequent cycles are considered for the reactor with fuel elements containing minor actinides along with enriched uranium. It was shown that one specialized reactor for the one cycle (900 days) can utilize minor actinides from several VVER-1000 reactors without any technological and structural modifications. Power released because of minor actinide fission is about 4% with respect to the total power

  1. Optical techniques for actinide research

    International Nuclear Information System (INIS)

    In recent years, substantial gains have been made in the development of spectroscopic techniques for electronic properties studies. These techniques have seen relatively small, but growing, application in the field of actinide research. Photoemission spectroscopies, reflectivity and absorption studies, and x-ray techniques will be discussed and illustrative examples of studies on actinide materials will be presented

  2. Surface energy and work function of the light actinides

    DEFF Research Database (Denmark)

    Kollár, J.; Vitos, Levente; Skriver, Hans Lomholt

    1994-01-01

    We have calculated the surface energy and work function of the light actinides Fr, Ra, Ac, Th, Pa, U, Np, and Pu by means of a Green's-function technique based on the linear-muffin-tin-orbitals method within the tight-binding representation. In these calculations we apply an energy functional whi...

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

    Science.gov (United States)

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

    1977-01-01

    Design power plant studies were carried out for two applications of the plasma core reactor: (1) As a breeder reactor, (2) As a reactor able to transmute actinides effectively. In addition to the above applications the reactor produced electrical power with a high efficiency. A reactor subsystem was designed for each of the two applications. For the breeder reactor, neutronics calculations were carried out for a U-233 plasma core with a molten salt breeding blanket. A reactor was designed with a low critical mass (less than a few hundred kilograms U-233) and a breeding ratio of 1.01. The plasma core actinide transmutation reactor was designed to transmute the nuclear waste from conventional LWR's. The spent fuel is reprocessed during which 100% of Np, Am, Cm, and higher actinides are separated from the other components. These actinides are then manufactured as oxides into zirconium clad fuel rods and charged as fuel assemblies in the reflector region of the plasma core actinide transmutation reactor. In the equilibrium cycle, about 7% of the actinides are directly fissioned away, while about 31% are removed by reprocessing.

  4. Hartree-Fock-Bogoliubov calculation of ground state properties of even-even and odd Mo and Ru isotopes

    CERN Document Server

    Bassem, Y El

    2016-01-01

    In a previous work [Int. J. Mod. Phys. E 24, 1550073 (2015)], hereafter referred as paper I, we have investigated the ground-state properties of Nd, Ce and Sm isotopes within Hartree-Fock-Bogoliubov method with SLy5 skyrme force in which the pairing strength has been generalized with a new proposed formula. However, that formula is more appropriate for the region of Nd. In this work, we have studied the ground-state properties of both even-even and odd Mo and Ru isotopes. For this, we have used Hartree- Fock-Bogoliubov method with SLy4 skyrme force, and a new formula of the pairing strength which is more accurate for this region of nuclei. The results have been compared with available experimental data, the results of Hartree-Fock-Bogoliubov calculations based on the D1S Gogny effective nucleon-nucleon interaction and predictions of some nuclear models such as Finite Range Droplet Model (FRDM) and Relativistic Mean Field (RMF) theory.

  5. The complete relativistic kinetic model of symmetry violation in isotopic expanding plasma. III. Specific entropy calculation

    CERN Document Server

    Ignatyev, Yu G

    2010-01-01

    A complete model of baryon production in an expanding, primordially symmetric hot Universe is constructed in the framework of general-relativistic kinetic theory. In this model specific model for a baryon is calculated and graphs of the value dependence are constructed.

  6. Criticality calculations of a generic fuel container for fuel assemblies PWR, by means of the code MCNP; Calculos de criticidad de un contenedor de combustible generico para ensambles combustibles PWR, mediante el codigo MCNP

    Energy Technology Data Exchange (ETDEWEB)

    Vargas E, S.; Esquivel E, J.; Ramirez S, J. R., E-mail: samuel.vargas@inin.gob.mx [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico)

    2013-10-15

    The purpose of the concept of burned consideration (Burn-up credit) is determining the capacity of the calculation codes, as well as of the nuclear data associates to predict the isotopic composition and the corresponding neutrons effective multiplication factor in a generic container of spent fuel during some time of relevant storage. The present work has as objective determining this capacity of the calculation code MCNP in the prediction of the neutrons effective multiplication factor for a fuel assemblies arrangement type PWR inside a container of generic storage. The calculations are divided in two parts, the first, in the decay calculations with specified nuclide concentrations by the reference for a pressure water reactor (PWR) with enriched fuel to 4.5% and a discharge burned of 50 GW d/Mtu. The second, in criticality calculations with isotopic compositions dependent of the time for actinides and important fission products, taking 30 time steps, for two actinide groups and fission products. (Author)

  7. Calculation of electron and isotopes dose point kernels with FLUKA Monte Carlo code for dosimetry in nuclear medicine therapy

    CERN Document Server

    Mairani, A; Valente, M; Battistoni, G; Botta, F; Pedroli, G; Ferrari, A; Cremonesi, M; Di Dia, A; Ferrari, M; Fasso, A

    2011-01-01

    Purpose: The calculation of patient-specific dose distribution can be achieved by Monte Carlo simulations or by analytical methods. In this study, FLUKA Monte Carlo code has been considered for use in nuclear medicine dosimetry. Up to now, FLUKA has mainly been dedicated to other fields, namely high energy physics, radiation protection, and hadrontherapy. When first employing a Monte Carlo code for nuclear medicine dosimetry, its results concerning electron transport at energies typical of nuclear medicine applications need to be verified. This is commonly achieved by means of calculation of a representative parameter and comparison with reference data. Dose point kernel (DPK), quantifying the energy deposition all around a point isotropic source, is often the one. Methods: FLUKA DPKS have been calculated in both water and compact bone for monoenergetic electrons (10-3 MeV) and for beta emitting isotopes commonly used for therapy ((89)Sr, (90)Y, (131)I, (153)Sm, (177)Lu, (186)Re, and (188)Re). Point isotropic...

  8. MCNPX Monte Carlo burnup simulations of the isotope correlation experiments in the NPP Obrigheim

    Energy Technology Data Exchange (ETDEWEB)

    Cao Yan, E-mail: ycao@anl.go [Nuclear Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (United States); Gohar, Yousry [Nuclear Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, IL 60439 (United States); Broeders, Cornelis H.M. [Forschungszentrum Karlsruhe, Institute for Neutron Physics and Reactor Technology, P.O. Box 3640, 76021 Karlsruhe (Germany)

    2010-10-15

    This paper describes the simulation work of the Isotope Correlation Experiment (ICE) using the MCNPX Monte Carlo computer code package. The Monte Carlo simulation results are compared with the ICE-Experimental measurements for burnup up to 30 GWD/t. The comparison shows the good capabilities of the MCNPX computer code package for predicting the depletion of the uranium fuel and the buildup of the plutonium isotopes in a PWR thermal reactor. The Monte Carlo simulation results show also good agreements with the experimental data for calculating several long-lived and stable fission products. However, for the americium and curium actinides, it is difficult to judge the predication capabilities for these actinides due to the large uncertainties in the ICE-Experimental data. In the MCNPX numerical simulations, a pin cell model is utilized to simulate the fuel lattice of the nuclear power reactor. Temperature dependent libraries based on JEFF3.1 nuclear data files are utilized for the calculations. In addition, temperature dependent libraries based ENDF/B-VII nuclear data files are utilized and the obtained results are very close to the JEFF3.1 results, except for {approx}10% differences in the prediction of the minor actinide isotopes buildup.

  9. Concentration of actinides in the food chain

    International Nuclear Information System (INIS)

    Considerable concern is now being expressed over the discharge of actinides into the environment. This report presents a brief review of the chemistry of the actinides and examines the evidence for interaction of the actinides with some naturally-occurring chelating agents and other factors which might stimulate actinide concentration in the food chain of man. This report also reviews the evidence for concentration of actinides in plants and for uptake through the gastrointestinal tract. (author)

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

    Science.gov (United States)

    Chang, G S; Ambrosek, R G

    2005-01-01

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

  11. Influence of longitudinal isotope substitution on the thermal conductivity of carbon nanotubes: Results of nonequilibrium molecular dynamics and local density functional calculations

    Energy Technology Data Exchange (ETDEWEB)

    Leroy, Frédéric, E-mail: f.leroy@theo.chemie.tu-darmstadt.de; Böhm, Michael C., E-mail: boehm@theo.chemie.tu-darmstadt.de [Eduard-Zintl-Institut für Anorganische und Physikalische Chemie, Technische Universität Darmstadt, D-64287 Darmstadt (Germany); Schulte, Joachim [Bruker Biospin GmbH, Silberstreifen, D-76287 Rheinstetten (Germany); Balasubramanian, Ganesh [Department of Mechanical Engineering, Iowa State University, Ames, Iowa 50011 (United States)

    2014-04-14

    We report reverse nonequilibrium molecular dynamics calculations of the thermal conductivity of isotope substituted (10,10) carbon nanotubes (CNTs) at 300 K. {sup 12}C and {sup 14}C isotopes both at 50% content were arranged either randomly, in bands running parallel to the main axis of the CNTs or in bands perpendicular to this axis. It is found that the systems with randomly distributed isotopes yield significantly reduced thermal conductivity. In contrast, the systems where the isotopes are organized in patterns parallel to the CNTs axis feature no reduction in thermal conductivity when compared with the pure {sup 14}C system. Moreover, a reduction of approximately 30% is observed in the system with the bands of isotopes running perpendicular to the CNT axis. The computation of phonon dispersion curves in the local density approximation and classical densities of vibrational states reveal that the phonon structure of carbon nanotubes is conserved in the isotope substituted systems with the ordered patterns, yielding high thermal conductivities in spite of the mass heterogeneity. In order to complement our conclusions on the {sup 12}C-{sup 14}C mixtures, we computed the thermal conductivity of systems where the {sup 14}C isotope was turned into pseudo-atoms of 20 and 40 atomic mass units.

  12. Influence of longitudinal isotope substitution on the thermal conductivity of carbon nanotubes: Results of nonequilibrium molecular dynamics and local density functional calculations

    International Nuclear Information System (INIS)

    We report reverse nonequilibrium molecular dynamics calculations of the thermal conductivity of isotope substituted (10,10) carbon nanotubes (CNTs) at 300 K. 12C and 14C isotopes both at 50% content were arranged either randomly, in bands running parallel to the main axis of the CNTs or in bands perpendicular to this axis. It is found that the systems with randomly distributed isotopes yield significantly reduced thermal conductivity. In contrast, the systems where the isotopes are organized in patterns parallel to the CNTs axis feature no reduction in thermal conductivity when compared with the pure 14C system. Moreover, a reduction of approximately 30% is observed in the system with the bands of isotopes running perpendicular to the CNT axis. The computation of phonon dispersion curves in the local density approximation and classical densities of vibrational states reveal that the phonon structure of carbon nanotubes is conserved in the isotope substituted systems with the ordered patterns, yielding high thermal conductivities in spite of the mass heterogeneity. In order to complement our conclusions on the 12C-14C mixtures, we computed the thermal conductivity of systems where the 14C isotope was turned into pseudo-atoms of 20 and 40 atomic mass units

  13. Actinides, accelerators and erosion

    OpenAIRE

    Fifield L. K.; Tims S.G.

    2012-01-01

    Fallout isotopes can be used as artificial tracers of soil erosion and sediment accumulation. The most commonly used isotope to date has been 137Cs. Concentrations of 137Cs are, however, significantly lower in the Southern Hemisphere, and furthermore have now declined to 35% of original values due to radioactive decay. As a consequence the future utility of 137Cs is limited in Australia, with many erosion applications becoming untenable within the next 20 years, and there is a need to replace...

  14. Self-consistent calculations of the strength function and radiative neutron capture cross section for stable and unstable tin isotopes

    CERN Document Server

    Goriely, S; Krewald, S

    2011-01-01

    The E1 strength function for 15 stable and unstable Sn even-even isotopes from A=100 till A=176 are calculated using the self-consistent microscopic theory which, in addition to the standard (Q)RPA approach, takes into account the single-particle continuum and the phonon coupling. Our analysis shows two distinct regions for which the integral characteristics of both the giant and pygmy resonances behave rather differently. For neutron-rich nuclei, starting from $^{132}$Sn, we obtain a giant E1 resonance which significantly deviates from the widely-used systematics extrapolated from experimental data in the $\\beta$-stability valley. We show that the inclusion of the phonon coupling is necessary for a proper description of the low-energy pygmy resonances and the corresponding transition densities for $A132$ region the influence of phonon coupling is significantly smaller. The radiative neutron capture cross sections leading to the stable $^{124}$Sn and unstable $^{132}$Sn and $^{150}$Sn nuclei are calculated wi...

  15. Fusion-Fission Burner for Transuranic Actinides

    Science.gov (United States)

    Choi, Chan

    2013-10-01

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

  16. Electronic structure of the actinide dioxides

    International Nuclear Information System (INIS)

    The electronic properties of the fluorite structured actinide dioxides have been investigated using the linear muffin tin orbital method in the atomic sphere approximation. CaF2 with the same structure was also studied because of the relative simplicity of its electronic structure and the greater amount of experimental data available. Band structures were calculated both non self consistently and self consistently. In the non self consistent calculations the effect of changing the approximation to the exchange-correlation potential and the starting atomic configurations was examined. Using the concepts of canonical bands the effects of hybridization were investigated. In particular the 5f electrons included in the band picture were found to mix more strongly into the valence band than indicated by experiment. On this basis the 5f electrons were not included in self consistent calculations which in the density functional formalism are capable of yielding ground state properties. Because of the non participation of the f electrons in the bonding UO2 only was considered as representative of the actinide dioxides. For comparison CaF2 was also examined. Using Pettifor's pressure formula to determine the equilibrium condition the lattice constants were calculated to be 0.5% and 5% respectively below the experimental values. (author)

  17. Environmental research on actinide elements

    International Nuclear Information System (INIS)

    The papers synthesize the results of research sponsored by DOE's Office of Health and Environmental Research on the behavior of transuranic and actinide elements in the environment. Separate abstracts have been prepared for the 21 individual papers

  18. Calculation of absorbed dose for skin contamination imparted by beta radiation through the VARSKIN modified code for 122 interesting isotopes for nuclear medicine, nuclear power plants and research

    International Nuclear Information System (INIS)

    In this work the implementation of a modification of the VARSKIN code for calculation of absorbed dose for contamination in skin imparted by external radiation fields generated by Beta emitting is presented. The modification consists on the inclusion of 47 isotopes of interest even Nuclear Plants for the dose evaluation in skin generated by 'hot particles'. The approach for to add these isotopes is the correlation parameter F and the average energy of the Beta particle, with relationship to those 75 isotopes of the original code. The methodology of the dose calculation of the VARSKIN code is based on the interpolation, (and integration of the interest geometries: punctual or plane sources), of the distribution functions scaled doses in water for beta and electrons punctual sources, tabulated by Berger. Finally a brief discussion of the results for their interpretation and use with purposes of radiological protection (dose insurance in relation to the considered biological effects) is presented

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

    Science.gov (United States)

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

    2016-03-01

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

  20. Radioactive Ion Beam Production by Fast-Neutron-Induced Fission in Actinide Targets at EURISOL

    CERN Document Server

    Herrera-Martínez, Adonai

    The European Isotope Separation On-Line Radioactive Ion Beam Facility (EURISOL) is set to be the 'next-generation' European Isotope Separation On-Line (ISOL) Radioactive Ion Beam (RIB) facility. It will extend and amplify current research on nuclear physics, nuclear astrophysics and fundamental interactions beyond the year 2010. In EURISOL, the production of high-intensity RIBs of specific neutron-rich isotopes is obtained by inducing fission in large-mass actinide targets. In our contribution, the use of uranium targets is shown to be advantageous to other materials, such as thorium. Therefore, in order to produce fissions in U-238 and reduce the plutonium inventory, a fast neutron energy spectrum is necessary. The large beam power required to achieve these RIB levels requires the use of a liquid proton-to-neutron converter. This article details the design parameters of the converter, with special attention to the coupled neutronics of the liquid converter and fission target. Calculations performed with the ...

  1. The electrochemical properties of actinide amalgams

    International Nuclear Information System (INIS)

    Selection of the values of standard potentials of An actinides and their amalgams was made. On the basis of the data obtained energy characteristics of alloy formation processes in the systems An-Hg were calculated and analyzed. It is ascertained that the properties of f-element solutions in mercury are similar to those of alkali and alkaline-earth metal amalgams with the only difference, i.e. in case of active metals of group 3 the number of realized charge value of ionic frames in condensed phase increases

  2. Reply to Nicholson's comment on "Consistent calculation of aquatic gross production from oxygen triple isotope measurements" by Kaiser (2011

    Directory of Open Access Journals (Sweden)

    J. Kaiser

    2012-08-01

    Full Text Available The comment by Nicholson (2011a questions the "consistency" of the "definition" of the "biological end-member" used by Kaiser (2011a in the calculation of oxygen gross production. "Biological end-member" refers to the relative oxygen isotope ratio difference between photosynthetic oxygen and Air-O2 (abbreviated 17δP and 18δP for 17O/16O and 18O/16O, respectively. The comment claims that this leads to an overestimate of the discrepancy between previous studies and that the resulting gross production rates are "30% too high". Nicholson recognises the improved accuracy of Kaiser's direct calculation ("dual-delta" method compared to previous approximate approaches based on 17O excess (17Δ and its simplicity compared to previous iterative calculation methods. Although he correctly points out that differences in the normalised gross production rate (g are largely due to different input parameters used in Kaiser's "base case" and previous studies, he does not acknowledge Kaiser's observation that iterative and dual-delta calculation methods give exactly the same g for the same input parameters (disregarding kinetic isotope fractionation during air-sea exchange. The comment is based on misunderstandings with respect to the "base case" 17δP and 18δP values. Since direct measurements of 17δP and 18δPdo not exist or have been lost, Kaiser constructed the "base case" in a way that was consistent and compatible with literature data. Nicholson showed that an alternative reconstruction of 17δP gives g values closer to previous studies. However, unlike Nicholson, we refrain from interpreting either reconstruction as a benchmark for the accuracy of g. A number of publications over the last 12 months

  3. Actinides, accelerators and erosion

    Science.gov (United States)

    Tims, S. G.; Fifield, L. K.

    2012-10-01

    Fallout isotopes can be used as artificial tracers of soil erosion and sediment accumulation. The most commonly used isotope to date has been 137Cs. Concentrations of 137Cs are, however, significantly lower in the Southern Hemisphere, and furthermore have now declined to 35% of original values due to radioactive decay. As a consequence the future utility of 137Cs is limited in Australia, with many erosion applications becoming untenable within the next 20 years, and there is a need to replace it with another tracer. Plutonium could fill this role, and has the advantages that there were six times as many atoms of Pu as of 137Cs in fallout, and any loss to decay has been negligible due to the long half-lives of the plutonium isotopes. Uranium-236 is another long-lived fallout isotope with significant potential for exploitation as a tracer of soil and sediment movement. Uranium is expected to be more mobile in soils than plutonium (or caesium), and hence the 236U/Pu ratio will vary with soil depth, and so could provide an independent measure of the amount of soil loss. In this paper we discuss accelerator based ultra-sensitive measurements of plutonium and 236U isotopes and their advantages over 137Cs as tracers of soil erosion and sediment movement.

  4. Actinides, accelerators and erosion

    Directory of Open Access Journals (Sweden)

    Fifield L.K.

    2012-10-01

    Full Text Available Fallout isotopes can be used as artificial tracers of soil erosion and sediment accumulation. The most commonly used isotope to date has been 137Cs. Concentrations of 137Cs are, however, significantly lower in the Southern Hemisphere, and furthermore have now declined to 35% of original values due to radioactive decay. As a consequence the future utility of 137Cs is limited in Australia, with many erosion applications becoming untenable within the next 20 years, and there is a need to replace it with another tracer. Plutonium could fill this role, and has the advantages that there were six times as many atoms of Pu as of 137Cs in fallout, and any loss to decay has been negligible due to the long half-lives of the plutonium isotopes. Uranium-236 is another long-lived fallout isotope with significant potential for exploitation as a tracer of soil and sediment movement. Uranium is expected to be more mobile in soils than plutonium (or caesium, and hence the 236U/Pu ratio will vary with soil depth, and so could provide an independent measure of the amount of soil loss. In this paper we discuss accelerator based ultra-sensitive measurements of plutonium and 236U isotopes and their advantages over 137Cs as tracers of soil erosion and sediment movement.

  5. The advanced liquid metal reactor actinide recycle system

    International Nuclear Information System (INIS)

    The current U.S. National Energy Strategy includes four key goals for nuclear policy: enhance safety and design standards, reduce economic risk, reduce regulatory risk, and establish an effective high-level nuclear waste program. The U.S. Department of Energy's Advanced Liquid Metal Reactor Actinide Recycle System is consistent with these objectives. The system has the ability to fulfill multiple missions with the same basic design concept. In addition to providing an option for long-term energy security, the system can be effectively utilized for recycling of actinides in light water reactor (LWR) spent fuel, provide waste management flexibility, including the reduction in the waste quantity and storage time and utilization of the available energy potential of LWR spent fuel. The actinide recycle system is comprised of (1) a compact liquid metal (sodium) cooled reactor system with optimized passive safety characteristics, and (2) pyrometallurgical metal fuel cycle presently under development of Argonne National Laboratory. The waste reduction of LWR spent fuel is accomplished by transmutation or fissioning of the longer-lived transuranic isotopes to shorter-lived fission products in the reactor. In this presentation the economical and environmental incentive of the actinide recycle system is addressed and the status of development including licensing aspects is described. 3 refs., 1 tab., 6 figs

  6. Nuclear data uncertainty analysis on a minor actinide burner for transmuting spent fuel

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hangbok

    1998-08-01

    A comprehensive sensitivity and uncertainty analysis was performed on a 1200 MWt minor actinides burner designed for a low burnup reactivity swing, negative doppler coefficient, and low sodium void worth. Sensitivities of the performance parameters were generated using depletion perturbation methods for the constrained close fuel cycle of the reactor. The uncertainty analysis was performed using the sensitivity and covariance data taken from ENDF-B/V and other published sources. The uncertainty analysis of a liquid metal reactor for burning minor actinide has shown that uncertainties in the nuclear data of several key minor actinide isotopes can introduce large uncertainties in the predicted performance of the core. The relative uncertainties in the burnup swing, doppler coefficient, and void worth were conservatively estimated to be 180 %, 97 %, and 46 %, respectively. An analysis was performed to prioritize the minor actinide reactions for reducing the uncertainties. (author). 41 refs., 17 tabs., 1 fig.

  7. Actinide-Only Burnup Credit for PWR Spent Nuclear Fuel Packages

    International Nuclear Information System (INIS)

    The objective of this topical report is to present to the NRC for review and acceptance a methodology for using burnup credit in the design of criticality control systems for PWR spent fuel transportation packages, while maintaining the criticality safety margins and related requirements of 10 CFR Part 71 and 72. The proposed methodology consists of five major steps as summarized below: (1) Validate a computer code system to calculate isotopic concentrations in SNF created during burnup in the reactor core and subsequent decay. (2) Validate a computer code system to predict the subcritical multiplication factor, keff, of a spent nuclear fuel package. (3) Establish bounding conditions for the isotopic concentration and criticality calculations. (4) Use the validated codes and bounding conditions to generate package loading criteria (burnup credit loading curves). and (5) Verify that SNF assemblies meet the package loading criteria and confirm proper fuel assembly selection prior to loading. (This step is required but the details are outside the scope of this topical report.) When reviewed and accepted by the NRC, this topical report will serve as a criterion document for criticality control analysts and will provide steps for the use of actinide-only burnup credit in the design of criticality control systems. The NRC-accepted burnup credit methodology will be used by commercial SNF storage and transportation package designers. Design-specific burnup credit criticality analyses will be defined, developed, and documented in the Safety Analysis Report (SAR) for each specific storage or transportation package that uses burnup credit. These SARs will then be submitted to the NRC for review and approval. This topical report is expected to be referenced in a number of storage and transportation cask applications to be submitted by commercial cask and canister designers to the NRC. Therefore, NRC acceptance of this topical report will result in increased efficiency of the

  8. Topical Report on Actinide-Only Burnup Credit for PWR Spent Nuclear Fuel Packages. Revision 2

    Energy Technology Data Exchange (ETDEWEB)

    None, None

    1998-09-01

    The objective of this topical report is to present to the NRC for review and acceptance a methodology for using burnup credit in the design of criticality control systems for PWR spent fuel transportation packages, while maintaining the criticality safety margins and related requirements of 10 CFR Part 71 and 72. The proposed methodology consists of five major steps as summarized below: (1) Validate a computer code system to calculate isotopic concentrations in SNF created during burnup in the reactor core and subsequent decay. (2) Validate a computer code system to predict the subcritical multiplication factor, keff, of a spent nuclear fuel package. (3) Establish bounding conditions for the isotopic concentration and criticality calculations. (4) Use the validated codes and bounding conditions to generate package loading criteria (burnup credit loading curves). and (5) Verify that SNF assemblies meet the package loading criteria and confirm proper fuel assembly selection prior to loading. (This step is required but the details are outside the scope of this topical report.) When reviewed and accepted by the NRC, this topical report will serve as a criterion document for criticality control analysts and will provide steps for the use of actinide-only burnup credit in the design of criticality control systems. The NRC-accepted burnup credit methodology will be used by commercial SNF storage and transportation package designers. Design-specific burnup credit criticality analyses will be defined, developed, and documented in the Safety Analysis Report (SAR) for each specific storage or transportation package that uses burnup credit. These SARs will then be submitted to the NRC for review and approval. This topical report is expected to be referenced in a number of storage and transportation cask applications to be submitted by commercial cask and canister designers to the NRC. Therefore, NRC acceptance of this topical report will result in increased efficiency of the

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

    Energy Technology Data Exchange (ETDEWEB)

    Borkowski, Marian; Lucchini, Jean-Francois; Richmann, Michael K.; Reed, Donald T.

    2009-09-01

    The solubility of actinides in the +3 oxidation state is an important input into the Waste Isolation Pilot Plant (WIPP) performance assessment (PA) models that calculate potential actinide release from the WIPP repository. In this context, the solubility of neodymium(III) was determined as a function of pH, carbonate concentration, and WIPP brine composition. Additionally, we conducted a literature review on the solubility of +3 actinides under WIPP-related conditions. Neodymium(III) was used as a redox-invariant analog for the +3 oxidation state of americium and plutonium, which is the oxidation state that accounts for over 90% of the potential release from the WIPP through the dissolved brine release (DBR) mechanism, based on current WIPP performance assessment assumptions. These solubility data extend past studies to brine compositions that are more WIPP-relevant and cover a broader range of experimental conditions than past studies.

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

    OpenAIRE

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

    2014-01-01

    Potential energy surfaces (PES's) of actinide nuclei are characterized by a two-humped barrier structure. At large deformations beyond the second barrier the occurrence of a third one was predicted by Mic-Mac model calculations in the 1970s, but contradictory results were later reported. In this paper, triple-humped barriers in actinide nuclei are investigated with covariant density functional theory (CDFT). Calculations are performed using the multidimensionally-constrained relativistic mean...

  11. Monte Carlo calculations on transmutation of trans-uranic nuclear waste isotopes using spallation neutrons difference of lead and graphite moderators

    CERN Document Server

    Hashemi-Nezhad, S R; Brandt, R; Krivopustov, M I; Kulakov, B A; Odoj, R; Sosnin, A N; Wan, J S; Westmeier, W

    2002-01-01

    Transmutation rates of sup 2 sup 3 sup 9 Pu and some minor actinides ( sup 2 sup 3 sup 7 Np, sup 2 sup 4 sup 1 Am, sup 2 sup 4 sup 5 Cm and sup 2 sup 4 sup 6 Cm), in two accelerator-driven systems (ADS) with lead or graphite moderating environments, were calculated using the LAHET code system. The ADS that were used had a large volume (approx 32 m sup 3) and contained no fissile material, except for a small amount of fissionable waste nuclei that existed in some cases. Calculations were performed at an incident proton energy of 1.5 GeV and the spallation target was lead. Also breeding rates of sup 2 sup 3 sup 9 Pu and sup 2 sup 3 sup 3 U as well as the transmutation rates of two long-lived fission products sup 9 sup 9 Tc and sup 1 sup 2 sup 9 I were calculated at different locations in the moderator. It is shown that an ADS with graphite moderator is a much more effective transmuter than that with lead moderator.

  12. 33rd Actinide Separations Conference

    Energy Technology Data Exchange (ETDEWEB)

    McDonald, L M; Wilk, P A

    2009-05-04

    Welcome to the 33rd Actinide Separations Conference hosted this year by the Lawrence Livermore National Laboratory. This annual conference is centered on the idea of networking and communication with scientists from throughout the United States, Britain, France and Japan who have expertise in nuclear material processing. This conference forum provides an excellent opportunity for bringing together experts in the fields of chemistry, nuclear and chemical engineering, and actinide processing to present and discuss experiences, research results, testing and application of actinide separation processes. The exchange of information that will take place between you, and other subject matter experts from around the nation and across the international boundaries, is a critical tool to assist in solving both national and international problems associated with the processing of nuclear materials used for both defense and energy purposes, as well as for the safe disposition of excess nuclear material. Granlibakken is a dedicated conference facility and training campus that is set up to provide the venue that supports communication between scientists and engineers attending the 33rd Actinide Separations Conference. We believe that you will find that Granlibakken and the Lake Tahoe views provide an atmosphere that is stimulating for fruitful discussions between participants from both government and private industry. We thank the Lawrence Livermore National Laboratory and the United States Department of Energy for their support of this conference. We especially thank you, the participants and subject matter experts, for your involvement in the 33rd Actinide Separations Conference.

  13. A transition cycle strategy to enhance minor actinide burning potential in the pan-shape LMR core

    International Nuclear Information System (INIS)

    This study summarizes the neutronic performances and fuel cycle behaviors of the pan-shape transuranic (TRU) burner core from the initial core through the end of a core life. The cycle-by-cycle evolution of isotopic compositions and neutronics characteristics are compared with those calculated from the analysis of an assumed equilibrium cycle. The amount of burnt TRU per cycle after Cycle 8 turned out to be comparable to that of the equilibrium cycle, while the isotopic compositions and the resulting neutronics performances up to about Cycle 20 have shown considerable deviations from those of the equilibrium cycle. The reference core in this analysis has been designed to meet a target sodium void reactivity at the end of the equilibrium cycle by reducing the active core height. Since the core isotopic loading approaches that of the equilibrium cycle after many cycles of operation, significant margins to the target sodium void reactivity are noted in the early cycles. This finding has led to the loading of concentrated minor actinides (MA) relative to the Pu isotopes in the first three cycles. Thereafter, they are homogeneously self-recycled with the external feed TRU makeup composed of typical LWR discharge TRU compositions. The transition cycle analysis with the higher MA loading reveals that the total MA consumed through 50 cycles of operation is 1.89 times larger than the case for the constant external feed makeup TRU with a typical LWR discharge compositions, without exceeding the sodium void reactivity observed in the equilibrium cycle

  14. Actinides reduction by recycling in a thermal reactor; Reduccion de actinidos por reciclado en un reactor termico

    Energy Technology Data Exchange (ETDEWEB)

    Ramirez S, J. R.; Martinez C, E.; Balboa L, H., E-mail: ramon.ramirez@inin.gob.mx [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico)

    2014-10-15

    This work is directed towards the evaluation of an advanced nuclear fuel cycle in which radioactive actinides could be recycled to remove most of the radioactive material; firstly a production reference of actinides in standard nuclear fuel of uranium at the end of its burning in a BWR reactor is established, after a fuel containing plutonium is modeled to also calculate the actinides production in MOX fuel type. Also it proposes a design of fuel rod containing 6% of actinides in a matrix of uranium from the tails of enrichment, then four standard uranium fuel rods are replaced by actinides rods to evaluate the production and transmutation thereof, the same procedure was performed in the fuel type MOX and the end actinide reduction in the fuel was evaluated. (Author)

  15. Actinide-specific sequestering agents and decontamination applications

    Energy Technology Data Exchange (ETDEWEB)

    Smith, William L. [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials and Molecular Research Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Raymond, Kenneth N. [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials and Molecular Research Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry

    1981-04-07

    With the commercial development of nuclear reactors, the actinides have become very important industrial elements. A major concern of the nuclear industry is the biological hazard associated with nuclear fuels and their wastes. The acute chemical toxicity of tetravalent actinides, as exemplified by Th(IV), is similar to Cr(III) or Al(III). However, the acute toxicity of 239Pu(IV) is similar to strychnine, which is much more toxic than any of the non-radioactive metals such as mercury. Although the more radioactive isotopes of the transuranium elements are more acutely toxic by weight than plutonium, the acute toxicities of 239Pu, 241Am, and 244Cm are nearly identical in radiation dose, ~100 μCi/kg in rodents. Finally and thus, the extreme acute toxicity of 239Pu is attributed to its high specific activity of alpha emission.

  16. Chemistry of lower valent actinide halides

    Energy Technology Data Exchange (ETDEWEB)

    Lau, K.H.; Hildenbrand, D.L.

    1992-01-01

    This research effort was concerned almost entirely with the first two members of the actinide series, thorium and uranium, although the work was later extended to some aspects of the neptunium-fluorine system in a collaborative program with Los Alamos National Laboratory. Detailed information about the lighter actinides will be helpful in modeling the properties of the heavier actinide compounds, which will be much more difficult to study experimentally. In this program, thermochemical information was obtained from high temperature equilibrium measurements made by effusion-beam mass spectrometry and by effusion-pressure techniques. Data were derived primarily from second-law analysis so as to avoid potential errors in third-law calculations resulting from uncertainties in spectroscopic and molecular constants. This approach has the additional advantage of yielding reaction entropies that can be checked for consistency with various molecular constant assignments for the species involved. In the U-F, U-Cl, and U-Br systems, all of the gaseous species UX, UX{sub 2}, UX{sub 3}, UX{sub 4}, and UX{sub 5}, where X represents the halogen, were identified and characterized; the corresponding species ThX, ThX{sub 2}, ThX{sub 3}, and ThX{sub 4} were studied in the Th-F, Th-Cl, and Th-Br systems. A number of oxyhalide species in the systems U-0-F, U-0-Cl, Th-0-F, and Th-O-Cl were studied thermochemically. Additionally, the sublimation thermodynamics of NpF{sub 4}(s) and NpO{sub 2}F{sub 2}(s) were studied by mass spectrometry.

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

    Science.gov (United States)

    Bauder, W.; Pardo, R. C.; Kondev, F. G.; Kondrashev, S.; Nair, C.; Nusair, O.; Palchan, T.; Scott, R.; Seweryniak, D.; Vondrasek, R.; Collon, P.; Paul, M.; Youinou, G.; Salvatores, M.; Palmotti, G.; Berg, J.; Maddock, T.; Imel, G.

    2014-09-01

    The MANTRA (Measurement of Actinide Neutron TRAnsmutations) project will improve energy-integrated neutron capture cross section data across the actinide region. These data are incorporated into nuclear reactor models and are an important piece in understanding Generation IV reactor designs. We will infer the capture cross sections by measuring isotopic ratios from actinide samples, irradiated in the Advanced Test Reactor at INL, with Accelerator Mass Spectrometry (AMS) at ATLAS (ANL). The superior sensitivity of AMS allows us to extract multiple cross sections from a single sample. In order to analyze the large number of samples needed for MANTRA and to meet the goal of extracting multiple cross sections per sample, we have made a number of modifications to the AMS setup at ATLAS. In particular, we are developing a technique to inject solid material into the ECR with laser ablation. With laser ablation, we can better control material injection and potentially increase efficiency in the ECR, thus creating less contamination in the source and reducing cross talk. I will present work on the laser ablation system and preliminary results from our AMS measurements. The MANTRA (Measurement of Actinide Neutron TRAnsmutations) project will improve energy-integrated neutron capture cross section data across the actinide region. These data are incorporated into nuclear reactor models and are an important piece in understanding Generation IV reactor designs. We will infer the capture cross sections by measuring isotopic ratios from actinide samples, irradiated in the Advanced Test Reactor at INL, with Accelerator Mass Spectrometry (AMS) at ATLAS (ANL). The superior sensitivity of AMS allows us to extract multiple cross sections from a single sample. In order to analyze the large number of samples needed for MANTRA and to meet the goal of extracting multiple cross sections per sample, we have made a number of modifications to the AMS setup at ATLAS. In particular, we are

  18. Fabrication of actinide mononitride fuel

    International Nuclear Information System (INIS)

    Fabrication of actinide mononitride fuel in JAERI is summarized. Actinide mononitride and their solid solutions were fabricated by carbothermic reduction of the oxides in N2 or N2-H2 mixed gas stream. Sintering study was also performed for the preparation of pellets for the property measurements and irradiation tests. The products were characterized to be high-purity mononitride with a single phase of NaCl-type structure. Moreover, fuel pins containing uranium-plutonium mixed nitride pellets were fabricated for the irradiation tests in JMTR and JOYO. (author)

  19. Fuel depletion calculation in MTR-LEU NUR reactor

    Directory of Open Access Journals (Sweden)

    Zeggar Foudil

    2008-01-01

    Full Text Available In this article, we present the results of a few energy groups calculations for the NUR reactor fuel depletion analysis up to 45 000 MWd/tU taken as the maximum fuel burn up. The WIMSD-4 cell code has been employed as a calculation tool. In this study, we are interested in actinides such as the uranium and plutonium isotopes, as well as fission products Xe-135, Sm-149, Sm-151, Eu-155, and Gd-157. Calculation results regarding the five energy groups are in a good agreement with those obtained with only two energy groups which can, therefore, be used in all subsequent calculations. Calculation results presented in this article can be used as a microscopic data base for estimating the amount of radioactive sources randomly dispersed in the environment. They can also be used to monitor the fuel assemblies inventory at the core level.

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

    Science.gov (United States)

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

    2015-01-01

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

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

    Science.gov (United States)

    Geckeis, Horst; Rabung, Thomas

    2008-12-12

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

  2. Chemistry of tetravalent actinides phosphates. The thorium phosphate-diphosphate as immobilisation matrix of actinides

    International Nuclear Information System (INIS)

    The author presents in this document its scientific works from 1992 to 2001, in order to obtain the enabling to manage scientific and chemical researches at the university Paris Sud Orsay. The first part gives an abstract of the thesis on the characterizations, lixiviation and synthesis of uranium and thorium based phosphate matrix in the framework of the search for a ceramic material usable in the radioactive waste storage. The second part presents briefly the researches realized at the CEA, devoted to a reliable, independent and accurate measure of some isotopes activity. The last part presents the abstracts of researches activities from 1996 to 2001 on the tetravalent actinides phosphates chemistry, the sintering of PDT and solid solutions of PDTU and the kinetic and thermodynamical studies of the PDT dissolution. Many references and some publication in full text are provided. (A.L.B.)

  3. Environmental research on actinide elements

    Energy Technology Data Exchange (ETDEWEB)

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

    1987-08-01

    The papers synthesize the results of research sponsored by DOE's Office of Health and Environmental Research on the behavior of transuranic and actinide elements in the environment. Separate abstracts have been prepared for the 21 individual papers. (ACR)

  4. Magnetic susceptibility of actinide(iii) cations: an experimental and theoretical study.

    Science.gov (United States)

    Autillo, Matthieu; Guerin, Laetitia; Bolvin, Hélène; Moisy, Philippe; Berthon, Claude

    2016-03-01

    In a previous paper, the influence of radioactive decay (α and β(-)) on magnetic susceptibility measurements by the Evans method has been demonstrated by the study of two americium isotopes. To characterize more accurately this phenomenon and particularly its influence on the Curie law, a new study has been performed on two uranium isotopes ((238)U and (233)U) and on tritiated water ((3)H2O). The results on the influence of α emissions have established a relationship between changes in the temperature dependence and the radioactivity in solution. Regarding the β(-) emissions, less influence was observed while no temperature dependence linked to this kind of radioactive emission could be identified. Once magnetic susceptibility measurements of actinide(iii) cations were corrected from radioactivity effects, methods of quantum chemistry have been used on free ions and aquo complexes to calculate the electronic structure explaining the magnetic properties of Pu(iii), Am(iii) and Cm(iii). The ligand field effect on the magnetic behavior (the Curie constant and temperature-independent susceptibilities) was analyzed by considering different solvation environments. PMID:26864302

  5. New BRC neutron evaluations of actinides with the TALYS code: Modelization and first validation tests

    Directory of Open Access Journals (Sweden)

    Romain P.

    2010-10-01

    Full Text Available The reader may have a look on references [1–3,5] for more details. Over the last five years, new evaluations of plutonium and uranium have been performed at Bruyèeres-le-Châtel (BRC from the resolved resonance region up to 30MeV. Only nuclear reactions models have been used to build these evaluations. Total, shape elastic and direct inelastic cross sections are obtained from a coupled channel model using a dispersive optical potential (BRC, [13] devoted to actinides. All the other cross sections are calculated owing to the Hauser-Fesbach theory (TALYS code [4].We take particular care over the fission channel. For uranium isotopes, a triple-humped barrier [3] is required in order to reproduce accurately the variations of the experimental fission cross sections. As not commonly expected, we show [5] that the effect of the class II or class III states located in the wells of the aforementioned fission barrier provide sometimes an anti-resonant transmission rather than a resonant. With increasing neutron incident energy, a lot of residual nuclei produced by nucleon emission lead to fission also. All available experimental data assigned to the various fission mechanisms of the same nucleus are used to define its fission barrier parameters. As a result of this approach, we are now able to provide consistent evaluations for a large series of isotopes. Of course, our new evaluations have been tested against integral data.

  6. $\\beta$-decay properties for neutron-rich Kr-Tc isotopes from deformed pn-QRPA calculations with realistic forces

    CERN Document Server

    Fang, Dong-Liang; Suzuki, Toshio

    2012-01-01

    In this work we studied $\\beta$-decay properties for deformed neutron-rich nuclei in the region Z=36-43. We use the deformed pn-QRPA methods with the realistic CD-Bonn forces, and include both the Gamow-Teller and first-forbidden types of decays in the calculation. The obtained $\\beta$-decay half-lives and neutron-emission probabilities of deformed isotopes are compared with experiment as well as with previous calculations. The advantages and disadvantages of the method are discussed.

  7. Calculations of the cross sections for synthesis of new {293-296}118 isotopes in {249-252}Cf(48Ca,xn) reactions

    CERN Document Server

    Cap, T; Kowal, M; Wilczynski, J

    2013-01-01

    A project of using a target consisting of the mixture of (249-252)Cf isotopes to be bombarded with the 48Ca beam, aimed to synthesize new isotopes of the heaviest known element Z = 118, is under way at the FLNR in Dubna. In the present work excitation functions for all the reactions: 249Cf(48Ca,xn)(297-x)118, 250Cf(48Ca,xn)(298-x)118, 251Cf(48Ca,xn)(299-x)118 and 252Cf(48Ca,xn)(300-x)118 have been calculated in the framework of the fusion-by-diffusion model, assuming fission barriers, ground-state masses and shell effects of the superheavy nuclei predicted by Kowal et al. Energy dependence of the effective cross sections for the synthesis of selected new isotopes: (293)118, (294)118, (295)118 and (296)118 is predicted for the particular isotopic composition of the Cf target prepared for the Dubna experiment.

  8. Actinides How well do we know their stellar production?

    CERN Document Server

    Goriely, S

    2001-01-01

    The reliable evaluation of the r-process production of the actinides and careful estimates of the uncertainties affecting these predictions are key ingredients especially in nucleo-cosmochronology studies based on the analysis of very metal-poor stars or on the composition of meteorites. This type of information is also required in order to make the best possible use of future high precision data on the actinide composition of galactic cosmic rays, of the local interstellar medium, or of meteoritic grains of presumed circumstellar origin. This paper provides the practitioners in these various fields with the most detailed and careful analysis of the r-process actinide production available to-date. In total, thirty-two different multi-event canonical calculations using different nuclear ingredients or astrophysics conditions are presented, and are considered to give a fair picture of the level of reliability of the predictions of the actinide production, at least in the framework of a simple r-process model. T...

  9. Toward laser ablation Accelerator Mass Spectrometry of actinides

    Science.gov (United States)

    Pardo, R. C.; Kondev, F. G.; Kondrashev, S.; Nair, C.; Palchan, T.; Scott, R.; Seweryniak, D.; Vondrasek, R.; Paul, M.; Collon, P.; Deibel, C.; Youinou, G.; Salvatores, M.; Palmotti, G.; Berg, J.; Fonnesbeck, J.; Imel, G.

    2013-01-01

    A project to measure neutron capture cross sections of a number of actinides in a reactor environment by Accelerator Mass Spectrometry (AMS) at the ATLAS facility of Argonne National Laboratory is underway. This project will require the precise and accurate measurement of produced actinide isotopes in many (>30) samples irradiated in the Advanced Test Reactor at Idaho National Laboratory with neutron fluxes having different energy distributions. The AMS technique at ATLAS is based on production of highly-charged positive ions in an electron cyclotron resonance (ECR) ion source followed by acceleration in the ATLAS linac and mass-to-charge (m/q) measurement at the focus of the Fragment Mass Analyzer. Laser ablation was selected as the method of feeding the actinide material into the ion source because we expect it will have higher efficiency and lower chamber contamination than either the oven or sputtering techniques, because of a much narrower angular distribution of emitted material. In addition, a new multi-sample holder/changer to allow quick change between samples and a computer-controlled routine allowing fast tuning of the accelerator for different beams, are being developed. An initial test run studying backgrounds, detector response, and accelerator scaling repeatability was conducted in December 2010. The project design, schedule, and results of the initial test run to study backgrounds are discussed.

  10. Value of 236U to actinide-only burnup credit

    International Nuclear Information System (INIS)

    The US Department of Energy (DOE) submitted a topical report to the US Nuclear Regulatory Commission (NRC) in May 1995 in order to gain approval of a method for criticality analysis of transport packages that takes account for the change in actinide isotopes with burnup [pressurized water reactors (PWRs) only]. Historically, the NRC has conservatively assumed that the fuel was in its initial conditions (without any burnable absorbers). In order to permit credit for the changes in actinide content, the NRC has required validation of the depletion and criticality codes for spent nuclear fuel, justification of conservative depletion modeling, and finally confirmation measurements before loading. The NRC requested additional information on March 22, 1996. The DOE responded by a revision of the topical report in May 1997. The NRC again responded with another set of requests of additional information in April 1998. In that set of questions, the NRC challenged the use of 236U in burnup credit. Uranium-236 is not found in any significant amount in any available critical experiments. The authors explore the value of 236U to actinide-only burnup credit

  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. Possibility of fusion power reactor to transmute minor actinides of spent nuclear fuel

    Energy Technology Data Exchange (ETDEWEB)

    Serikov, A. E-mail: serikov@nfi.kiae.ru; Shatalov, G.; Sheludjakov, S.; Shpansky, Yu.; Vasiliev, N

    2002-12-01

    A possibility to use fusion power reactor (FPR) is considered for burning long-life elements of spent nuclear fuel in parallel with energy production. In this study a principal design of FPR blanket was examined for transmutation of long-life minor actinides (Np, Am, Cm). A production of minor actinide isotopes is equal to 20-30 kg/1 GW{sub (e)} year for now operating fission reactors, and their amounts will rise with the expected growth of fission reactor power. These isotopes have long-life time and can be dangerous in big amounts in future. Plutonium isotopes are not included in an assumption that they will be used in fission reactors. The major goals of the study were to determine FPR blanket composition corresponding to fast transmutation rate of actinides and tritium self-supply simultaneously. Tritium breeding ratio (TBR) was obtained at level 1.11 for water cooling and reached up 1.56 in variant with helium-cooled assemblies with Np nitride. It was concluded that rows with actinides from processed waste fuel should be arranged near the plasma first wall. Advantages of helium above water cooling are observed in the twice-increased loading of waste fissionable materials and essential increase of achievable TBR. Burnout of Np, Am, Cm would remain at a level {approx}40-50% after 4 full power years.

  13. Simultaneous Evaluation of Fission Cross Sections for Cm Isotopes

    Directory of Open Access Journals (Sweden)

    Lee Y.-O.

    2010-03-01

    Full Text Available Fission Cross Sections for a complete set of Cm-isotopes, 240-250Cm, have been calculated in the incident energy range from above resonance region to 20 MeV. This work aims at providing the fission cross sections with consistent set of model parameters for Cm isotopes, as a part of a complete evaluation including covariance files for several minor actinides which play a great role in the Advanced Fuel Cycle (AFC design and applications as well as the design of new generation of nuclear reactors (GEN-IV. This was accomplished by means of computational analyses carried out with the nuclear model code EMPIRE-2.19 which is the modular system of nuclear reaction codes. A Fission model of this work took into account transmission derived in the WKB approximation within an optical model through a double-humped fission barrier.

  14. Quantum instanton calculation of rate constant for CH4 + OH → CH3 + H2O reaction: Torsional anharmonicity and kinetic isotope effect

    Science.gov (United States)

    Wang, Wenji; Zhao, Yi

    2012-12-01

    Thermal rate constants for the title reaction are calculated by using the quantum instanton approximation within the full dimensional Cartesian coordinates. The results reveal that the quantum effect is remarkable for the reaction at both low and high temperatures, and the obtained rates are in good agreement with experimental measurements at high temperatures. Compared to the harmonic approximation, the torsional anharmonic effect of the internal rotation has a little influence on the rates at low temperatures, however, it enhances the rate by about 20% at 1000 K. In addition, the free energy barriers for the isotopic reactions and the temperature dependence of kinetic isotope effects are also investigated. Generally speaking, for the title reaction, the replacement of OH with OD will reduce the free energy barrier, while substituting D for H (connected to C) will increase the free energy barrier.

  15. Molecular Characterization of Actinide Oxocations from Protactinium to Plutonium

    International Nuclear Information System (INIS)

    This presentation addresses the structural characterization by EXAFS of actinide cations at oxidation states (V) and (VI) as one walks across the periodic table from Z = 91 (protactinium) to Z = 94 (plutonium). A structural comparison between Pa, U, Np and Pu oxocations in aqueous solution at formal oxidation states (V) and (VI) is carried out. These results are corroborated by quantum chemical and molecular dynamics calculations

  16. Molecular Characterization of Actinide Oxocations from Protactinium to Plutonium

    Science.gov (United States)

    Den Auwer, C.; Guilbaud, P.; Guillaumont, D.; Moisy, P.; Digandomenico, V.; Le Naour, C.; Trubert, D.; Simoni, E.; Hennig, C.; Scheinost, A.; Conradson, S. D.

    2007-02-01

    This presentation addresses the structural characterization by EXAFS of actinide cations at oxidation states (V) and (VI) as one walks across the periodic table from Z = 91 (protactinium) to Z = 94 (plutonium). A structural comparison between Pa, U, Np and Pu oxocations in aqueous solution at formal oxidation states (V) and (VI) is carried out. These results are corroborated by quantum chemical and molecular dynamics calculations.

  17. Actinide chemistry in ionic liquids.

    Science.gov (United States)

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

    2013-04-01

    This Forum Article provides an overview of the reported studies on the actinide chemistry in ionic liquids (ILs) with a particular focus on several fundamental chemical aspects: (i) complex formation, (ii) electrochemistry, and (iii) extraction behavior. The majority of investigations have been dedicated to uranium, especially for the 6+ oxidation state (UO2(2+)), because the chemistry of uranium in ordinary solvents has been well investigated and uranium is the most abundant element in the actual nuclear fuel cycles. Other actinides such as thorium, neptunium, plutonium, americium, and curiumm, although less studied, are also of importance in fully understanding the nuclear fuel engineering process and the safe geological disposal of radioactive wastes. PMID:22873132

  18. Actinide recovery techniques utilizing electromechanical processes

    International Nuclear Information System (INIS)

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

  19. Actinide Waste Forms and Radiation Effects

    Science.gov (United States)

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

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

  20. The Multi MegaWatt target station of EURISOL: High Power deposition on the spallation and the actinides targets (SATIF9)

    CERN Document Server

    Kharoua, C

    This presentation will present some of the greatest challenges in the design of this high power spallation sources with a special attention on the high power densities, entailing large structural stresses, and the heat removal, requiring detailed thermo-hydraulics calculations. Alternatively, a windowless target configuration has been proposed, based on a liquid mercury transverse film design. With this design, higher power densities and fission rates may be achieved, also avoiding the technical issues related to the beam window. In the second part of this presentation a brief summary of the actinide targets will be presented. The thermal simulations as well as the fission rates and isotopes production simulation are important calculation to evaluate the capability of the Multi-Megawatt target station.

  1. Benchmark of SCALE (SAS2H) isotopic predictions of depletion analyses for San Onofre PWR MOX fuel

    Energy Technology Data Exchange (ETDEWEB)

    Hermann, O.W.

    2000-02-01

    The isotopic composition of mixed-oxide (MOX) fuel, fabricated with both uranium and plutonium, after discharge from reactors is of significant interest to the Fissile Materials Disposition Program. The validation of the SCALE (SAS2H) depletion code for use in the prediction of isotopic compositions of MOX fuel, similar to previous validation studies on uranium-only fueled reactors, has corresponding significance. The EEI-Westinghouse Plutonium Recycle Demonstration Program examined the use of MOX fuel in the San Onofre PWR, Unit 1, during cycles 2 and 3. Isotopic analyses of the MOX spent fuel were conducted on 13 actinides and {sup 148}Nd by either mass or alpha spectrometry. Six fuel pellet samples were taken from four different fuel pins of an irradiated MOX assembly. The measured actinide inventories from those samples has been used to benchmark SAS2H for MOX fuel applications. The average percentage differences in the code results compared with the measurement were {minus}0.9% for {sup 235}U and 5.2% for {sup 239}Pu. The differences for most of the isotopes were significantly larger than in the cases for uranium-only fueled reactors. In general, comparisons of code results with alpha spectrometer data had extreme differences, although the differences in the calculations compared with mass spectrometer analyses were not extremely larger than that of uranium-only fueled reactors. This benchmark study should be useful in estimating uncertainties of inventory, criticality and dose calculations of MOX spent fuel.

  2. Long-term plant availability of actinides

    International Nuclear Information System (INIS)

    Environmental releases of actinide elements raise issues about which data are very limited. Quantitative information is required to assess the long-term behavior of actinides and their potential hazards resulting from the transport through food chains leading to man. Of special interest is the effect of time on the changes in the availability of actinide elements for uptake by plants from soil. This study provides valuable information on the effects of weathering and aging on the uptake of actinides from soil by range and crop plants grown under realistic field conditions

  3. Chemistry of actinides and fission products

    International Nuclear Information System (INIS)

    This task is concerned primarily with the fundamental chemistry of the actinide and fission product elements. Special efforts are made to develop research programs in collaboration with researchers at universities and in industry who have need of national laboratory facilities. Specific areas currently under investigation include: (1) spectroscopy and photochemistry of actinides in low-temperature matrices; (2) small-angle scattering studies of hydrous actinide and fission product polymers in aqueous and nonaqueous solvents; (3) kinetic and thermodynamic studies of complexation reactions in aqueous and nonaqueous solutions; and (4) the development of inorganic ion exchange materials for actinide and lanthanide separations. Recent results from work in these areas are summarized here

  4. Determination of long-lived actinides in soil leachates by inductively coupled plasma: Mass spectrometry

    International Nuclear Information System (INIS)

    Inductively coupled plasma -- mass spectrometry (ICP-MS) was used to concurrently determine multiple long-lived (t1/2 > 104 y) actinide isotopes in soil samples. Ultrasonic nebulization was found to maximize instrument sensitivity. Instrument detection limits for actinides in solution ranged from 50 mBq L-1 (239Pu) to 2 μBq L-1 (235U) Hydride adducts of 232Th and 238U interfered with the determinations of 233U and 239 Pu; thus, extraction chromatography was, used to eliminate the sample matrix, concentrate the analytes, and separate uranium from the other actinides. Alpha spectrometric determinations of 230Th, 239Pu, and the 234U/238U activity ratio in soil leachates compared well with ICP-MS determinations; however, there were some small systematic differences (ca. 10%) between ICP-MS and a-spectrometric determinations of 234U and 238U activities

  5. The uncertainty analysis of a liquid metal reactor for burning minor actinides from light water reactors

    Energy Technology Data Exchange (ETDEWEB)

    Choi, Hang Bok [Korea Atomic Energy Research Institute, Taejon (Korea, Republic of)

    1998-12-31

    The neutronics analysis of a liquid metal reactor for burning minor actinides has shown that uncertainties in the nuclear data of several key minor actinide isotopes can introduce large uncertainties in the predicted performance of the core. A comprehensive sensitivity and uncertainty analysis was performed on a 1200 MWth actinide burner designed for a low burnup reactivity swing, negative doppler coefficient, and low sodium void worth. Sensitivities were generated using depletion perturbation methods for the equilibrium cycle of the reactor and covariance data was taken ENDF-B/V and other published sources. The relative uncertainties in the burnup swing, doppler coefficient, and void worth were conservatively estimated to be 180%, 97%, and 46%, respectively. 5 refs., 1 fig., 3 tabs. (Author)

  6. Updated multi-group cross sections of minor actinides with improved resonance treatment

    International Nuclear Information System (INIS)

    The study of minor actinide in transmutation reactors and other future applications makes resonance self-shielding treatment a significant issue for criticality and isotope depletion. Resonance treatment for minor actinides has been carried out by subgroup method with improved interference effect through interference correction. Subgroup data was generated using RMET21 and GENP codes along with multi-group cross section data by NJOY nuclear data processing system. Updated multi-group cross section data library for a neutron transport code nTRACER was compared with solutions from MCNPX. The resonance interaction of uranium with minor actinides has been included by modified interference treatment of interference correction in subgroup methodology. The comparison of cross sections and multiplication factor in pin and assembly problems showed significant improvement from systematic resonance treatment especially for 237Np and 243Am. (author)

  7. Standard practice for alternate actinide calibration for inductively coupled plasma-mass spectrometry

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2004-01-01

    1.1 This practice provides guidance for an alternate linear calibration for the determination of selected actinide isotopes in appropriately prepared aqueous solutions by Inductively Coupled Plasma-Mass Spectrometry (ICP-MS). This alternate calibration is mass bias adjusted using thorium-232 (232Th) and uranium-238 (238U) standards. One of the benefits of this standard practice is the ability to calibrate for the analysis of highly radioactive actinides using calibration standards at much lower specific activities. Environmental laboratories may find this standard practice useful if facilities are not available to handle the highly radioactive standards of the individual actinides of interest. 1.2 The instrument response for a series of determinations of known concentration of 232Th and 238U defines the mass versus response relationship. For each standard concentration, the slope of the line defined by 232Th and 238U is used to derive linear calibration curves for each mass of interest using interference equ...

  8. Actinide-only burnup credit for spent fuel transport

    International Nuclear Information System (INIS)

    A conservative methodology is described that would allow taking credit for burn up in the criticality safety analysis of spent nuclear fuel packages. Requirements for its implementation include isotopic and criticality validation, generation of package loading criteria using limiting parameters, and assembly burn up verification by measurement. The method allows credit for the changes in the 234U, 235U, 236U, 238U, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, and 241Am concentrations with burnup. No credit for fission product neutron absorbers is taken. Analyses are included regarding the methodology's financial benefits and conservative margin. It is estimated that the proposed actinide-only burnup credit methodology would save 20% of the transport costs. Nevertheless, the methodology includes a substantial margin. Conservatism due to the isotopic correction factors, limiting modelling parameters, limiting axial profiles and exclusion of the fission products ranges from 10 to 25% k. (author)

  9. Recent Improvements at CEA on Trace Analysis of Actinides in Environmental Samples

    International Nuclear Information System (INIS)

    In this paper, we present some results of R and D works conducted at CEA to improve on the one side the performance of the techniques already in use for detection of undeclared activities, and on the other side to develop new capabilities, either as alternative to the existing techniques or new methods that bring new information, complementary to the isotopic composition. For the trace analysis of plutonium in swipe samples by ICP-MS, we demonstrate that a thorough knowledge of the background in the actinide mass range is highly desirable. In order to avoid false plutonium detection in the femtogram range, correction from polyatomic interferences including mercury, lead or iridium atoms are in some case necessary. Efforts must be put on improving the purification procedure. Micro-Raman spectrometry allows determining the chemical composition of uranium compound at the scale of the microscopic object using a pre-location of the particles thanks to SEM and a relocation of these particles thanks to mathematical calculations. However, particles below 5 μm are hardly relocated and a coupling device between the SEM and the micro-Raman spectrometer for direct Raman analysis after location of a particle of interest is currently under testing. Lastly, laser ablation - ICP-MS is an interesting technique for direct isotopic or elemental analysis of various solid samples and proves to be a suitable alternative technique for particle analysis, although precision over isotopic ratio measurement is strongly limited by the short duration and irregularity of the signals. However, sensitivity and sample throughput are high and more developments are in progress to validate and improve this method. (author)

  10. Recent Improvements of Actinides Trace Analysis in Environmental Samples for Nuclear Activities Detection

    International Nuclear Information System (INIS)

    In this paper, we present some results of R and D works conducted at CEA to improve on the one side the performance of the techniques already in use for detection of undeclared activities, and on the other side to develop new capabilities, either as alternative to the existing techniques or new methods that bring new information, complementary to the isotopic composition. For the trace analysis of plutonium in swipe samples by ICP-MS, we demonstrate that a thorough knowledge of the background in the actinide mass range is highly desirable. In order to avoid false plutonium detection in the femtogram range, correction from polyatomic interferences including mercury, lead or iridium atoms are in some case necessary. Efforts must be put on improving the purification procedure. Micro-Raman spectrometry allows determining the chemical composition of uranium compound at the scale of the microscopic object using a pre-location of the particles thanks to SEM and a relocation of these particles thanks to mathematical calculations. However, particles below 5 μm are hardly relocated and a coupling device between the SEM and the micro-Raman spectrometer for direct Raman analysis after location of a particle of interest is currently under testing. Lastly, laser ablation - ICP-MS is an interesting technique for direct isotopic or elemental analysis of various solid samples and proves to be a suitable alternative technique for particle analysis, although precision over isotopic ratio measurement is strongly limited by the short duration and irregularity of the signals. However, sensitivity and sample throughput are high and more developments are in progress to validate and improve this method. (author)

  11. Study on burn-up credit and minor actinide in post-irradiation analysis

    International Nuclear Information System (INIS)

    Accuracy of burnup calculation for actinide is very important as to the study of burn-up credit. For minor-actinides such as Am243 and Cm244, however, typical burnup calculation codes are not accurate enough. The accuracy for both nuclides was studied by using the SWAT code. The study showed that the C/E values of both nuclides could be improved at the same time by changing the cross section of Pu242. A study of burnup calculation related to the cross section of Pu242 should be performed to improve the accuracy for both nuclides. (author)

  12. Studies of actinides in a superanoxic fjord

    Energy Technology Data Exchange (ETDEWEB)

    Roos, P.

    1997-04-01

    Water column and sediment profiles of Pu, Am, Th and U have been obtained in the superanoxic Framvaren fjord, southern Norway. The concentration of bomb test fallout Pu, Am as well as `dissolved` Th in the bottom water are the highest recorded in the marine environment. The behaviour of the actinides in the anoxic water mass is to a large extent governed by the behaviour of the colloidal material. Ultrafiltration reveals that 40-60% of the actinides are associated to the large colloids, surprisingly this is valid also for U. The sediment acts as a source for Pu, Am, and Th to the water column but primarily as a sink for U. The remobilization of Pu, Am and Th is evident from the water column profiles which have similar diffusion shape profiles as other constituents originating from the sediments. The vertical eddy diffusion coefficient calculated from the Pu profile is in the same order of magnitude as reported from the H{sub 2}S profile. Decreased bottom water concentrations (but a constant water column inventory) between 1989 and 1995 as well as pore water Pu concentrations nearly identical to the overlaying bottom water indicates that the present Pu flux from the sediments are low. Contrary to Pu and Am, the water column Th inventory ({sup 232}Th and {sup 230}Th) continues to increase. The flux of {sup 232}Th from the sediments was determined from changes in water column inventory between 1989 and 1995 and from a pore water profile to be in the order of 2-8 Bq/m{sup 2}/y. 208 refs.

  13. Optimisation and application of ICP-MS and alpha-spectrometry for determination of isotopic ratios of depleted uranium and plutonium in samples collected in Kosovo

    OpenAIRE

    Boulyga, S. F.; Testa, C; Desideri, D.; Becker, J. S.

    2001-01-01

    The determination of environmental contamination with natural and artificial actinide isotopes and evaluation of their source requires precise isotopic determination of actinides, above all uranium and plutonium. This can be achieved by alpha spectrometry or by inductively coupled plasma mass spectrometry (ICP-MS) after chemical separation of actinides. The performance of a sector-field ICP-MS (ICP-SFMS) coupled to a low-flow micronebulizer with a membrane desolvation unit, "Aridus'', was stu...

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

    Science.gov (United States)

    Goriely, S.; Arnould, M.

    2001-12-01

    The reliable evaluation of the r-process production of the actinides and careful estimates of the uncertainties affecting these predictions are key ingredients especially in nucleo-cosmochronology studies based on the analysis of very metal-poor stars or on the composition of meteorites. This type of information is also required in order to make the best possible use of future high precision data on the actinide composition of galactic cosmic rays, of the local interstellar medium, or of meteoritic grains of presumed circumstellar origin. This paper provides the practitioners in these various fields with the most detailed and careful analysis of the r-process actinide production available to-date. This study is based on a version of the multi-event canonical model of the r-process which discards the largely used waiting point approximation. It considers also different combinations of models for the calculation of nuclear masses, beta -decay and fission rates. Two variants of the model used to predict nuclear reaction rates are adopted. In addition, the influence of the level of Pb and Bi production by the r-process on the estimated actinide production is evaluated by relying on the solar abundances of these two elements. In total, thirty-two different cases are presented, and are considered to give a fair picture of the level of reliability of the predictions of the actinide production, at least in the framework of a simple r-process model. This simplicity is imposed by our inability to identify the proper astrophysical sites for the r-process. As a guide to the practitioners, constraints on the actinide yield predictions and associated uncertainties are suggested on grounds of the measured abundances of r-nuclides, including Th and U, in the star CS 31082-001, and under the critical and questionable assumption of the ``universality'' of the r-process. We also define alternative constraints based on the nucleo-cosmochronological results derived from the present

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

    International Nuclear Information System (INIS)

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Petrov, B. Y.; Kuijper, J. C.; Oppe, J.; De Haas, J. B. M. [Nuclear Research and Consultancy Group, Westerduinweg 3, 1755 ZG Petten (Netherlands)

    2012-07-01

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

  17. Gas core reactors for actinide transmutation and breeder applications. Annual report

    International Nuclear Information System (INIS)

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

  18. Molecular cluster theory of chemical bonding in actinide oxide

    International Nuclear Information System (INIS)

    The electronic structure of actinide monoxides AcO and dioxides AcO2, where Ac = Th, U, Np, Pu, Am, Cm and Bk has been studied by molecular cluster methods based on the first-principles one-electron local density theory. Molecular orbitals for nearest neighbor clusters AcO10-6 and AcO12-8 representative of monoxide and dioxide lattices were obtained using non-relativistic spin-restricted and spin-polarized Hartree-Fock-Slater models for the entire series. Fully relativistic Dirac-Slater calculations were performed for ThO, UO and NpO in order to explore magnitude of spin-orbit splittings and level shifts in valence structure. Self-consistent iterations were carried out for NpO, in which the NpO6 cluster was embedded in the molecular field of the solid. Finally, a ''moment polarized'' model which combines both spin-polarization and relativistic effects in a consistent fashion was applied to the NpO system. Covalent mixing of oxygen 2p and Ac 5f orbitals was found to increase rapidly across the actinide series; metal s,p,d covalency was found to be nearly constant. Mulliken atomic population analysis of cluster eigenvectors shows that free-ion crystal field models are unreliable, except for the light actinides. X-ray photoelectron line shapes have been calculated and are found to compare rather well with experimental data on the dioxides

  19. Trace analysis of actinides in the environment using resonance ionization mass spectrometry

    International Nuclear Information System (INIS)

    In this work the resonant ionization of neutral atoms using laser radiation was applied and optimized for ultra-trace analysis of the actinides thorium, uranium, neptunium and plutonium. The sensitive detection of these actinides is a challange for the monitoring and quantification of radioactive releases from nuclear facilities. Using resonance ionization spectroscopy combined with a newly developed quadrupole-mass-spectrometer, numerous energy levels in the atomic structure of these actinides could be identified. With this knowledge efficient excitation schemes for the mentioned actinides could be identified and characterised. The applied in-source-ionization ensures for a high detection efficiency due to the good overlap of laser radiation with the atomic beam and allows therefore for a low sample consumption which is required for the analysis of radio nuclides. The selective excitation processes in the resonant ionization method supresses unwanted contaminations and was optimized for analytical detection of ultra-trace amounts in environmental samples as well as for determination of isotopic compositions. The efficient in-source-ionization combined with high power pulsed laser radiation allows for detections efficiency up to 1%. For plutonium detection limits in the range of 104-105 atoms could be demonstrated for synthetic samples as well as for first environmental samples. The usage of narrow bandwidth continuous wave lasers in combination with a transversal overlap of the laser radiation and the free propagating atomic beam enable for resolving individual isotopic shifts of the resonant transitions. This results in a high selectivity against dominant neighboring isotopes but with a significant loss in detection efficiency. For the ultra-trace isotope 236U a detection limit down to 10-9 for the isotope ratio N (236U)/N (238U) could be determined.

  20. Reactor Fuel Isotopics and Code Validation for Nuclear Applications

    Energy Technology Data Exchange (ETDEWEB)

    Francis, Matthew W. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Weber, Charles F. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Pigni, Marco T. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Gauld, Ian C. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

    2015-02-01

    Experimentally measured isotopic concentrations of well characterized spent nuclear fuel (SNF) samples have been collected and analyzed by previous researchers. These sets of experimental data have been used extensively to validate the accuracy of depletion code predictions for given sets of burnups, initial enrichments, and varying power histories for different reactor types. The purpose of this report is to present the diversity of data in a concise manner and summarize the current accuracy of depletion modeling. All calculations performed for this report were done using the Oak Ridge Isotope GENeration (ORIGEN) code, an internationally used irradiation and decay code solver within the SCALE comprehensive modeling and simulation code. The diversity of data given in this report includes key actinides, stable fission products, and radioactive fission products. In general, when using the current ENDF/B-VII.0 nuclear data libraries in SCALE, the major actinides are predicted to within 5% of the measured values. Large improvements were seen for several of the curium isotopes when using improved cross section data found in evaluated nuclear data file ENDF/B-VII.0 as compared to ENDF/B-V-based results. The impact of the flux spectrum on the plutonium isotope concentrations as a function of burnup was also shown. The general accuracy noted for the actinide samples for reactor types with burnups greater than 5,000 MWd/MTU was not observed for the low-burnup Hanford B samples. More work is needed in understanding these large discrepancies. The stable neodymium and samarium isotopes were predicted to within a few percent of the measured values. Large improvements were seen in prediction for a few of the samarium isotopes when using the ENDF/B-VII.0 libraries compared to results obtained with ENDF/B-V libraries. Very accurate predictions were obtained for 133Cs and 153Eu. However, the predicted values for the stable ruthenium and rhodium isotopes varied

  1. PAPIN: A Fortran-IV program to calculate cross section probability tables, Bondarenko and transmission self-shielding factors for fertile isotopes in the unresolved resonance region

    Energy Technology Data Exchange (ETDEWEB)

    Munoz-Cobos, J.G.

    1981-08-01

    The Fortran IV code PAPIN has been developed to calculate cross section probability tables, Bondarenko self-shielding factors and average self-indication ratios for non-fissile isotopes, below the inelastic threshold, on the basis of the ENDF/B prescriptions for the unresolved resonance region. Monte-Carlo methods are utilized to generate ladders of resonance parameters in the unresolved resonance region, from average resonance parameters and their appropriate distribution functions. The neutron cross-sections are calculated by the single level Breit-Wigner (SLBW) formalism, with s, p and d-wave contributions. The cross section probability tables are constructed by sampling the Doppler-broadened cross sections. The various self-shielded factors are computed numerically as Lebesgue integrals over the cross section probability tables. The program PAPIN has been validated through extensive comparisons with several deterministic codes.

  2. Spin and orbital moments in actinide compounds

    DEFF Research Database (Denmark)

    Lebech, B.; Wulff, M.; Lander, G.H.

    1991-01-01

    experiments designed to determine the magnetic moments at the actinide and transition-metal sublattice sites in compounds such as UFe2, NpCo2, and PuFe2 and to separate the spin and orbital components at the actinide sites. The results show, indeed, that the ratio of the orbital to spin moment is reduced...

  3. Prompt fission neutron spectrum of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Capote, R. [International Atomic Energy Agency, Vienna (Austria); Chen, Y. -J. [China Institute of Atomic Energy, Beijing (China); Hambsch, F. J. [European Commission, Joint Research Centre - IRRM, Geel (Belgium); Jurado, B. [CENBG, CNRS/IN2P3, Gradignan (France); Kornilov, N. [Ohio Univ., Athens, OH (United States); Lestone, J. P. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Litaize, O. [CEA, DEN, DER, SPRC, Saint-Paul-Lez-Durance (France); Morillon, B. [CEA, DAM, DIF, Arpajon (France); Neudecker, D. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Oberstedt, S. [European Commission, Joint Research Centre - IRRM, Geel (Belgium); Ohsawa, T. [Kinki Univ., Osaka-fu (Japan); Otuka, N. [International Atomic Energy Agency, Vienna (Austria); Pronyaev, V. G. [Institute of Physics and Power Engineering, Obninsk (Russian Federation); Saxena, A. [Bhabha Atomic Research Centre, Mumbai (India); Schmidt, K. H. [CENBG, CNRS/IN2P3, Gradignan (France); Serot, O. [CEA, DEN, DER, SPRC, Saint-Paul-Lez-Durance (France); Shcherbakov, O. A. [Petersburg Nuclear Physics Institute of NRC " Kurchatov Institute" , Gatchina (Russian Federation); Shu, N. -C. [China Institute of Atomic Energy, Beijing (China); Smith, D. L. [Argonne National Lab. (ANL), Argonne, IL (United States); Talou, P. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Trkov, A. [International Atomic Energy Agency, Vienna (Austria); Tudora, A. C. [Univ. of Bucharest, Magurele (Romania); Vogt, R. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Univ. of California, Davis, CA (United States); Vorobyev, A. S. [Petersburg Nuclear Physics Institute of NRC " Kurchatov Institute" , Gatchina (Russian Federation)

    2016-01-06

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

  4. Isotope shifts of the three lowest 1S states of the B+ ion calculated with a finite-nuclear-mass approach and with relativistic and quantum electrodynamics corrections

    Science.gov (United States)

    Bubin, Sergiy; Komasa, Jacek; Stanke, Monika; Adamowicz, Ludwik

    2010-03-01

    We present very accurate quantum mechanical calculations of the three lowest S-states [1s22s2(S10), 1s22p2(S10), and 1s22s3s(S10)] of the two stable isotopes of the boron ion, B10+ and B11+. At the nonrelativistic level the calculations have been performed with the Hamiltonian that explicitly includes the finite mass of the nucleus as it was obtained by a rigorous separation of the center-of-mass motion from the laboratory frame Hamiltonian. The spatial part of the nonrelativistic wave function for each state was expanded in terms of 10 000 all-electron explicitly correlated Gaussian functions. The nonlinear parameters of the Gaussians were variationally optimized using a procedure involving the analytical energy gradient determined with respect to the nonlinear parameters. The nonrelativistic wave functions of the three states were subsequently used to calculate the leading α2 relativistic corrections (α is the fine structure constant; α =1/c, where c is the speed of light) and the α3 quantum electrodynamics (QED) correction. We also estimated the α4 QED correction by calculating its dominant component. A comparison of the experimental transition frequencies with the frequencies obtained based on the energies calculated in this work shows an excellent agreement. The discrepancy is smaller than 0.4 cm-1.

  5. Isotope shifts of the three lowest 1S states of the B+ ion calculated with a finite-nuclear-mass approach and with relativistic and quantum electrodynamics corrections.

    Science.gov (United States)

    Bubin, Sergiy; Komasa, Jacek; Stanke, Monika; Adamowicz, Ludwik

    2010-03-21

    We present very accurate quantum mechanical calculations of the three lowest S-states [1s(2)2s(2)((1)S(0)), 1s(2)2p(2)((1)S(0)), and 1s(2)2s3s((1)S(0))] of the two stable isotopes of the boron ion, (10)B(+) and (11)B(+). At the nonrelativistic level the calculations have been performed with the Hamiltonian that explicitly includes the finite mass of the nucleus as it was obtained by a rigorous separation of the center-of-mass motion from the laboratory frame Hamiltonian. The spatial part of the nonrelativistic wave function for each state was expanded in terms of 10,000 all-electron explicitly correlated Gaussian functions. The nonlinear parameters of the Gaussians were variationally optimized using a procedure involving the analytical energy gradient determined with respect to the nonlinear parameters. The nonrelativistic wave functions of the three states were subsequently used to calculate the leading alpha(2) relativistic corrections (alpha is the fine structure constant; alpha=1/c, where c is the speed of light) and the alpha(3) quantum electrodynamics (QED) correction. We also estimated the alpha(4) QED correction by calculating its dominant component. A comparison of the experimental transition frequencies with the frequencies obtained based on the energies calculated in this work shows an excellent agreement. The discrepancy is smaller than 0.4 cm(-1).

  6. Covariance evaluation for actinide nuclear data in JENDL-4

    International Nuclear Information System (INIS)

    Full text: The JENDL-4.0 was released in March 2010. It provides neutron nuclear data for 79 actinides from Ac to Fm. All of the actinides include covariance data. The covariance data were evaluated for reaction cross sections, resonance parameters, angular distributions of elastic scattering, average number of neutrons per fission, and prompt fission neutron spectra. They were deduced basically based on the consistent methodologies with the nuclear data evaluations. Statistical processing of experimental data sometimes gives unacceptably small uncertainty compared with experimental data. They may arise from ignoring unknown errors and correlation of experimental data and also from the modeling errors. The covariance data obtained from statistical estimation using the least-squares method were sometimes modified to be reasonable taking account of consistency with dispersion of experimental data, which may reflect the uncertainties of the data. For the fast neutron fission cross sections of 6 major actinides of 233,235,238U and 239,240,241Pu were evaluated simultaneously using both cross section and their ratio data with the least- squares fitting code SOK. It gave the covariance matrices that have cross correlations between different nuclei included in the analyses. For the minor actinide, the least-squares fitting code GMA was used for fission cross section evaluation for fast neutrons. The covariance data were obtained from the calculations at the same time. For other reaction cross sections, covariance matrices were evaluated using CCONE-KALMAN code system. Sensitivities to model parameters were calculated by CCONE code and used to estimate covariance matrices of the parameters with KALMAN code. Covariance matrices for other data such as resonance parameters and average numbers of fission neutrons were also evaluated based on experimental data. The evaluated covariance data were compiled to the ENDF-6 format files and included in JENDL-4.

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

    International Nuclear Information System (INIS)

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

  8. A kinematic-based methodology for radiological protection: Runoff analysis to calculate the effective dose for internal exposure caused by ingestion of radioactive isotopes

    Science.gov (United States)

    Sasaki, Syota; Yamada, Tadashi; Yamada, Tomohito J.

    2014-05-01

    We aim to propose a kinematic-based methodology similar with runoff analysis for readily understandable radiological protection. A merit of this methodology is to produce sufficiently accurate effective doses by basic analysis. The great earthquake attacked the north-east area in Japan on March 11, 2011. The system of electrical facilities to control Fukushima Daiichi nuclear power plant was completely destroyed by the following tsunamis. From the damaged reactor containment vessels, an amount of radioactive isotopes had leaked and been diffused in the vicinity of the plant. Radiological internal exposure caused by ingestion of food containing radioactive isotopes has become an issue of great interest to the public, and has caused excessive anxiety because of a deficiency of fundamental knowledge concerning radioactivity. Concentrations of radioactivity in the human body and internal exposure have been studied extensively. Previous radiologic studies, for example, studies by International Commission on Radiological Protection(ICRP), employ a large-scale computational simulation including actual mechanism of metabolism in the human body. While computational simulation is a standard method for calculating exposure doses among radiology specialists, these methods, although exact, are too difficult for non-specialists to grasp the whole image owing to the sophistication. In this study, the human body is treated as a vessel. The number of radioactive atoms in the human body can be described by an equation of continuity, which is the only governing equation. Half-life, the period of time required for the amount of a substance decreases by half, is only parameter to calculate the number of radioactive isotopes in the human body. Half-life depends only on the kinds of nuclides, there are no arbitrary parameters. It is known that the number of radioactive isotopes decrease exponentially by radioactive decay (physical outflow). It is also known that radioactive isotopes

  9. Combining theoretical chemistry and Xanes multi-edge experiments to probe actinide valence states

    International Nuclear Information System (INIS)

    Both structural and electronic properties of the actinide cations are of fundamental interest in order to describe the intramolecular interactions. The 5f and 6d orbitals are the first partially or totally vacant states of these elements and their properties reflect the nature of the actinide-ligand bond. Because of its chemical and orbital selectivities, XANES spectroscopy is useful to probe the actinides' frontier orbitals and then understand the cation reactivity toward chelating ligands. The actinide L3 edge contains structural information on the coordination polyhedron because of important scattering features. But very little electronic information can be extracted, due to the short core-hole lifetime, broadening the edge signal. On the other hand, the actinide M4,5 edges provide a better resolution and allow one to achieve electronic and structural information. Furthermore, coupling simulations of the experimental spectra and quantum chemical calculations lead to quantitative information such as the determination of the actinide coordination sphere and its effective charge. (authors)

  10. Combining theoretical chemistry and Xanes multi-edge experiments to probe actinide valence states

    Energy Technology Data Exchange (ETDEWEB)

    Fillaux, C.; Guilbaud, Ph.; Guillaumont, D.; Moisy, Ph.; Den Auwer, Ch. [CEA Valrho, Dir. de l' Energie Nucleaire (DEN/DRCP/SCPS), 30 - Marcoule (France); Berthet, J.C. [CEA Saclay, Dept. de Recherche sur l' Etat Condense, les Atomes et les Molecules (DSM/DRECAM/SCM), 91 - Gif sur Yvette (France); Conradsonc, St.D. [Los Alamos National Laboratory, Los Alamos, NM (United States); Hennig, C. [Forschungszentrum Rossendorf, ROBL at ESRF, 38 - Grenoble (France); Roques, J.; Simoni, E. [Institut de Physique Nucleaire, 91 - Orsay (France); Shuh, D.K.; Tyliszczak, T.; Castro-Rodriguez, I. [Lawrence Berkeley National Laboratory, Berkeley, CA (United States)

    2007-10-15

    Both structural and electronic properties of the actinide cations are of fundamental interest in order to describe the intramolecular interactions. The 5f and 6d orbitals are the first partially or totally vacant states of these elements and their properties reflect the nature of the actinide-ligand bond. Because of its chemical and orbital selectivities, XANES spectroscopy is useful to probe the actinides' frontier orbitals and then understand the cation reactivity toward chelating ligands. The actinide L3 edge contains structural information on the coordination polyhedron because of important scattering features. But very little electronic information can be extracted, due to the short core-hole lifetime, broadening the edge signal. On the other hand, the actinide M4,5 edges provide a better resolution and allow one to achieve electronic and structural information. Furthermore, coupling simulations of the experimental spectra and quantum chemical calculations lead to quantitative information such as the determination of the actinide coordination sphere and its effective charge. (authors)

  11. Reduction of minor actinides for recycling in a light water reactor

    International Nuclear Information System (INIS)

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

  12. Catalytic Organic Transformations Mediated by Actinide Complexes

    Directory of Open Access Journals (Sweden)

    Isabell S. R. Karmel

    2015-10-01

    Full Text Available This review article presents the development of organoactinides and actinide coordination complexes as catalysts for homogeneous organic transformations. This chapter introduces the basic principles of actinide catalysis and deals with the historic development of actinide complexes in catalytic processes. The application of organoactinides in homogeneous catalysis is exemplified in the hydroelementation reactions, such as the hydroamination, hydrosilylation, hydroalkoxylation and hydrothiolation of alkynes. Additionally, the use of actinide coordination complexes for the catalytic polymerization of α-olefins and the ring opening polymerization of cyclic esters is presented. The last part of this review article highlights novel catalytic transformations mediated by actinide compounds and gives an outlook to the further potential of this field.

  13. Actinide co-conversion by internal gelation

    International Nuclear Information System (INIS)

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

  14. Actinide ion sensor for pyroprocess monitoring

    Science.gov (United States)

    Jue, Jan-fong; Li, Shelly X.

    2014-06-03

    An apparatus for real-time, in-situ monitoring of actinide ion concentrations which comprises a working electrode, a reference electrode, a container, a working electrolyte, a separator, a reference electrolyte, and a voltmeter. The container holds the working electrolyte. The voltmeter is electrically connected to the working electrode and the reference electrode and measures the voltage between those electrodes. The working electrode contacts the working electrolyte. The working electrolyte comprises an actinide ion of interest. The reference electrode contacts the reference electrolyte. The reference electrolyte is separated from the working electrolyte by the separator. The separator contacts both the working electrolyte and the reference electrolyte. The separator is ionically conductive to the actinide ion of interest. The reference electrolyte comprises a known concentration of the actinide ion of interest. The separator comprises a beta double prime alumina exchanged with the actinide ion of interest.

  15. The complex formation of selected actinides (U, Np, Cm) with microbial ligands

    International Nuclear Information System (INIS)

    One of the urgent tasks in the field of nuclear technology is the final storage of radioactive substances. As a part of the safety requirements the protection of humans and the environment from the danger of radioactive substances in case of the release from the final storage is essential. For performing long-term safety calculations the detailed understanding of the physico-chemical effects and influences which cause the mobilisation and transport of actinides are necessary. The presented work was a discrete part of a project, which was focused on the clarification of the influence of microorganisms on the migration of actinides in case of the release of actinides from a final storage. The influence of microbial produced substances on the mobilisation of selected actinides was studied thereby. The microbial produced substances studied in this project were synthesized by bacteria from the Pseudomonas genus under special conditions. Fluorescent Pseudomonads secrete bacterial pyoverdin-type siderophores with a high potential to complex and transport metals, especially iron(III). The aim of the project was to determine how and under which conditions the bioligands are able to complex also radioactive substances and therefore to transport them. For this work the alpha-emitting actinides uranium, curium and neptunium were chosen because their long-life cycle and their radiotoxicity are a matter of particular interest. This work dealed with the interaction of the actinides U(VI), Np(V) and Cm(III) with model ligands simulating the functionality of the pyoverdins. So, such bioligands can essentially influence the behaviour of actinides in the environment. The results of this work contribute to a better understanding and assessment of the influence of the microbial ligands to the mobilisation and migration of the radionuclides. The outcomes could be used to quantify the actinide-mobilising effect of the bioligands, which are released, for example, in the vicinity of a

  16. Detailed Burnup Calculations for Testing Nuclear Data

    Science.gov (United States)

    Leszczynski, F.

    2005-05-01

    A general method (MCQ) has been developed by introducing a microscopic burnup scheme that uses the Monte Carlo calculated fluxes and microscopic reaction rates of a complex system and a depletion code for burnup calculations as a basis for solving nuclide material balance equations for each spatial region in which the system is divided. Continuous energy-dependent cross-section libraries and full 3D geometry of the system can be input for the calculations. The resulting predictions for the system at successive burnup time steps are thus based on a calculation route where both geometry and cross sections are accurately represented, without geometry simplifications and with continuous energy data, providing an independent approach for benchmarking other methods and nuclear data of actinides, fission products, and other burnable absorbers. The main advantage of this method over the classical deterministic methods currently used is that the MCQ System is a direct 3D method without the limitations and errors introduced on the homogenization of geometry and condensation of energy of deterministic methods. The Monte Carlo and burnup codes adopted until now are the widely used MCNP and ORIGEN codes, but other codes can be used also. For using this method, there is need of a well-known set of nuclear data for isotopes involved in burnup chains, including burnable poisons, fission products, and actinides. For fixing the data to be included in this set, a study of the present status of nuclear data is performed, as part of the development of the MCQ method. This study begins with a review of the available cross-section data of isotopes involved in burnup chains for power and research nuclear reactors. The main data needs for burnup calculations are neutron cross sections, decay constants, branching ratios, fission energy, and yields. The present work includes results of selected experimental benchmarks and conclusions about the sensitivity of different sets of cross

  17. Isotopic Paleoclimatology

    Science.gov (United States)

    Bowen, R.

    Paleotemperature scales were calculated by H. C. Urey and others in the 1950s to assess past temperatures, and later work using the stable isotopes of oxygen, hydrogen, and carbon employed standards such as Peedee belemnite (PDB) and Standard Mean Ocean Water (SMOW). Subsequently, subjects as diverse as ice volume and paleotemperatures, oceanic ice and sediment cores, Pleistocene/Holocene climatic changes, and isotope chronostratigraphy extending back to the Precambrian were investigated.

  18. Topical report on actinide-only burnup credit for PWR spent nuclear fuel packages. Revision 1

    Energy Technology Data Exchange (ETDEWEB)

    None, None

    1997-04-01

    A methodology for performing and applying nuclear criticality safety calculations, for PWR spent nuclear fuel (SNF) packages with actinide-only burnup credit, is described. The changes in the U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, and Am-241 concentration with burnup are used in burnup credit criticality analyses. No credit for fission product neutron absorbers is taken. The methodology consists of five major steps. (1) Validate a computer code system to calculate isotopic concentrations of SNF created during burnup in the reactor core and subsequent decay. A set of chemical assay benchmarks is presented for this purpose as well as a method for assessing the calculational bias and uncertainty, and conservative correction factors for each isotope. (2) Validate a computer code system to predict the subcritical multiplication factor, k{sub eff}, of a spent nuclear fuel package. Fifty-seven UO{sub 2}, UO{sub 2}/Gd{sub 2}O{sub 3}, and UO{sub 2}/PuO{sub 2} critical experiments have been selected to cover anticipated conditions of SNF. The method uses an upper safety limit on k{sub eff} (which can be a function of the trending parameters) such that the biased k{sub eff}, when increased for the uncertainty is less than 0.95. (3) Establish bounding conditions for the isotopic concentration and criticality calculations. Three bounding axial profiles have been established to assure the ''end effect'' is accounted for conservatively. (4) Use the validated codes and bounding conditions to generate package loading criteria (burnup credit loading curves). Burnup credit loading curves show the minimum burnup required for a given initial enrichment. The utility burnup record is compared to this requirement after the utility accounts for the uncertainty in its record. Separate curves may be generated for each assembly design, various minimum cooling times and burnable absorber histories. (5) Verify that SNF assemblies meet the package

  19. TOPICAL REPORT ON ACTINIDE-ONLY BURNUP CREDIT FOR PWR SPENT NUCLEAR FUEL PACKAGES

    International Nuclear Information System (INIS)

    A methodology for performing and applying nuclear criticality safety calculations, for PWR spent nuclear fuel (SNF) packages with actinide-only burnup credit, is described. The changes in the U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, and Am-241 concentration with burnup are used in burnup credit criticality analyses. No credit for fission product neutron absorbers is taken. The methodology consists of five major steps. (1) Validate a computer code system to calculate isotopic concentrations of SNF created during burnup in the reactor core and subsequent decay. A set of chemical assay benchmarks is presented for this purpose as well as a method for assessing the calculational bias and uncertainty, and conservative correction factors for each isotope. (2) Validate a computer code system to predict the subcritical multiplication factor, keff, of a spent nuclear fuel package. Fifty-seven UO2, UO2/Gd2O3, and UO2/PuO2 critical experiments have been selected to cover anticipated conditions of SNF. The method uses an upper safety limit on keff (which can be a function of the trending parameters) such that the biased keff, when increased for the uncertainty is less than 0.95. (3) Establish bounding conditions for the isotopic concentration and criticality calculations. Three bounding axial profiles have been established to assure the ''end effect'' is accounted for conservatively. (4) Use the validated codes and bounding conditions to generate package loading criteria (burnup credit loading curves). Burnup credit loading curves show the minimum burnup required for a given initial enrichment. The utility burnup record is compared to this requirement after the utility accounts for the uncertainty in its record. Separate curves may be generated for each assembly design, various minimum cooling times and burnable absorber histories. (5) Verify that SNF assemblies meet the package loading criteria and confirm proper assembly selection prior to loading

  20. Ionic Interactions in Actinide Tetrahalides

    Science.gov (United States)

    Akdeniz, Z.; Karaman, A.; Tosi, M. P.

    2001-05-01

    We determine a model of the ionic interactions in AX 4 compounds (where A is an atom in the actinide series from Th to Am and X = F, Cl, Br or I) by an analysis of data on the static and dynamic structure of their molecular monomers. The potential energy function that we adopt is taken from earlier work on rare-earth trihalides [Z. Akdeniz, Z. Q q e k and M. P. Tosi, Z. Naturforsch. 55a, 861 (2000)] and in particular allows for the electronic polarizability of the actinide ion. This polarizability quantitatively determines the antisymmetric-bending vibrational mode, but its magnitude remains compatible with a symmetric tetrahedral shape of the molecule at equilibrium. The fluorides have an especially high degree of ionic character, and the interionic-force parameters for each halide of the U, Np, Pu and Am series show regular trends, suggesting that extrapolations to the other transuranic-element halides may usefully be made. The Th compounds show some deviations from these trends, and the interionic-force model that we determine for ThCl4 differs somewhat from that obtained in a previous study. We therefore return on the evaluation of the relative stability of charged oligomers of ThCl4 and ZrCl4 and find confirmation of our earlier results on this problem.

  1. The ALMR actinide burning system

    International Nuclear Information System (INIS)

    The advanced liquid-metal reactor (ALMR) actinide burning system is being developed under the sponsorship of the US Department of Energy to bring its unique capabilities to fruition for deployment in the early 21st century. The system consists of four major parts: the reactor plant, the metal fuel and its recycle, the processing of light water reactor (LWR) spent fuel to extract the actinides, and the development of a residual waste package. This paper addresses the status and outlook for each of these four major elements. The ALMR is being developed by an industrial group under the leadership of General Electric (GE) in a cost-sharing arrangement with the US Department of Energy. This effort is nearing completion of the advanced conceptual design phase and will enter the preliminary design phase in 1994. The innovative modular reactor design stresses simplicity, economics, reliability, and availability. The design has evolved from GE's PRISM design initiative and has progressed to the final stages of a prelicensing review by the US Nuclear Regulatory Commission (NRC); a safety evaluation report is expected by the end of 1993. All the major issues identified during this review process have been technically resolved. The next design phases will focus on implementation of the basic safety philosophy of passive shutdown to a safe, stable condition, even without scram, and passive decay heat removal. Economic projections to date show that it will be competitive with non- nuclear and advanced LWR nuclear alternatives

  2. Electronic structure and ionicity of actinide oxides from first principles

    DEFF Research Database (Denmark)

    Petit, Leon; Svane, Axel; Szotek, Z.;

    2010-01-01

    The ground-state electronic structures of the actinide oxides AO, A2O3, and AO2 (A=U, Np, Pu, Am, Cm, Bk, and Cf) are determined from first-principles calculations, using the self-interaction corrected local spin-density approximation. Emphasis is put on the degree of f-electron localization, which...... for AO2 and A2O3 is found to follow the stoichiometry, namely, corresponding to A4+ ions in the dioxide and A3+ ions in the sesquioxides. In contrast, the A2+ ionic configuration is not favorable in the monoxides, which therefore become metallic. The energetics of the oxidation and reduction...... in the actinide dioxides is discussed, and it is found that the dioxide is the most stable oxide for the actinides from Np onward. Our study reveals a strong link between preferred oxidation number and degree of localization which is confirmed by comparing to the ground-state configurations of the corresponding...

  3. Fabrication of fuel and recycling of minor actinides in fast reactors

    OpenAIRE

    Somers, Joseph

    2010-01-01

    Fuels for future fast reactors will not only produce energy, but they must also actively contribute to the minimisation of long lived wastes produced by these, and other reactor systems. The fuels must incorporate minor actinides (MA = Np, Am, Cm) for neutron transmutation into short lived isotopes. Within Europe oxide fuels are favoured. Transmutation can be considered in homogeneous or heterogeneous reactor recycle modes (i.e. in fuels or targets, respectively). Fabrication of such fuels...

  4. Characterization of actinide physics specimens for the US/UK joint experiment in the Dounreay Prototype Fast Reactor

    International Nuclear Information System (INIS)

    The United States and the United Kingdom are engaged in a joint research program in which samples of the higher actinides are irradiated in the Dounreay Prototype Fast Reactor in Scotland. The purpose of the porogram is (1) to study the materials behavior of selected higher actinide fuels and (2) to determine the integral cross sections of a wide variety of the higher actinide isotopes. Samples of the actinides are incorporated in fuel pins inserted in the core. For the fuel study, the actinides selected are 241Am and 244Cm in the form of Am2O3, Cm2O3, and Am6Cm(RE)7O21, where (RE) represents a mixture of lanthanides. For the cross-section determinations, the samples are milligram quantities of actinide oxides of 248Cm, 246Cm, 244Cm, 243Cm, 243Am, 241Am, 244Pu, 242Pu, 241Pu, 240Pu, 239Pu, 238Pu, 237Np, 238U, 236U, 235U, 234U, 233U, 232Th, 230Th, and 231Pa encapsulated in vanadium. Coincident with the irradiations, neutron flux and energy spectral measurements are made with vanadium-encapsulated dosimeter materials located within the same fuel pins

  5. Minimization of actinide waste by multi-recycling of thoriated fuels in the EPR reactor

    Science.gov (United States)

    Rose, S. J.; Wilson, J. N.; Capellan, N.; David, S.; Guillemin, P.; Ivanov, E.; Méplan, O.; Nuttin, A.; Siem, S.

    2012-02-01

    The multi-recycling of innovative uranium/thorium oxide fuels for use in the European Pressurized water Reactor (EPR) has been investigated. If increasing quantities of 238U, the fertile isotope in standard UO2 fuel, are replaced by 232Th, then a greater yield of new fissile material (233U) is produced during the cycle than would otherwise be the case. This leads to economies of natural uranium of around 45% if the uranium in the spent fuel is multi-recycled. In addition we show that minor actinide and plutonium waste inventories are reduced and hence waste radio-toxicities and decay heats are up to a factor of 20 lower after 103 years. Two innovative fuel types named S90 and S20, ThO2 mixed with 90% and 20% enriched UO2 respectively, are compared as an alternative to standard uranium oxide (UOX) and uranium/plutonium mixed oxide (MOX) fuels at the longest EPR fuel discharge burn-ups of 65 GWd/t. Fissile and waste inventories are examined, waste radio-toxicities and decay heats are extracted and safety feedback coefficients are calculated.

  6. Minimization of actinide waste by multi-recycling of thoriated fuels in the EPR reactor

    Directory of Open Access Journals (Sweden)

    Nuttin A.

    2012-02-01

    Full Text Available The multi-recycling of innovative uranium/thorium oxide fuels for use in the European Pressurized water Reactor (EPR has been investigated. If increasing quantities of 238U, the fertile isotope in standard UO2 fuel, are replaced by 232Th, then a greater yield of new fissile material (233U is produced during the cycle than would otherwise be the case. This leads to economies of natural uranium of around 45% if the uranium in the spent fuel is multi-recycled. In addition we show that minor actinide and plutonium waste inventories are reduced and hence waste radio-toxicities and decay heats are up to a factor of 20 lower after 103 years. Two innovative fuel types named S90 and S20, ThO2 mixed with 90% and 20% enriched UO2 respectively, are compared as an alternative to standard uranium oxide (UOX and uranium/plutonium mixed oxide (MOX fuels at the longest EPR fuel discharge burn-ups of 65 GWd/t. Fissile and waste inventories are examined, waste radio-toxicities and decay heats are extracted and safety feedback coefficients are calculated.

  7. Calculation of the absorbed dose for contamination in skin imparted by beta radiation through the Varskin code modified for 122 isotopes of interest for nuclear medicine, nuclear plants and research

    International Nuclear Information System (INIS)

    In this work the implementation of a modification of the Varskin code for calculation of absorbed dose by contamination in skin imparted by external radiation fields generated by beta emitting is presented. The necessary data for the execution of the code are: isotope, dose depth, isotope activity, geometry type, source radio and time of integration of the isotope, being able to execute combinations of up to five radionuclides. This program it was implemented in Fortran 5 by means of the FFSKIN source program and the executable one in binary language BFFSKIN being the maximum execution time of 5 minutes. (Author)

  8. 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.

  9. Chemical properties of the heavier actinides and transactinides

    International Nuclear Information System (INIS)

    The chemical properties of each of the elements 99 (Es) through 105 are reviewed and their properties correlated with the electronic structure expected for 5f and 6d elements. A major feature of the heavier actinides, which differentiates them from the comparable lanthanides, is the increasing stability of the divalent oxidation state with increasing atomic number. The divalent oxidation state first becomes observable in the anhydrous halides of californium and increases in stability through the series to nobelium, where this valency becomes predominant in aqueous solution. In comparison with the analogous 4f electrons, the 5f electrons in the latter part of the series are more tightly bound. Thus, there is a lowering of the 5f energy levels with respect to the Fermi level as the atomic number increases. The metallic state of the heavier actinides has not been investigated except from the viewpoint of the relative volatility among members of the series. In aqueous solutions, ions of these elements behave as a normal trivalent actinides and lanthanides (except for nobelium). Their ionic radii decrease with increasing nuclear charge which is moderated because of increased screening of the outer 6p electrons by the 5f electrons. The actinide series of elements is completed with the element lawrencium (Lr) in which the electronic configuration is 5f147s27p. From Mendeleev's periodicity and Dirac-Fock calculations, the next group of elements is expected to be a d-transition series corresponding to the elements Hf through Hg. The chemical properties of elements 104 and 105 only have been studied and they indeed appear to show the properties expected of eka-Hf and eka-Ta. However, their nuclear lifetimes are so short and so few atoms can be produced that a rich variety of chemical information is probably unobtainable

  10. Chemical properties of the heavier actinides and transactinides

    Energy Technology Data Exchange (ETDEWEB)

    Hulet, E.K.

    1981-01-01

    The chemical properties of each of the elements 99 (Es) through 105 are reviewed and their properties correlated with the electronic structure expected for 5f and 6d elements. A major feature of the heavier actinides, which differentiates them from the comparable lanthanides, is the increasing stability of the divalent oxidation state with increasing atomic number. The divalent oxidation state first becomes observable in the anhydrous halides of californium and increases in stability through the series to nobelium, where this valency becomes predominant in aqueous solution. In comparison with the analogous 4f electrons, the 5f electrons in the latter part of the series are more tightly bound. Thus, there is a lowering of the 5f energy levels with respect to the Fermi level as the atomic number increases. The metallic state of the heavier actinides has not been investigated except from the viewpoint of the relative volatility among members of the series. In aqueous solutions, ions of these elements behave as a normal trivalent actinides and lanthanides (except for nobelium). Their ionic radii decrease with increasing nuclear charge which is moderated because of increased screening of the outer 6p electrons by the 5f electrons. The actinide series of elements is completed with the element lawrencium (Lr) in which the electronic configuration is 5f/sup 14/7s/sup 2/7p. From Mendeleev's periodicity and Dirac-Fock calculations, the next group of elements is expected to be a d-transition series corresponding to the elements Hf through Hg. The chemical properties of elements 104 and 105 only have been studied and they indeed appear to show the properties expected of eka-Hf and eka-Ta. However, their nuclear lifetimes are so short and so few atoms can be produced that a rich variety of chemical information is probably unobtainable.

  11. Use of high gradient magnetic separation for actinide application

    International Nuclear Information System (INIS)

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Bliss, Mary; Stave, Jean A.

    2012-10-01

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

  13. Experimental studies of actinides in molten salts

    International Nuclear Information System (INIS)

    This review stresses techniques used in studies of molten salts containing multigram amounts of actinides exhibiting intense alpha activity but little or no penetrating gamma radiation. The preponderance of studies have used halides because oxygen-containing actinide compounds (other than oxides) are generally unstable at high temperatures. Topics discussed here include special enclosures, materials problems, preparation and purification of actinide elements and compounds, and measurements of various properties of the molten volts. Property measurements discussed are phase relationships, vapor pressure, density, viscosity, absorption spectra, electromotive force, and conductance. 188 refs., 17 figs., 6 tabs

  14. Electronic structure and magnetic properties of actinides

    International Nuclear Information System (INIS)

    The study of the actinide series shows the change between transition metal behavior and lanthanide behavior, between constant weak paramagnetism for thorium and strong Curie-Weiss paramagnetism for curium. Curium is shown to be the first metal of the actinide series to be magnetically ordered, its Neel temperature being 52K. The magnetic properties of the actinides depending on all the peripheral electrons, their electronic structure was studied and an attempt was made to determine it by means of a phenomenological model. Attempts were also made to interrelate the different physical properties which depend on the outer electronic structure

  15. Experimental studies of actinides in molten salts

    Energy Technology Data Exchange (ETDEWEB)

    Reavis, J.G.

    1985-06-01

    This review stresses techniques used in studies of molten salts containing multigram amounts of actinides exhibiting intense alpha activity but little or no penetrating gamma radiation. The preponderance of studies have used halides because oxygen-containing actinide compounds (other than oxides) are generally unstable at high temperatures. Topics discussed here include special enclosures, materials problems, preparation and purification of actinide elements and compounds, and measurements of various properties of the molten volts. Property measurements discussed are phase relationships, vapor pressure, density, viscosity, absorption spectra, electromotive force, and conductance. 188 refs., 17 figs., 6 tabs.

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

    OpenAIRE

    Soucek, Pavel; Cassayre, Laurent; Eloirdi, Rachel; Malmbeck, Rikard; Meier, Roland; Nourry, Christophe; Claux, Benoit; Glatz, Jean-Paul

    2014-01-01

    International audience; A chlorination route is being investigated for recovery of actinides from actinide-aluminium alloys, which originate from pyrochemical recovery of actinides from spent metallic nuclear fuel by electrochemical methods in molten LiCl-KCl. In the present work, the most important steps of this route were experimentally tested using U-Pu-Al alloy prepared by electrodeposition of U and Pu on solid aluminium plate electrodes. The investigated processes were vacuum distillatio...

  17. Recovery of actinides from actinide-aluminium alloys by chlorination: Part I

    OpenAIRE

    Cassayre, Laurent; Soucek, Pavel; Mendes, Eric; Malmbeck, Rikard; Nourry, Christophe; Eloirdi, Rachel; Glatz, Jean-Paul

    2011-01-01

    Pyrochemical processes in molten LiCl–KCl are being developed in ITU for recovery of actinides from spent nuclear fuel. The fuel is anodically dissolved to the molten salt electrolyte and actinides are electrochemically reduced on solid aluminium cathodes forming solid actinide–aluminium alloys. A chlorination route is being investigated for recovery of actinides from the alloys. This route consists in three steps: Vacuum distillation for removal of the salt adhered on the electrode, chlorina...

  18. Shape coexistence in neutron-deficient Hg isotopes studied via lifetime measurements in $^{184,186}$Hg and two-state mixing calculations

    CERN Document Server

    Gaffney, L P; Page, R.D.; Grahn, T.; Scheck, M.; Butler, P.A.; Bertone, P.F.; Bree, N.; Carroll, R.J.; Carpenter, M.P.; Chiara, C.J.; Dewald, A.; Filmer, F.; Fransen, C.; Huyse, M.; Janssens, R.V.F.; Joss, D.T.; Julin, R.; Kondev, F.G.; Nieminen, P.; Pakarinen, J.; Rigby, S.V.; Rother, W.; Van Duppen, P.; Watkins, H.V.; Wrzosek-Lipska, K.; Zhu, S.

    2014-01-01

    The neutron-deficient mercury isotopes, $^{184,186}$Hg, were studied with the Recoil Distance Doppler Shift (RDDS) method using the Gammasphere array and the K\\"oln Plunger device. The Differential Decay Curve Method (DDCM) was employed to determine the lifetimes of the yrast states in $^{184,186}$Hg. An improvement on previously measured values of yrast states up to $8^{+}$ is presented as well as first values for the $9_{3}$ state in $^{184}$Hg and $10^{+}$ state in $^{186}$Hg. $B(E2)$ values are calculated and compared to a two-state mixing model which utilizes the variable moment of inertia (VMI) model, allowing for extraction of spin-dependent mixing strengths and amplitudes.

  19. Ion-molecule reactions involving HCO$^+$ and N$_2$H$^+$: Isotopologue equilibria from new theoretical calculations and consequences for interstellar isotope fractionation

    CERN Document Server

    Mladenović, Mirjana

    2014-01-01

    $Aims$: We revisit with new augmented accuracy the theoretical dynamics of basic isotope exchange reactions involved in the $^{12}$C/$^{13}$C, $^{16}$O/$^{18}$O, and $^{14}$N/$^{15}$N balance because these reactions have already been studied experimentally in great detail. $Methods$: Electronic structure methods were employed to explore potential energy surfaces, full-dimensional rovibrational calculations to compute rovibrational energy levels that are numerically exact, and chemical network models to estimate the abundance ratios under interstellar conditions. $Results$: New exothermicities, derived for HCO$^+$ reacting with CO, provide rate coefficients markedly different from previous theoretical values in particular at low temperatures, resulting in new abundance ratios relevant for carbon chemistry networks. In concrete terms, we obtain a reduction in the abundance of H$^{12}$C$^{18}$O$^+$ and an increase in the abundance of H$^{13}$C$^{16}$O$^+$ and D$^{13}$C$^{16}$O$^+$. In all studied cases, the reac...

  20. Characterization of partitioning relevant lanthanide and actinide complexes by NMR spectroscopy

    International Nuclear Information System (INIS)

    In the present work the interaction of N-donor ligands, such as 2,6-Bis(5,6-dipropyl-1,2,4-triazin-3-yl)pyridine (nPrBTP) and 2,6-Bis(5-(2,2-dimethylpropyl)1H-pyrazol)-3-yl-pyridine (C5-BPP), with trivalent lanthanide and actinide ions was studied. Ligands of this type show a high selectivity for the separation of trivalent actinide ions over lanthanides from nitric acid solutions. However, the reason for this selectivity, which is crucial for future partitioning and transmutation strategies for radioactive wastes, is still unknown. So far, the selectivity of some N-donor ligands is supposed to be an effect of an increased covalency in the actinide-ligand bond, compared to the lanthanide compounds. NMR spectroscopy on paramagnetic metal complexes is an excellent tool for the elucidation of bonding modes. The overall paramagnetic chemical shift consists of two contributions, the Fermi Contact Shift (FCS), due to electron spin delocalisation through covalent bonds, and the Pseudo Contact Shift (PCS), which describes the dipolar coupling of the electron magnetic moment and the nuclear spin. By assessing the FCS share in the paramagnetic shift, the degree of covalency in the metal-ligand bond can be gauged. Several methods to discriminate FCS and PCS have been used on the data of the nPrBTP- and C5-BPP-complexes and were evaluated regarding their applicability on lanthanide and actinide complexes with N-donor ligands. The study comprised the synthesis of all Ln(III) complexes with the exceptions of Pm(III) and Gd(III) as well as the Am(III) complex as a representative of the actinide series with both ligands. All complexes were fully characterised (1H, 13C and 15N spectra) using NMR spectroscopy. By isotope enrichment with the NMR-active 15N in positions 8 and 9 in both ligands, resonance signals of these nitrogen atoms were detected for all complexes. The Bleaneymethod relies on different temperature dependencies for FCS (T-1) and PCS (T-2) that occur upon description

  1. Comparison of actinides and fission products recycling scheme with the normal plutonium recycling scheme in fast reactors

    OpenAIRE

    Salahuddin Asif; Iqbal Masood

    2013-01-01

    Multiple recycling of actinides and non-volatile fission products in fast reactors through the dry re-fabrication/reprocessing atomics international reduction oxidation process has been studied as a possible way to reduce the long-term potential hazard of nuclear waste compared to that resulting from reprocessing in a wet PUREX process. Calculations have been made to compare the actinides and fission products recycling scheme with the normal plutonium recycling scheme in a fast reactor....

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1999-02-12

    By reviewing how microorganisms interact with actinides in subsurface environments, we assess how bioremediation controls the fate of actinides. Actinides often are co-contaminants with strong organic chelators, chlorinated solvents, and fuel hydrocarbons. Bioremediation can immobilize the actinides, biodegrade the co-contaminants, or both. Actinides at the IV oxidation state are the least soluble, and microorganisms accelerate precipitation by altering the actinide's oxidation state or its speciation. We describe how microorganisms directly oxidize or reduce actinides and how microbiological reactions that biodegrade strong organic chelators, alter the pH, and consume or produce precipitating anions strongly affect actinide speciation and, therefore, mobility. We explain why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions. Due to the complex interactions of the microbiological and chemical phenomena, mathematical modeling is an essential tool for research on and application of bioremediation involving co-contamination with actinides. We describe the development of mathematical models that link microbiological and geochemical reactions. Throughout, we identify the key research needs.

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

    International Nuclear Information System (INIS)

    By reviewing how microorganisms interact with actinides in subsurface environments, we assess how bioremediation controls the fate of actinides. Actinides often are co-contaminants with strong organic chelators, chlorinated solvents, and fuel hydrocarbons. Bioremediation can immobilize the actinides, biodegrade the co-contaminants, or both. Actinides at the IV oxidation state are the least soluble, and microorganisms accelerate precipitation by altering the actinide's oxidation state or its speciation. We describe how microorganisms directly oxidize or reduce actinides and how microbiological reactions that biodegrade strong organic chelators, alter the pH, and consume or produce precipitating anions strongly affect actinide speciation and, therefore, mobility. We explain why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions. Due to the complex interactions of the microbiological and chemical phenomena, mathematical modeling is an essential tool for research on and application of bioremediation involving co-contamination with actinides. We describe the development of mathematical models that link microbiological and geochemical reactions. Throughout, we identify the key research needs

  4. Actinide recovery from pyrochemical residues

    International Nuclear Information System (INIS)

    We demonstrated a new process for recovering plutonium and americium from pyrochemical waste. The method is based on chloride solution anion exchange at low acidity, or acidity that eliminates corrosive HCl fumes. Developmental experiments of the process flow chart concentrated on molten salt extraction (MSE) residues and gave >95% plutonium and >90% americium recovery. The recovered plutonium contained 62- from high-chloride low-acid solution. Americium and other metals are washed from the ion exchange column with lN HNO3-4.8M NaCl. After elution, plutonium is recovered by hydroxide precipitation, and americium is recovered by NaHCO3 precipitation. All filtrates from the process can be discardable as low-level contaminated waste. Production-scale experiments are in progress for MSE residues. Flow charts for actinide recovery from electro-refining and direct oxide reduction residues are presented and discussed

  5. The Use of Molybdenum-Based Ceramic-Metal (CerMet) Fuel for the Actinide Management in LWRs

    International Nuclear Information System (INIS)

    The technical and economic aspects of the use of molybdenum depleted in the isotope 95Mo (DepMo) for the transmutation of actinides in a light water reactor are discussed. DepMo has a low neutron absorption cross section and good physical and chemical properties. Therefore, DepMo is expected to be a good inert matrix in ceramic-metal fuel. The costs of the use of DepMo have been assessed, and it was concluded that these costs can be justified for the transmutation of the actinides neptunium, americium, and plutonium

  6. Preparation of actinide targets by electrodeposition

    Science.gov (United States)

    Trautmann, N.; Folger, H.

    1989-10-01

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

  7. Actinide research to solve some practical problems

    International Nuclear Information System (INIS)

    The following topics are discussed: generation of plutonium inventories by nuclear power plants; resettlement of the Marshallese Islanders into an actinide contaminated environment; high radiation background areas of the world; and radiation hazards to uranium miners

  8. Electronic structure and correlation effects in actinides

    Energy Technology Data Exchange (ETDEWEB)

    Albers, R.C.

    1998-12-01

    This report consists of the vugraphs given at a conference on electronic structure. Topics discussed are electronic structure, f-bonding, crystal structure, and crystal structure stability of the actinides and how they are inter-related.

  9. Overview of actinide chemistry in the WIPP

    Energy Technology Data Exchange (ETDEWEB)

    Borkowski, Marian [Los Alamos National Laboratory; Lucchini, Jean - Francois [Los Alamos National Laboratory; Richmann, Michael K [Los Alamos National Laboratory; Reed, Donald T [Los Alamos National Laboratory; Khaing, Hnin [Los Alamos National Laboratory; Swanson, Juliet [Los Alamos National Laboratory

    2009-01-01

    The year 2009 celebrates 10 years of safe operations at the Waste Isolation Pilot Plant (WIPP), the only nuclear waste repository designated to dispose defense-related transuranic (TRU) waste in the United States. Many elements contributed to the success of this one-of-the-kind facility. One of the most important of these is the chemistry of the actinides under WIPP repository conditions. A reliable understanding of the potential release of actinides from the site to the accessible environment is important to the WIPP performance assessment (PA). The environmental chemistry of the major actinides disposed at the WIPP continues to be investigated as part of the ongoing recertification efforts of the WIPP project. This presentation provides an overview of the actinide chemistry for the WIPP repository conditions. The WIPP is a salt-based repository; therefore, the inflow of brine into the repository is minimized, due to the natural tendency of excavated salt to re-seal. Reducing anoxic conditions are expected in WIPP because of microbial activity and metal corrosion processes that consume the oxygen initially present. Should brine be introduced through an intrusion scenario, these same processes will re-establish reducing conditions. In the case of an intrusion scenario involving brine, the solubilization of actinides in brine is considered as a potential source of release to the accessible environment. The following key factors establish the concentrations of dissolved actinides under subsurface conditions: (1) Redox chemistry - The solubility of reduced actinides (III and IV oxidation states) is known to be significantly lower than the oxidized forms (V and/or VI oxidation states). In this context, the reducing conditions in the WIPP and the strong coupling of the chemistry for reduced metals and microbiological processes with actinides are important. (2) Complexation - For the anoxic, reducing and mildly basic brine systems in the WIPP, the most important

  10. BWR Assembly Optimization for Minor Actinide Recycling

    Energy Technology Data Exchange (ETDEWEB)

    G. Ivan Maldonado; John M. Christenson; J.P. Renier; T.F. Marcille; J. Casal

    2010-03-22

    The Primary objective of the proposed project is to apply and extend the latest advancements in LWR fuel management optimization to the design of advanced boiling water reactor (BWR) fuel assemblies specifically for the recycling of minor actinides (MAs).

  11. Advanced Aqueous Separation Systems for Actinide Partitioning

    Energy Technology Data Exchange (ETDEWEB)

    Nash, Kenneth L.; Clark, Sue; Meier, G Patrick; Alexandratos, Spiro; Paine, Robert; Hancock, Robert; Ensor, Dale

    2012-03-21

    One of the most challenging aspects of advanced processing of spent nuclear fuel is the need to isolate transuranium elements from fission product lanthanides. This project expanded the scope of earlier investigations of americium (Am) partitioning from the lanthanides with the synthesis of new separations materials and a centralized focus on radiochemical characterization of the separation systems that could be developed based on these new materials. The primary objective of this program was to explore alternative materials for actinide separations and to link the design of new reagents for actinide separations to characterizations based on actinide chemistry. In the predominant trivalent oxidation state, the chemistry of lanthanides overlaps substantially with that of the trivalent actinides and their mutual separation is quite challenging.

  12. Lanthanides and actinides in ionic liquids

    OpenAIRE

    Binnemans, Koen

    2007-01-01

    This lecture gives an overview of the research possibilities offered by combining f-elements (lanthanides and actinides) with ionic liquids [1] Many ionic liquids are solvents with weakly coordinating anions. Solvation of lanthanide and actinide ions in these solvents is different from what is observed in conventional organic solvents and water. The poorly solvating behavior can also lead to the formation of coordination compounds with low coordination numbers. The solvation of f-elements can...

  13. Superconductivity in rare earth and actinide compounds

    International Nuclear Information System (INIS)

    Rare earth and actinide compounds and the extraordinary superconducting and magnetic phenomena they exhibit are surveyed. The rare earth and actinide compounds described belong to three classes of novel superconducting materials: high temperature, high field superconductors (intermetallics and layered cuprates); superconductors containing localized magnetic moments; heavy fermion superconductors. Recent experiments on the resistive upper critical field of high Tc cuprate superconductors and the peak effect in the critical current density of the f-electron superconductor CeRu2 are discussed. (orig.)

  14. The Actinide Transition Revisited by Gutzwiller Approximation

    Science.gov (United States)

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

    2015-03-01

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

  15. Lattice effects in the light actinides

    Energy Technology Data Exchange (ETDEWEB)

    Lawson, A.C.; Cort, B.; Roberts, J.A.; Bennett, B.I.; Brun, T.O.; Dreele, R.B. von [Los Alamos National Lab., NM (United States); Richardson, J.W. Jr. [Argonne National Lab., IL (United States)

    1998-12-31

    The light actinides show a variety of lattice effects that do not normally appear in other regions of the periodic table. The article will cover the crystal structures of the light actinides, their atomic volumes, their thermal expansion behavior, and their elastic behavior as reflected in recent thermal vibration measurements made by neutron diffraction. A discussion of the melting points will be given in terms of the thermal vibration measurements. Pressure effects will be only briefly indicated.

  16. Transmutation of actinides in power reactors.

    Science.gov (United States)

    Bergelson, B R; Gerasimov, A S; Tikhomirov, G V

    2005-01-01

    Power reactors can be used for partial short-term transmutation of radwaste. This transmutation is beneficial in terms of subsequent storage conditions for spent fuel in long-term storage facilities. CANDU-type reactors can transmute the main minor actinides from two or three reactors of the VVER-1000 type. A VVER-1000-type reactor can operate in a self-service mode with transmutation of its own actinides.

  17. Analysis of the minority actinides transmutation in a sodium fast reactor with uniform load pattern by the MCNPX-CINDER code; Analisis de la transmutacion de actinidos en un reactor rapido de sodio con modelo de carga homogeneo mediante el codigo MCNPX-CINDER

    Energy Technology Data Exchange (ETDEWEB)

    Ochoa Valero, R.; Garcia-Herranz, N.; Aragones, J. M.

    2010-07-01

    The aim of this study is to evaluate the minority actinides transmutation in sodium fast reactors (SFR) assuming a uniform load pattern. It is determined the isotopic evolution of the actinides along burn, and the evolution of the reactivity and the reactivity coefficients. For that, it is used the MCNPX neutron transport code coupled with the inventory code CINDER90.

  18. Chemistry of tetravalent actinides phosphates. The thorium phosphate-diphosphate as immobilisation matrix of actinides; Chimie des phosphates d'actinides tetravalents. Le phosphate-diphosphate de thorium en tant que matrice d'imobilisation des actinides

    Energy Technology Data Exchange (ETDEWEB)

    Dacheux, N

    2002-07-01

    The author presents in this document its scientific works from 1992 to 2001, in order to obtain the enabling to manage scientific and chemical researches at the university Paris Sud Orsay. The first part gives an abstract of the thesis on the characterizations, lixiviation and synthesis of uranium and thorium based phosphate matrix in the framework of the search for a ceramic material usable in the radioactive waste storage. The second part presents briefly the researches realized at the CEA, devoted to a reliable, independent and accurate measure of some isotopes activity. The last part presents the abstracts of researches activities from 1996 to 2001 on the tetravalent actinides phosphates chemistry, the sintering of PDT and solid solutions of PDTU and the kinetic and thermodynamical studies of the PDT dissolution. Many references and some publication in full text are provided. (A.L.B.)

  19. Evaluation of actinide partitioning and transmutation

    International Nuclear Information System (INIS)

    After a few centuries of radioactive decay the long-lived actinides, the elements of atomic numbers 89-103, may constitute the main potential radiological health hazard in nuclear wastes. This is because all but a very few fission products (principally technetium-99 and iodine-129) have by then undergone radioactive decay to insignificant levels, leaving the actinides as the principal radionuclides remaining. It was therefore at first sight an attractive concept to recycle the actinides to nuclear reactors, so as to eliminate them by nuclear fission. Thus, investigations of the feasibility and potential benefits and hazards of the concept of 'actinide partitioning and transmutation' were started in numerous countries in the mid-1970s. This final report summarizes the results and conclusions of technical studies performed in connection with a four-year IAEA Co-ordinated Research Programme, started in 1976, on the ''Environmental Evaluation and Hazard Assessment of the Separation of Actinides from Nuclear Wastes followed by either Transmutation or Separate Disposal''. Although many related studies are still continuing, e.g. on waste disposal, long-term safety assessments, and waste actinide management (particularly for low and intermediate-level wastes), some firm conclusions on the overall concept were drawn by the programme participants, which are reflected in this report

  20. Recent progress in actinide borate chemistry.

    Science.gov (United States)

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

    2011-10-21

    The use of molten boric acid as a reactive flux for synthesizing actinide borates has been developed in the past two years providing access to a remarkable array of exotic materials with both unusual structures and unprecedented properties. [ThB(5)O(6)(OH)(6)][BO(OH)(2)]·2.5H(2)O possesses a cationic supertetrahedral structure and displays remarkable anion exchange properties with high selectivity for TcO(4)(-). Uranyl borates form noncentrosymmetric structures with extraordinarily rich topological relationships. Neptunium borates are often mixed-valent and yield rare examples of compounds with one metal in three different oxidation states. Plutonium borates display new coordination chemistry for trivalent actinides. Finally, americium borates show a dramatic departure from plutonium borates, and there are scant examples of families of actinides compounds that extend past plutonium to examine the bonding of later actinides. There are several grand challenges that this work addresses. The foremost of these challenges is the development of structure-property relationships in transuranium materials. A deep understanding of the materials chemistry of actinides will likely lead to the development of advanced waste forms for radionuclides present in nuclear waste that prevent their transport in the environment. This work may have also uncovered the solubility-limiting phases of actinides in some repositories, and allows for measurements on the stability of these materials. PMID:21915396

  1. Heavy element and actinide decay data: UKHEDD-2 data files

    International Nuclear Information System (INIS)

    A re-evaluation has been made of the decay data for 126 heavy elements and actinides of direct application in nuclear fuel cycle calculations. Computer-based data files have been produced in ENDF/B-VI format, including lists of the references used to produce the proposed decay schemes and comments that identify their inadequacies. These evaluated data include half-lives, average decay energies, branching ratios, alpha, beta and gamma-ray energies and emission probabilities, internal conversion coefficients, spontaneous fission decay data and all associated uncertainties. (author)

  2. X-ray study of chemical bonding in actinides(IV) and lanthanides(III) hexa-cyanoferrates

    International Nuclear Information System (INIS)

    Bimetallic cyanide molecular solids derived from Prussian blue are well known to foster long-range magnetic ordering and show an intense inter-valence charge transfer band resulting from an exchange interaction through the cyanide-bridge. For those reasons the ferrocyanide and ferricyanide building blocks have been chosen to study electronic delocalization and covalent character in actinide bonding using an experimental and theoretical approach based on X-ray absorption spectroscopy. In 2001, the actinide (IV) and early lanthanides (III) hexacyanoferrate have been found by powder X-ray diffraction to be isostructural (hexagonal, P63/m group). Here, extended X-ray Absorption Fine Structure (EXAFS) at the iron K-edge and actinide L3-edge have been undertaken to probe the local environment of both actinides and iron cations. In an effort to describe the cyano bridge, a double edge fitting procedure including both iron and actinide edges and based on multiple scattering approach has been developed. We have also investigated the electronic properties of these molecular solids. Low energy electronic transitions have been used iron L2,3 edge, nitrogen and carbon K-edge and also actinides N4,5 edge to directly probe the valence molecular orbitals of the complex. Using a phenomenological approach, a clear distinctive behaviour between actinides and lanthanides has been shown. Then a theoretical approach using quantum chemistry calculation has shown more specifically the effect of covalency in the actinide-ferrocyanide bond. More specifically, π interactions were underlined by both theoretical and experimental methods. Finally, in agreement with the ionic character of the lanthanide bonding no inter-valence charge transfer has been observed in the corresponding optical spectra of these compounds. On the contrary, optical spectra for actinides adducts (except for thorium) show an intense inter-valence charge transfer band like in the transition metal cases which is

  3. Advanced processes for minor actinides recycling: studies towards potential industrialization

    International Nuclear Information System (INIS)

    In June 2006, a new act on sustainable management of radioactive waste was voted by the French parliament with a national plan on radioactive materials and radioactive waste management (PNG-MDR). Concerning partitioning and transmutation, the program is connected to 4. generation reactors, in which transmutation of minor actinides could be operated. In this frame, the next important milestone is 2012, with the assessment of the possible transmutation roads, which are either homogeneous recycling of the minor actinides in the whole reactor fleet, with a low content of M.A (∼3%) in all fuel assemblies, or heterogeneous recycling of the minor actinides in about one third of the reactor park, with a higher content of M.A. (∼20%) in dedicated targets dispatched in the periphery of the reactor. Advanced processes for the recycling of minor actinides are being developed to address the challenges of these various management options. An important part of the program consists in getting closer to process implementation conditions. The processes based on liquid-liquid extraction benefit from the experience gained by operating the PUREX process at the La Hague plant. In the field of extracting apparatus, a large experience is available. In the field of extracting apparatus, a large experience is already available. Nevertheless, the processes present specificities which have to be considered more precisely. They have been classified in the following fields: - Evolution of the simulation codes, including phenomenological representations: with such a simulation tool, it will be possible to assess operating tolerances, lead sensitivity studies and calculate transient states; - Definition of the implementation conditions in continuous contactors (such as pulse columns), according to the extractant physico-chemical characteristics; - Scale-up of new extractants, such as malonamides used in the DIAMEX process, facing purity specifications and costs estimation; - Solvent clean

  4. Ion-molecule reactions involving HCO+ and N2H+: Isotopologue equilibria from new theoretical calculations and consequences for interstellar isotope fractionation

    Science.gov (United States)

    Mladenović, M.; Roueff, E.

    2014-06-01

    Aims: We revisit with new augmented accuracy the theoretical dynamics of basic isotope exchange reactions involved in the 12C/13C, 16O/18O, and 14N/15N balance because these reactions have already been studied experimentally in great detail. Methods: Electronic structure methods were employed to explore potential energy surfaces, full-dimensional rovibrational calculations to compute rovibrational energy levels that are numerically exact, and chemical network models to estimate the abundance ratios under interstellar conditions. Results: New exothermicities, derived for HCO+ reacting with CO, provide rate coefficients markedly different from previous theoretical values in particular at low temperatures, resulting in new abundance ratios relevant for carbon chemistry networks. In concrete terms, we obtain a reduction in the abundance of H12C18O+ and an increase in the abundance of H13C16O+ and D13C16O+. In all studied cases, the reaction of the ion with a neutral polarizable molecule proceeds through the intermediate proton-bound complex found to be very stable. For the complexes OCH+··· CO, OCH+··· OC, COHOC+, N2··· HCO+, N2H+··· OC, and N2HN2+, we also calculated vibrational frequencies and dissociation energies. Conclusions: The linear proton-bound complexes possess sizeable dipole moments, which may facilitate their detection.

  5. A first principles investigation of the electronic structure of actinide oxides

    DEFF Research Database (Denmark)

    Petit, Leon; Svane, Axel; Szotek, Zdzislawa;

    2010-01-01

    The ground state electronic structures of the actinide oxides AO, A2O3 and AO2 (A=U, Np, Pu, Am, Cm, Bk, Cf) are determined from first-principles calculations using the selfinteraction corrected local spin-density approximation. Our study reveals a strong link between preferred oxidation number a...

  6. Intercomparison of derived integral data from evaluated data libraries of the actinides

    International Nuclear Information System (INIS)

    Resonance integrals and fission spectrum averaged cross-sections are calculated for the actinides from all recent major evaluated libraries. Whenever possible the results are compared against measurements. It is found that the experimental data are scarce and that there exist considerable differences between experimentally measured data and those derived from the evaluated libraries. (author). 93 refs and tabs

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

    International Nuclear Information System (INIS)

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

  8. FTIR study of the photoinduced processes of plant phytochrome phyA using isotope-labeled bilins and density functional theory calculations.

    Science.gov (United States)

    Schwinté, Pascale; Foerstendorf, Harald; Hussain, Zakir; Gärtner, Wolfgang; Mroginski, Maria-Andrea; Hildebrandt, Peter; Siebert, Friedrich

    2008-08-01

    Fourier transform infrared spectroscopy was used to analyze the chromophore structure in the parent states Pr and Pfr of plant phytochrome phyA and the respective photoproducts lumi-R and lumi-F. The spectra were obtained from phyA adducts assembled with either uniformly or selectively isotope-labeled phytochromobilin and phycocyanobilin. The interpretation of the experimental spectra is based on the spectra of chromophore models calculated by density functional theory. Global (13)C-labeling of the tetrapyrrole allows for the discrimination between chromophore and protein bands in the Fourier transform infrared difference spectra. All infrared difference spectra display a prominent difference band attributable to a stretching mode with large contributions from the methine bridge between the inner pyrrole rings (B-C stretching). Due to mode coupling, frequencies and isotopic shifts of this mode suggest that the Pr chromophore may adopt a distorted ZZZssa or ZZZasa geometry with a twisted A-B methine bridge. The transition to lumi-R is associated with only minor changes of the amide I bands indicating limited protein structural changes during the isomerization site of the C-D methine bridge. Major protein structural changes occur upon the transition to Pfr in which the chromophore adopts a ZZEssa or ZZEasa-like state. In addition, specific interactions with the protein alter the structure of the B-C methine bridge as concluded from the substantial downshift of the respective stretching mode. These interactions are removed during the photoreaction to lumi-F (ZZE-->ZZZ), which involves only small protein structural changes. PMID:18390618

  9. MOLECULAR SPECTROSCPY AND REACTIONS OF ACTINIDES IN THE GAS PHASE AND CRYOGENIC MATRICES

    Energy Technology Data Exchange (ETDEWEB)

    Heaven, Michael C.; Gibson, John K.; Marcalo, Joaquim

    2009-02-01

    In this chapter we review the spectroscopic data for actinide molecules and the reaction dynamics for atomic and molecular actinides that have been examined in the gas phase or in inert cryogenic matrices. The motivation for this type of investigation is that physical properties and reactions can be studied in the absence of external perturbations (gas phase) or under minimally perturbing conditions (cryogenic matrices). This information can be compared directly with the results from high-level theoretical models. The interplay between experiment and theory is critically important for advancing our understanding of actinide chemistry. For example, elucidation of the role of the 5f electrons in bonding and reactivity can only be achieved through the application of experimentally verified theoretical models. Theoretical calculations for the actinides are challenging due the large numbers of electrons that must be treated explicitly and the presence of strong relativistic effects. This topic has been reviewed in depth in Chapter 17 of this series. One of the goals of the experimental work described in this chapter has been to provide benchmark data that can be used to evaluate both empirical and ab initio theoretical models. While gas-phase data are the most suitable for comparison with theoretical calculations, there are technical difficulties entailed in generating workable densities of gas-phase actinide molecules that have limited the range of species that have been characterized. Many of the compounds of interest are refractory, and problems associated with the use of high temperature vapors have complicated measurements of spectra, ionization energies, and reactions. One approach that has proved to be especially valuable in overcoming this difficulty has been the use of pulsed laser ablation to generate plumes of vapor from refractory actinide-containing materials. The vapor is entrained in an inert gas, which can be used to cool the actinide species to room

  10. Comparative Study of f-Element Electronic Structure across a Series of Multimetallic Actinide, Lanthanide-Actinide and Lanthanum-Actinide Complexes Possessing Redox-Active Bridging Ligands

    Energy Technology Data Exchange (ETDEWEB)

    Schelter, Eric J.; Wu, Ruilian; Veauthier, Jacqueline M.; Bauer, Eric D.; Booth, Corwin H.; Thomson, Robert K.; Graves, Christopher R.; John, Kevin D.; Scott, Brian L.; Thompson, Joe D.; Morris, David E.; Kiplinger, Jaqueline L.

    2010-02-24

    A comparative examination of the electronic interactions across a series of trimetallic actinide and mixed lanthanide-actinide and lanthanum-actinide complexes is presented. Using reduced, radical terpyridyl ligands as conduits in a bridging framework to promote intramolecular metal-metal communication, studies containing structural, electrochemical, and X-ray absorption spectroscopy are presented for (C{sub 5}Me{sub 5}){sub 2}An[-N=C(Bn)(tpy-M{l_brace}C{sub 5}Me4R{r_brace}{sub 2})]{sub 2} (where An = Th{sup IV}, U{sup IV}; Bn = CH{sub 2}C{sub 6}H{sub 5}; M = La{sup III}, Sm{sup III}, Yb{sup III}, U{sup III}; R = H, Me, Et) to reveal effects dependent on the identities of the metal ions and R-groups. The electrochemical results show differences in redox energetics at the peripheral 'M' site between complexes and significant wave splitting of the metal- and ligand-based processes indicating substantial electronic interactions between multiple redox sites across the actinide-containing bridge. Most striking is the appearance of strong electronic coupling for the trimetallic Yb{sup III}-U{sup IV}-Yb{sup III}, Sm{sup III}-U{sup IV}-Sm{sup III}, and La{sup III}-U{sup IV}-La{sup III} complexes, [8]{sup -}, [9b]{sup -} and [10b]{sup -}, respectively, whose calculated comproportionation constant K{sub c} is slightly larger than that reported for the benchmark Creutz-Taube ion. X-ray absorption studies for monometallic metallocene complexes of U{sup III}, U{sup IV}, and U{sup V} reveal small but detectable energy differences in the 'white-line' feature of the uranium L{sub III}-edges consistent with these variations in nominal oxidation state. The sum of this data provides evidence of 5f/6d-orbital participation in bonding and electronic delocalization in these multimetallic f-element complexes. An improved, high-yielding synthesis of 4{prime}-cyano-2,2{prime}:6{prime},2{double_prime}-terpyridine is also reported.

  11. Bruyères-le-Châtel Neutron Evaluations of Actinides with the TALYS Code: The Fission Channel

    Science.gov (United States)

    Romain, P.; Morillon, B.; Duarte, H.

    2016-01-01

    For several years, various neutron evaluations of plutonium and uranium isotopes have been performed at Bruyères-le-Châtel (BRC), from 1 keV up to 30 MeV. Since only nuclear reaction models have been used to produce these evaluations, our approach was named the "Full Model" approach. Total, shape elastic and direct inelastic cross sections were obtained from the coupled channels model using a dispersive optical potential developed for actinides, with a large enough coupling scheme including the lowest octupolar band. All other cross sections were calculated using the Hauser-Feshbach theory (TALYS code) with a pre-equilibrium component above 8-10 MeV. In this paper, we focus our attention on the fission channel. More precisely, we will present the BRC contribution to fission modeling and the philosophy adopted in our "Full Model" approach. Performing evaluations with the "Full Model" approach implies the optimization of a large number of model parameters. With increasing neutron incident energy, many residual nuclei produced by nucleon emission also lead to fission. All available experimental data assigned to various fission mechanisms of the same nucleus were used to determine fission barrier parameters. For uranium isotopes, triple-humped fission barriers were required in order to reproduce accurately variations of the experimental fission cross sections. Our BRC fission modeling has shown that the effects of the class II or class III states located in the wells of the fission barrier sometimes provide an anti-resonant transmission rather than a resonant one. Consistent evaluations were produced for a large series of U and Pu isotopes. Resulting files were tested against integral data.

  12. Standard test method for analysis of total and isotopic uranium and total thorium in soils by inductively coupled plasma-mass spectrometry

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2008-01-01

    1.1 This test method covers the measurement of total uranium (U) and thorium (Th) concentrations in soils, as well as the determination of the isotopic weight percentages of 234U, 235U, 236U, and 238U, thereby allowing for the calculation of individual isotopic uranium activity or total uranium activity. This inductively coupled plasma-mass spectroscopy (ICP-MS) method is intended as an alternative analysis to methods such as alpha spectroscopy or thermal ionization mass spectroscopy (TIMS). Also, while this test method covers only those isotopes listed above, the instrumental technique may be expanded to cover other long-lived radioisotopes since the preparation technique includes the preconcentration of the actinide series of elements. The resultant sample volume can be further reduced for introduction into the ICP-MS via an electrothermal vaporization (ETV) unit or other sample introduction device, even though the standard peristaltic pump introduction is applied for this test method. The sample preparatio...

  13. First burnup credit application including actinides and fission products for transport and storage cask by using French experiments

    International Nuclear Information System (INIS)

    The burnup credit (BUC) methodology for a transport and storage cask application, including actinides and fission products, is implemented at AREVA TN using the French BUC calculation route for pressurized water reactor (PWR) UO2 used fuel. The methodology is based on the connection of the French depletion code DARWIN2 and the French criticality safety package CRISTAL V1. The BUC methodology includes the experimental validation of the computation codes dedicated to the calculation of the used fuel inventory calculations. Indeed, the results of the comparison calculation–experiment (C-E)/E allow to determine either a set of isotopic correction factors (ICFs) for the BUC nuclides considered in the criticality calculation or keff-penalty terms directly used for the definition of the keff-acceptance criterion for the criticality assessment of the transport and storage cask. These ICFs or keff-penalty terms are one of the key of the BUC method to guarantee the conservativeness of the fuel reactivity in safety-criticality calculations using BUC approach. A French BUC program has been developed at CEA/Cadarache in the framework of the CEA-AREVA collaboration in order to validate fuel inventory calculations. This program involves two kinds of experiments: chemical analyses and microprobe measurements of PWR irradiated fuel pins (French PIE program) on one hand, and reactivity worth measurements of the BUC nuclides in the MINERVE reactor on the other hand. This paper highlights, through a first industrial AREVA TN's application of the BUC method, including fission products, that the French PIE program and reactivity worth measurements in MINERVE reactor are suitable for the implementation of BUC in transport and storage cask applications loaded with PWR UO2 used fuels assemblies. (author)

  14. Inventory of programs. Calculation of the isotope inventory after a hypothetical accident at the Cofrentes Nuclear power; Calculo del inventario isotopico despues de un hipotetico accidente en la Central Nuclear de Cofrentes

    Energy Technology Data Exchange (ETDEWEB)

    Albendea, M.

    2014-07-01

    Iberdrola is developing a new application to calculate the inventory of radiological material, then of a hypothetical accident, with the name of inventory. This application allows you to calculate the inventory isotopic, analysers and accurate thermal of all or part of the nucleus of the plant of Cofrentes, even of any single element, based on its history of irradiation and specific periods of decay, since the reactor at any time after the shutdown. (Author)

  15. Solubility of actinide surrogates in nuclear glasses

    International Nuclear Information System (INIS)

    This paper discusses the results of a study of actinide surrogates in a nuclear borosilicate glass to understand the effect of processing conditions (temperature and oxidizing versus reducing conditions) on the solubility limits of these elements. The incorporation of cerium oxide, hafnium oxide, and neodymium oxide in this borosilicate glass was investigated. Cerium is a possible surrogate for tetravalent and trivalent actinides, hafnium for tetravalent actinides, and neodymium for trivalent actinides. The material homogeneity was studied by optical, scanning electron microscopy. Cerium LIII XANES spectroscopy showed that the Ce3+/Cetotal ratio increased from about 0.5 to 0.9 as the processing temperature increased from 1100 to 1400 deg. C. Cerium LIII XANES spectroscopy also confirmed that the increased Ce solubility in glasses melted under reducing conditions was due to complete reduction of all the cerium in the glass. The most significant results pointed out in the current study are that the solubility limits of the actinide surrogates increases with the processing temperature and that Ce3+ is shown to be more soluble than Ce4+ in this borosilicate glass

  16. TUCS/phosphate mineralization of actinides

    Energy Technology Data Exchange (ETDEWEB)

    Nash, K.L. [Argonne National Lab., IL (United States)

    1997-10-01

    This program has as its objective the development of a new technology that combines cation exchange and mineralization to reduce the concentration of heavy metals (in particular actinides) in groundwaters. The treatment regimen must be compatible with the groundwater and soil, potentially using groundwater/soil components to aid in the immobilization process. The delivery system (probably a water-soluble chelating agent) should first concentrate the radionuclides then release the precipitating anion, which forms thermodynamically stable mineral phases, either with the target metal ions alone or in combination with matrix cations. This approach should generate thermodynamically stable mineral phases resistant to weathering. The chelating agent should decompose spontaneously with time, release the mineralizing agent, and leave a residue that does not interfere with mineral formation. For the actinides, the ideal compound probably will release phosphate, as actinide phosphate mineral phases are among the least soluble species for these metals. The most promising means of delivering the precipitant would be to use a water-soluble, hydrolytically unstable complexant that functions in the initial stages as a cation exchanger to concentrate the metal ions. As it decomposes, the chelating agent releases phosphate to foster formation of crystalline mineral phases. Because it involves only the application of inexpensive reagents, the method of phosphate mineralization promises to be an economical alternative for in situ immobilization of radionuclides (actinides in particular). The method relies on the inherent (thermodynamic) stability of actinide mineral phases.

  17. Comparison of 138La:139La-isotope-ratio-enhancement calculations by use of spectral-simulation and density-matrix methods

    International Nuclear Information System (INIS)

    The isotope-ratio-enhancement calculations for 138La are carried out using spectral-simulation (SS) and density-matrix (DM) methods for the 5d6s22D3/2-5d6s6p 4F3/20 (753.9-nm) transition that was considered by Young and Shaw [J. Opt. Soc. Am. B 12, 1398-1402 (1995)] a first-step transition in their diode-laser-initiated, resonance-ionization mass spectrometry experiments. The results from the two methods are compared with each other and with the reported experimental result. The SS result is noted to be more sensitive to the residual Doppler width but less sensitive to the laser linewidth than the DM result. It is further noted that under exact correspondence with experimental conditions, the DM result is in much better agreement with the experimental result obtained by Young and Shaw in their two-color resonant, three-photon photoionization of La by use of a narrowband, cw diode laser for the first-step excitation and a broadband, pulsed dye laser for further excitation and ionization

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

    Energy Technology Data Exchange (ETDEWEB)

    Timothy A. Hyde

    2012-06-01

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

  19. 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

  20. Optimization study and neutronic and thermal-hydraulic design calculations of a 75 KWTH aqueous homogeneous reactor for medical isotopes production

    Energy Technology Data Exchange (ETDEWEB)

    Perez, Daniel Milian; Lorenzo, Daniel E. Milian; Garcia, Lorena P. Rodriguez; Llanes, Jesus Salomon; Hernandez, Carlos R. Garcia, E-mail: dperez@instec.cu, E-mail: dmilian@instec.cu, E-mail: lorenapilar@instec.cu, E-mail: cgh@instec.cu [Instituto Superior de Tecnologias y Ciencias Aplicadas (InSTEC), La Habana (Cuba); Lira, Carlos A. Brayner de Oliveira, E-mail: cabol@ufpe.br [Universidade Federal de Pernambuco (UFPE), Recife (Brazil); Rodriguez, Manuel Cadavid, E-mail: mcadavid2001@yahoo.com [Tecnologia Nuclear Medica Spa, TNM (Chile)

    2015-07-01

    {sup 99m}Tc is the most common radioisotope used in nuclear medicine. It is a very useful radioisotope, which is used in about 30-40 million procedures worldwide every year. Medical diagnostic imaging techniques using {sup 99m}Tc represent approximately 80% of all nuclear medicine procedures. Although {sup 99m}Tc can be produced directly on a cyclotron or other type of particle accelerator, currently is almost exclusively produced from the beta-decay of its 66-h parent {sup 99}Mo. {sup 99}Mo production system in an Aqueous Homogeneous Reactor (AHR) is potentially advantageous because of its low cost, small critical mass, inherent passive safety, and simplified fuel handling, processing and purification characteristics. In this paper, an AHR conceptual design using Low Enriched Uranium (LEU) is studied and optimized for the production of {sup 99}Mo. Aspects related with the neutronic behavior such as optimal reflector thickness, critical height, medical isotopes production and the reactivity feedback introduced in the solution by the volumetric expansion of the fuel solution due to thermal expansion of the fuel solution and the void volume generated by radiolytic gas bubbles were evaluated. Thermal-hydraulics studies were carried out in order to show that sufficient cooling capacity exists to prevent fuel overheating. The neutronic and thermal-hydraulics calculations have been performed with the MCNPX computational code and the version 14 of ANSYS CFX respectively. The neutronic calculations demonstrated that the reactor is able to produce 370 six-day curies of {sup 99}Mo in 5 days operation cycles and the CFD simulation demonstrated that the heat removal systems provide sufficient cooling capacity to prevent fuel overheating, the maximum temperature reached by the fuel (89.29 deg C) was smaller to the allowable temperature limit (90 deg C). (author)

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

    International Nuclear Information System (INIS)

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

  2. STRONTIUM AND ACTINIDE SEPARATIONS FROM HIGH LEVEL NUCLEAR WASTE SOLUTIONS USING MONOSODIUM TITANATE 1. SIMULANT TESTING

    Energy Technology Data Exchange (ETDEWEB)

    HOBBS, D. T.; BARNES, M. J.; PULMANO, R. L.; MARSHALL, K. M.; EDWARDS, T. B.; BRONIKOWSKI, M. G.; FINK, S. D.

    2005-04-14

    High-level nuclear waste produced from fuel reprocessing operations at the Savannah River Site (SRS) requires pretreatment to remove {sup 137}Cs, {sup 90}Sr and alpha-emitting radionuclides (i.e., actinides) prior to disposal. Separation processes planned at SRS include caustic side solvent extraction, for {sup 137}Cs removal, and ion exchange/sorption of {sup 90}Sr and alpha-emitting radionuclides with an inorganic material, monosodium titanate (MST). The predominant alpha-emitting radionuclides in the highly alkaline waste solutions include plutonium isotopes {sup 238}Pu, {sup 239}Pu and {sup 240}Pu. This paper provides a summary of data acquired to measure the performance of MST to remove strontium and actinides from simulated waste solutions. These tests evaluated the influence of ionic strength, temperature, solution composition and the oxidation state of plutonium.

  3. Actinides and lanthanides under pressure: the pseudopotential approach; Actinides et terres rares sous pression: approche pseudopotentiel

    Energy Technology Data Exchange (ETDEWEB)

    Richard, N

    2002-07-01

    In the Density Functional Theory Framework, the pseudopotential formalism offers a broader scope of study than other theoretical methods such as global relaxation of the parameters of the cell or ab initio molecular dynamics simulations. This method has been widely used to study light elements or transition metals but never to study f elements. We have generated two non local norm conserving Trouillier-Martins pseudopotentials (one in LDA and one in GGA) for the cerium. To check the validity of the pseudopotentials, we have calculated the equilibrium volume and the incompressibility modulus and compared our results to previous all-electron calculations. If the GGA and non linear core corrections are used, the equation of state is in a good agreement with the experimental equation of state. A static study of the previously proposed high pressure phases give a transitions fcc-a''(I)-bct. Using the pseudopotentials we have generated, an ab initio molecular dynamics simulation at constant pressure, in the region between 5 and 12 GPa where the stable phase of cerium is not well defined, lead us to predict that a centred monoclinic structure, as the a''(I) phase previously observed in some experiments, is the most stable phase. We have also generated pseudopotentials for the light actinides (Th, Pa, U and Np). We have study their phase transitions under pressure at zero temperature. We compared our results with all electron results. The structure parameters have always been relaxed in this study. And for the first time in pseudopotential calculation, the spin-orbit coupling has been taken into account. The curves describing the variation of the volume or the incompressibility modulus depending on the elements and the phase transitions are always in agreement with the one found in the all electron calculations. (author)

  4. Research on Actinides in Nuclear Fuel Cycles

    International Nuclear Information System (INIS)

    The electrochemical/spectroscopic integrated measurement system was designed and set up for spectro-electrochemical measurements of lanthanide and actinide ions in high temperature molten salt media. A compact electrochemical cell and electrode system was also developed for the minimization of reactants, and consequently minimization of radioactive waste generation. By applying these equipment, oxidation and reduction behavior of lanthanide and actinide ions in molten salt media have been made. Also, thermodynamic parameter values are determined by interpreting the results obtained from electrochemical measurements. Several lanthanide ions exhibited fluorescence properties in molten salt. Also, UV-VIS measurement provided the detailed information regarding the oxidation states of lanthanide and actinide ions in high temperature molten salt media

  5. The analysis and handling concept of minor actinides of NPP’s waste by using Ads technology

    International Nuclear Information System (INIS)

    The contents of minor actinide elements (americium, neptunium and curium) on the spent fuel inventory from PWR operation of NPP have been calculated using Vista program. The calculation used parameters: enrichment 3.968%, power 1000 M We and burn-up is 60 M Wd/kg. The result of calculation showed that the arising of minor actinide elements on the spent fuel is 16.205 kg/year and 43.471 kg/year for PWR-UOX and PWR-MOX respectively. It is also discussed a concept of the use of ADS technology for transmuting the minor actinide elements contained in spent fuels. The result of the discussion showed that an ADS of 400 M Wth will serve 7 PWRs-UOX, and on the PWR system using UOX and MOX fuels an ADS will serve 3 PWRs. (author)

  6. Oak Ridge National Laboratory's isotope enrichment program

    International Nuclear Information System (INIS)

    The Isotope Enrichment Program (IEP) at Oak Ridge National Laboratory (ORNL) is responsible for the production and distribution of ∼225 enriched stable isotopes from 50 multi-isotopic elements. In addition, ORNL distributes enriched actinide isotopes and provides extensive physical- and chemical-form processing of enriched isotopes to meet customer requirements. For more than 50 yr, ORNL has been a major provider of enriched isotopes and isotope-related services to research, medical, and industrial institutions throughout the world. Consolidation of the Isotope Distribution Office (IDO), the Isotope Research Materials Laboratory (IRML), and the stable isotope inventories in the Isotope Enrichment Facility (IEF) have improved operational efficiencies and customer services. Recent changes in the IEP have included adopting policies for long-term contracts, which offer program stability and pricing advantages for the customer, and prorated service charges, which greatly improve pricing to the small research users. The former U.S. Department of Energy (DOE) Loan Program has been converted to a lease program, which makes large-quantity or very expensive isotopes available for nondestructive research at a nominal cost. Current efforts are being pursued to improve and expand the isotope separation capabilities as well as the extensive chemical- and physical-form processing that now exists. The IEF's quality management system is ISO 9002 registered and accredited in the United States, Canada, and Europe

  7. International Workshop on Orbital and Spin Magnetism of Actinides (IWOSMA-3)

    Energy Technology Data Exchange (ETDEWEB)

    Temmerman, W; Tobin, J; der Laan, G v

    2006-11-08

    This International Workshop on Orbital and Spin Magnetism of Actinides (IWOSMA) is the third in a series. The first workshop took place in Daresbury in 1999 and the second in Berkeley, CA, USA in 2002. These workshops are informal gatherings of theoreticians and experimentalists addressing the latest issues in the electronic and magnetic properties of actinides. The magnetism of transition metal systems and lanthanide systems is now fairly well understood, where d and f electrons can be described in a delocalized and localized model, respectively. On the other hand, actinide systems do not fit in such a description. The localization of the 5f is in between that of the 3d and 4f and the strong spin-orbit interaction necessitates a relativistic approach. Furthermore, electron correlation effects play a major role in these compounds. Recently, it has become possible to determine element-specific magnetic moments using neutron diffraction and x-ray scattering and absorption. The latter technique makes it even possible to separate the orbital and spin contribution to the total magnetic moment. The results are very interesting but difficult to reproduce with present state-of-art calculations. Not only a very large orbital polarization but also a large magnetic dipole term has been measured in cubic compounds, such as US. This allows for severe testing of the extra terms included in band theory to account for orbital polarization. It is also clear that deeper insight in magnetism can be obtained by studying the unusual behavior of the actinides. The recent development and application of such techniques as DMFT could contribute to the understanding of magnetism in actinides. Despite the fact that actinides for health reasons will find less application in technological market products, the understanding of their magnetic and electronic properties will no doubt provide key elements for a general description of electron correlation and relativistic effects.

  8. Actinide phosphonate complexes in aqueous solutions

    International Nuclear Information System (INIS)

    Complexes formed by actinides with carboxylic acids, polycarboxylic acids, and aminopolycarboxylic acids play a central role in both the basic and process chemistry of the actinides. Recent studies of f-element complexes with phosphonic acid ligands indicate that new ligands incorporating doubly ionizable phosphonate groups (-PO3H2) have many properties which are unique chemically, and promise more efficient separation processes for waste cleanup and environmental restoration. Simple diphosphonate ligands form much stronger complexes than isostructural carboxylates, often exhibiting higher solubility as well. In this manuscript recent studies of the thermodynamics and kinetics of f-element complexation by 1,1 and 1,2 diphosphonic acid ligands are described

  9. Sequential analysis of selected actinides in urine

    International Nuclear Information System (INIS)

    The monitoring of personnel by urinalysis for suspected contamination by actinides necessitated the development and implementation of an analytical scheme that will separate and identify alpha emitting radionuclides of these elements. The present work deals with Pu, Am, and Th. These elements are separated from an ashed urine sample by means of coprecipitation and ion exchange techniques. The final analysis is carried out by electroplating the actinides and counting in a α-spectrometer. Mean recoveries of these elements from urine are: Pu 64%, Am 74% and Th 69%. (auth)

  10. Spin–orbit coupling in actinide cations

    DEFF Research Database (Denmark)

    Bagus, Paul S.; Ilton, Eugene S.; Martin, Richard L.;

    2012-01-01

    The limiting case of Russell–Saunders coupling, which leads to a maximum spin alignment for the open shell electrons, usually explains the properties of high spin ionic crystals with transition metals. For actinide compounds, the spin–orbit splitting is large enough to cause a significantly reduc...... spin alignment. Novel concepts are used to explain the dependence of the spin alignment on the 5f shell occupation. We present evidence that the XPS of ionic actinide materials may provide direct information about the angular momentum coupling within the 5f shell....

  11. Actinide elements in aquatic and terrestrial environments

    International Nuclear Information System (INIS)

    Progress is reported on the following research projects: water-sediment interactions of U, Pu, Am, and Cm; relative availability of actinide elements from abiotic to aquatic biota; comparative uptake of transuranic elements by biota bordering Pond 3513; metabolic reduction of 239Np from Np(V) to Np(IV) in cotton rats; evaluation of hazards associated with transuranium releases to the biosphere; predicting Pu in bone; adsorption--solubility--complexation phenomena in actinide partitioning between sorbents and solution; comparative soil extraction data; and comparative plant uptake data

  12. Actinide and fission product separation and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1993-07-01

    The second international information exchange meeting on actinide and fission product separation and transmutation, took place in Argonne National Laboratory in Illinois United States, on 11-13 November 1992. The proceedings are presented in four sessions: Current strategic system of actinide and fission product separation and transmutation, progress in R and D on partitioning processes wet and dry, progress in R and D on transmutation and refinements of neutronic and other data, development of the fuel cycle processes fuel types and targets. (A.L.B.)

  13. Actinide and fission product separation and transmutation

    International Nuclear Information System (INIS)

    The second international information exchange meeting on actinide and fission product separation and transmutation, took place in Argonne National Laboratory in Illinois United States, on 11-13 November 1992. The proceedings are presented in four sessions: Current strategic system of actinide and fission product separation and transmutation, progress in R and D on partitioning processes wet and dry, progress in R and D on transmutation and refinements of neutronic and other data, development of the fuel cycle processes fuel types and targets. (A.L.B.)

  14. LWR decay heat calculations using a GRS improved ENDF/B-6 based ORIGEN data library

    Energy Technology Data Exchange (ETDEWEB)

    Hesse, U.; Hummelsheim, K.I.; Kilger, R.; Moser, F.E.; Langenbuch, S. [Gesellschaft fur Anlagen- und Reaktorsicherheit (GRS) mbH, Forschungsinstitute, Garching (Germany)

    2008-07-01

    The known ORNL ORIGEN code is widely spread over the world for inventory, activity and decay heat tasks and is used stand-alone or implemented in activation, shielding or burn-up systems. More than 1000 isotopes with more than six coupled neutron capture and radioactive decay channels are handled simultaneously by the code. The characteristics of the calculated inventories, e.g., masses, activities, neutron and photon source terms or the decay heat during short or long decay time steps are achieved by summing over all isotopes, characterized in the ORIGEN libraries. An extended nuclear GRS-ORIGENX data library is now developed for practical appliance. The library was checked for activation tasks of structure material isotopes and for actinide and fission product burn-up calculations compared with experiments and standard methods. The paper is directed to the LWR decay heat calculation features of the new library and shows the differences of dynamical and time integrated results of Endf/B-6 based and older Endf/B-5 based libraries for decay heat tasks compared to fission burst experiments, ANS curves and some other published data. A multi-group time exponential evaluation is given for the fission burst power of {sup 235}U, {sup 238}U, {sup 239}Pu and {sup 241}Pu, to be used in quick LWR reactor accident decay heat calculation tools. (authors)

  15. Measurement of electro-sprayed 238 and 239+240 plutonium isotopes using 4{pi}-alpha spectrometry. Application to environmental samples; Spectrometrie alpha 4{pi} de sources d'actinides realisees par electronebulisation. Developpement et optimisation d'un protocole applique au mesurage des isotopes 238 et 239+240 du plutonium dans l'environnement

    Energy Technology Data Exchange (ETDEWEB)

    Charmoille-Roblot, M. [CEA/Fontenay-aux-Roses, Dept. de Protection de l' Environnement (DPRE), 92 (France)]|[Paris-11 Univ., 91 - Orsay (France)

    1999-07-01

    A new protocol for plutonium deposition using the electro-spray technique coupled with 4{pi}-{alpha} spectrometry is proposed to improve the detection limit, shorten the counting time. In order to increase the detection efficiency, it was proposed to measure 238 and 239+240 plutonium isotopes electro-sprayed deposit simultaneously on both sides of the source support, that must be as transparent as possible to alpha-emissions, in a two-alpha detectors chamber. A radiochemical protocol was adapted to electro-spray constraints and a very thin carbon foil was selected for 4{pi} -alpha spectrometry. The method was applied to a batch of sediment samples and gave the same results as an electrodeposited source measured using conventional alpha spectrometry with a 25 % gain on counting time and 10 % on plutonium 238 detection limit. Validation and application of the technique have been made on reference samples. (author)

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-09-23

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

  17. Chemical compatibility of HLW borosilicate glasses with actinides

    International Nuclear Information System (INIS)

    During liquid storage of HLLW the formation of actinide enriched sludges is being expected. Also during melting of HLW glasses an increase of top-to-bottom actinide concentrations can take place. Both effects have been studied. Besides, the vitrification of plutonium enriched wastes from Pu fuel element fabrication plants has been investigated with respect to an isolated vitrification process or a combined one with the HLLW. It is shown that the solidification of actinides from HLLW and actinide waste concentrates will set no principal problems. The leaching of actinides has been measured in salt brine at 230C and 1150C. (orig.)

  18. Actinide recycle in LMFBRs as a waste management alternative

    Energy Technology Data Exchange (ETDEWEB)

    Beaman, S.L.

    1979-08-21

    A strategy of actinide burnup in fast reactor systems has been investigated as an approach for reducing the long term hazards and storage requirements of the actinide waste elements and their decay daughters. The actinide recycle studies also included plutonium burnup studies in the event that plutonium is no longer required as a fuel. Particular emphasis was placed upon the timing of the recycle program, the requirements for separability of the waste materials, and the impact of the actinides on the reactor operations and performance. It is concluded that actinide recycle and plutonium burnout are attractive alternative waste management concepts. 25 refs., 14 figs., 34 tabs.

  19. Cross sections for fuel depletion and radioisotope production calculations in TRIGA reactors

    International Nuclear Information System (INIS)

    For TRIGA Reactors, the fuel depletion and isotopic inventory calculations, depends on the computer code and in the cross sections of some important actinides used. Among these we have U-235, U-238, Pu-239, Pu-240 and Pu-241. We choose ORIGEN2, a code with a good reputation in this kind of calculations, we observed the cross sections for these actinides in the libraries that we have (PWR's and BWR), the fission cross section for U-235 was about 50 barns. We used a PWR library and our results were not satisfactory, specially for standard elements. We decided to calculate cross sections more suitable for our reactor, for that purpose we simulate the standard and FLIP TRIGA cells with the transport code WIMS. We used the fuel average flux and COLAPS (a home made program), to generate suitable cross sections for ORIGEN2, by collapsing the WIMS library cross sections of these nuclides. For the radioisotope production studies using the Central Thimble, we simulate the A and B rings and used the A average flux to collapse cross sections. For these studies, the required nuclides sometimes are not present in WIMS library, for them we are planning to process the ENDF/B data, with NJOY system, and include the cross sections to WIMS library or to collapse them using the appropriate average-flux and the program COLAPS. (author)

  20. 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

  1. Energy-Dependent Fission Q Values Generalized for All Actinides

    Energy Technology Data Exchange (ETDEWEB)

    Vogt, R

    2008-09-25

    We generalize Madland's parameterization of the energy release in fission to obtain the dependence of the fission Q values on incident neutron energy, E{sub n}, for all major and minor actinides. These Q(E{sub n}) parameterizations are included in the ENDL2008 release. This paper describes calculations of energy-dependent fission Q values based on parameterizations of the prompt energy release in fission [1], developed by Madland [1] to describe the prompt energy release in neutron-induced fission of {sup 235}U, {sup 238}U, and {sup 239}Pu. The energy release is then related to the energy deposited during fission so that experimentally measurable quantities can be used to obtain the Q values. A discussion of these specific parameterizations and their implementation in the processing code for Monte Carlo neutron transport, MCFGEN, [2] is described in Ref. [3]. We extend this model to describe Q(E) for all actinides, major and minor, in the Evaluated Nuclear Data Library (ENDL) 2008 release, ENDL2008.

  2. Numerical analysis on reduction of radioactive actinides by recycling of nuclear fuel

    International Nuclear Information System (INIS)

    Worldwide, human growth has reached unparalleled levels historically, this implies a need for more energy, and just in 2007 was consumed in the USA 4157 x 109 kWh of electricity and there were 6 x 109 metric tons of carbon dioxide, which causes a devastating effect on our environment. To this problem, a solution to the demand for non-fossil energy is nuclear energy, which is one of the least polluting and the cheapest among non-fossil energy; however, a problem remains unresolved the waste generation of nuclear fuels. In this work the option of a possible transmutation of actinides in a nuclear reactor of BWR was analyzed, an example of this are the nuclear reactors at the Laguna Verde nuclear power plant, which have generated spent fuel stored in pools awaiting a decision for final disposal or any other existing alternative. Assuming that the spent fuel was reprocessed to separate useful materials and actinides such as plutonium and uranium remaining, could take these actinides and to recycle them inside the same reactor that produced them, so il will be reduced the radiotoxicity of spent fuel. The main idea of this paper is to evaluate by means of numeric simulation (using the Core Management System (CMS)) the reduction of minor actinides in the case of being recycled in fresh fuel of the type BWR. The actinides were introduced hypothetically in the fuel pellets to 6% by weight, and then use a burned in the range of 0-65 G Wd/Tm, in order to have a better panorama of their behavior and thus know which it is the best choice for maximum reduction of actinides. Several cases were studied, that is to say were used as fuels; the UO2 and MOX. Six different cases were also studied to see the behavior of actinides in different situations. The CMS platform calculation was used for the analysis of the cases presented. Favorable results were obtained, having decreased from a range of 35% to 65% of minor actinides initially introduced in the fuel rods, reducing the

  3. Some aspects of risk reduction strategy by multiple recycling in fast burner reactors of the plutonium and minor actinide inventories

    International Nuclear Information System (INIS)

    The paper shows the impact of recycling LWR-MOX fuel in a fast burner reactor on the plutonium (Pu) and minor actinide (MA) inventories and on the related radio activities. Reprocessing of the targets for multiple recycling will become increasingly difficult as the burn up increases. Multiple recycling of Pu + MA in fast reactors is a feasible option which has to be studied very carefully: the Pu (except the isotopes Pu-238 and Pu-240), Am and Np levels decrease as a function of the recycle number, while the Cm-244 level accumulates and gradually transforms into Cm-245. Long cooling times (10 + 2 years) are necessary with aqueous processing. The paper discusses the problems associated with multiple reprocessing of highly active fuel types and particularly the impact of Pu-238, Am-241 and Cm-244 on the fuel cycle operations. The calculations were performed with the zero-dimensional ORIGEN-2 code. The validity of the results depends on that of the code and its cross section library. The time span to reduce the initial inventory of Pu + MA by a factor of 10, amounts to 255 years when average burn ups are limited to 150 GWd t-1. (orig.)

  4. Evaluation of fission product worth margins in PWR spent nuclear fuel burnup credit calculations

    International Nuclear Information System (INIS)

    Current criticality safety calculations for the transportation of irradiated LWR fuel make the very conservative assumption that the fuel is fresh. This results in a very substantial overprediction of the actual keff of the transportation casks; in certain cases, this decreases the amount of spent fuel which can be loaded in a cask, and increases the cost of transporting the spent fuel to the repository. Accounting for the change of reactivity due to fuel depletion is usually referred to as ''burnup credit.'' The US DOE is currently funding a program aimed at establishing an actinide only burnup credit methodology (in this case, the calculated reactivity takes into account the buildup or depletion of a limited number of actinides). This work is undergoing NRC review. While this methodology is being validated on a significant experimental basis, it implicitly relies on additional margins: in particular, the absorption of neutrons by certain actinides and by all fission products is not taken into account. This provides an important additional margin and helps guarantee that the methodology is conservative provided these neglected absorption are known with reasonable accuracy. This report establishes the accuracy of fission product absorption rate calculations: (1) the analysis of European fission product worth experiments demonstrates that fission product cross-sections available in the US provide very good predictions of fission product worth; (2) this is confirmed by a direct comparison of European and US cross section evaluations; (3) accuracy of Spent Nuclear Fuel (SNF) fission product content predictions is established in a recent ORNL report where several SNF isotopic assays are analyzed; and (4) these data are then combined to establish in a conservative manner the fraction of the predicted total fission product absorption which can be guaranteed based on available experimental data

  5. Evaluation of fission product worth margins in PWR spent nuclear fuel burnup credit calculations.

    Energy Technology Data Exchange (ETDEWEB)

    Blomquist, R.N.; Finck, P.J.; Jammes, C.; Stenberg, C.G.

    1999-02-17

    Current criticality safety calculations for the transportation of irradiated LWR fuel make the very conservative assumption that the fuel is fresh. This results in a very substantial overprediction of the actual k{sub eff} of the transportation casks; in certain cases, this decreases the amount of spent fuel which can be loaded in a cask, and increases the cost of transporting the spent fuel to the repository. Accounting for the change of reactivity due to fuel depletion is usually referred to as ''burnup credit.'' The US DOE is currently funding a program aimed at establishing an actinide only burnup credit methodology (in this case, the calculated reactivity takes into account the buildup or depletion of a limited number of actinides). This work is undergoing NRC review. While this methodology is being validated on a significant experimental basis, it implicitly relies on additional margins: in particular, the absorption of neutrons by certain actinides and by all fission products is not taken into account. This provides an important additional margin and helps guarantee that the methodology is conservative provided these neglected absorption are known with reasonable accuracy. This report establishes the accuracy of fission product absorption rate calculations: (1) the analysis of European fission product worth experiments demonstrates that fission product cross-sections available in the US provide very good predictions of fission product worth; (2) this is confirmed by a direct comparison of European and US cross section evaluations; (3) accuracy of Spent Nuclear Fuel (SNF) fission product content predictions is established in a recent ORNL report where several SNF isotopic assays are analyzed; and (4) these data are then combined to establish in a conservative manner the fraction of the predicted total fission product absorption which can be guaranteed based on available experimental data.

  6. Actinide and fission product partitioning and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1995-07-01

    The third international information exchange meeting on actinide and fission product partitioning and transmutation, took place in Cadarache France, on 12-14 December 1994. The proceedings are presented in six sessions : an introduction session, the major programmes and international cooperation, the systems studies, the reactors fuels and targets, the chemistry and a last discussions session. (A.L.B.)

  7. Treatment of actinide-containing organic waste

    International Nuclear Information System (INIS)

    A method has been developed for reducing the volume of organic wastes and recovering the actinide elements. The waste, together with gaseous oxygen (air) is introduced into a molten salt, preferably an alkali metal carbonate such as sodium carbonate. The bath is kept at 7500 - 10000C and 0.5 - 10 atm to thermally decompose and partially oxidize the waste, while substantially reducing its volume. The gaseous effluent, mainly carbon dioxide and water vapour, is vented to the atmosphere through a series of filters to remove trace amounts of actinide elements or particulate alkali metal salts. The remaining combustion products are entrained in the molten salt. Part of the molten salt-combustion product mixture is withdrawn and mixed with an aqueous medium. Insoluble combustion products are then removed from the aqueous medium and are leached with a mixture of hydrofluoric and nitric acids to solubilize the actinide elements. The actinide elements are easily recovered from the acid solution using conventional techniques. (DN)

  8. Report of the panel on inhaled actinides

    International Nuclear Information System (INIS)

    Some topics discussed are as follows: assessment of risks to man of inhaling actinides; use of estimates for developing protection standards; epidemiology of lung cancer in exposed human populations; development of respiratory tract models; and effects in animals: dose- and effect-modifying factors

  9. Actinide and fission product partitioning and transmutation

    International Nuclear Information System (INIS)

    The third international information exchange meeting on actinide and fission product partitioning and transmutation, took place in Cadarache France, on 12-14 December 1994. The proceedings are presented in six sessions : an introduction session, the major programmes and international cooperation, the systems studies, the reactors fuels and targets, the chemistry and a last discussions session. (A.L.B.)

  10. Placental transfer of plutonium and other actinides

    International Nuclear Information System (INIS)

    The report is based on an extensive literature search. All data available from studies on placental transfer of plutonium and other actinides in man and animals have been collected and analysed, and the report presents the significant results as well as unresolved questions and knowledge gaps which may serve as a waypost to future research work. (orig./MG)

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

    Energy Technology Data Exchange (ETDEWEB)

    Allender, Jeffrey S. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Bridges, Nicholas J. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Loftin, Bradley M. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Dunsmuir, Michael D. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-07-14

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

  12. Statistical clumped isotope signatures.

    Science.gov (United States)

    Röckmann, T; Popa, M E; Krol, M C; Hofmann, M E G

    2016-01-01

    High precision measurements of molecules containing more than one heavy isotope may provide novel constraints on element cycles in nature. These so-called clumped isotope signatures are reported relative to the random (stochastic) distribution of heavy isotopes over all available isotopocules of a molecule, which is the conventional reference. When multiple indistinguishable atoms of the same element are present in a molecule, this reference is calculated from the bulk (≈average) isotopic composition of the involved atoms. We show here that this referencing convention leads to apparent negative clumped isotope anomalies (anti-clumping) when the indistinguishable atoms originate from isotopically different populations. Such statistical clumped isotope anomalies must occur in any system where two or more indistinguishable atoms of the same element, but with different isotopic composition, combine in a molecule. The size of the anti-clumping signal is closely related to the difference of the initial isotope ratios of the indistinguishable atoms that have combined. Therefore, a measured statistical clumped isotope anomaly, relative to an expected (e.g. thermodynamical) clumped isotope composition, may allow assessment of the heterogeneity of the isotopic pools of atoms that are the substrate for formation of molecules. PMID:27535168

  13. Study of strontium extraction as cryptate complex in view to 102 element separation from the actinides

    International Nuclear Information System (INIS)

    In the present report is studied in detail the extraction of strontium, in tracer amounts, as cryptate and its separation from the lanthanides and transplutonium elements with a high degree of purification. Influence of different parameters: pH of the aqueous phase, cryptant concentration, counteranion concentration, nature of the solvent are investigated. It is intended to use this method to separate the 102 element from actinides in the study of the isotope 102 259 produced in irradiation of a curium 248 target by oxygen 18 ions

  14. Characterization and development of an active scintillating target for nuclear reaction studies on actinides

    International Nuclear Information System (INIS)

    This article presents the development of a new kind of active actinide target, based on organic liquid scintillators containing the dissolved isotope. Amongst many advantages one can mention the very high detection efficiency, the Pulse Shape Discrimination capability, the fast response allowing high count rates and good time resolution and the ease of fabrication. The response of this target to fission fragments has been studied. The discrimination of alpha, fission and proton recoil events is demonstrated. The alpha decay and fission detection efficiencies are simulated and compared to measurements. Finally the use of such a target in the context of fast neutron induced reactions is discussed.

  15. Calculation of Transactinide Homolog Isotope Production Reactions Possible with the Center for Accelerator Mass Spectrometry (CAMS) at Lawrence Livermore National Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Moody, K J; Shaughnessy, D A; Gostic, J M

    2011-11-29

    for evaluation of homolog chemical properties. CAMS also offers an environment for testing these systems 'online' by incorporating automated chemical systems into the beamline so that tracers can be created, transported, and chemically separated all on the shorter timescales required for transactinide experiments. Even though CAMS is limited in the types and energies of ions they can accelerate, there are still a wide variety of reactions that can be performed there with commercially available target materials. The half-lives of these isotopes vary over a range that could be used for both online chemistry (where shorter half-lives are required) and benchtop tracers studies (where longer lived isotopes are preferred). In this document, they present a summary of tracer production reactions that could be performed at CAMS, specifically for online, automated chemical studies. They are from chemical groups four through seven, 13, and 14, which would be appropriate for studies of elements 104-107, 113, and 114. Reactions were selected that had (a) commercially available target material, (b) half-lives long enough for transport from a target chamber to an automated chemistry system, and (c) cross-sections at CAMS available projectile energies that were large enough to produce enough atoms to result in a statistically relevant signal after losses for transport and chemistry were considered. In addition, the resulting product atoms had to decay with an observable gamma-ray using standard Ge gamma-ray detectors. The table includes calculations performed for both metal targets and their corresponding oxides.

  16. Actinide collisions for QED and superheavy elements with the time-dependent Hartree-Fock theory and the Balian-Vénéroni variational principle

    Directory of Open Access Journals (Sweden)

    Kedziora David J.

    2011-10-01

    produce transfermium nuclei (Z > 100 in the collision of prolate deformed actinides such as 232Th+250Cf. The collision of the tip of one nucleus with the side of the other results in a nucleon flux toward the latter. The probability distributions for transfermium production in such a collision are computed. The produced nuclei are more neutron-rich than those formed in fusion reactions, thus, leading to more stable isotopes closer to the predicted superheavy island of stability. In addition to mass and charge dispersion, the Balian-Veneroni variational principle is used to compute correlations between Z and N distributions, which are zero in standard TDHF calculations.

  17. The electronic g matrix of some actinide complexes

    International Nuclear Information System (INIS)

    Complete text of publication follows: The molecular g-factors are crucial parameters in Electron Paramagnetic Resonance (EPR) spectroscopy. They parametrize the Zeeman effect that involves the interaction of a spin magnetic moment with a magnetic field. Before the 90's, g-factors were mostly calculated by semi-empirical methods while in the last decade, ab initio techniques have been developed based on wave functions or density functional theories either using a sum over states (SOS) expansion or using response theory [1]. We have recently proposed an alternative method based on wave function theory including spin-orbit effects by the SO-RASSI method [2]. This method has been applied with success to small molecules containing atoms until the third series of the transition metals and to a mixed-valence bimetallic complex[3] and in this work, it is applied to actinide complexes with a 5f1 configuration. To our knowledge, only few attempts have been made to calculate g-factors of actinide complexes from first principles [4, 5]. Relativistic effects in actinide complexes are important, so the deviation of g-factors from the value of the free electron is large and can even become negative. Most of the experiments measuring magnetic properties of actinide complexes date from the sixties. EPR and magnetic susceptibilities give the absolute values of the g-factors while experiment using circularly polarized light provide the sign of the product of the three factors. Magnetic properties of these compounds are easily understood using ligand field theory models. In the first part of this presentation, we will discuss the arbitrary character of the g-matrix and specially of the effect of phase factors and of the choice of the spin quantification axis and we will show that only the G tensor gg* has a physical significance. In the second part, equilibrium distances, excitation energies and g-factors of the AnXq-6 series with An = Pa,U,Np and X = F,Cl,Br are calculated using the

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

    Energy Technology Data Exchange (ETDEWEB)

    Pagano, Justin [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2016-01-08

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

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

    International Nuclear Information System (INIS)

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

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

    Science.gov (United States)

    Van Der Sluys, William G.; Burns, Carol J.; Smith, David C.

    1992-01-01

    A process of preparing an actinide compound of the formula An.sub.x Z.sub.y wherein An is an actinide metal atom selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, x is selected from the group consisting of one, two or three, Z is a main group element atom selected from the group consisting of nitrogen, phosphorus, oxygen and sulfur and y is selected from the group consisting of one, two, three or four, by admixing an actinide organometallic precursor wherein said actinide is selected from the group consisting of thorium, uranium, plutonium, neptunium, and americium, a suitable solvent and a protic Lewis base selected from the group consisting of ammonia, phosphine, hydrogen sulfide and water, at temperatures and for time sufficient to form an intermediate actinide complex, heating said intermediate actinide complex at temperatures and for time sufficient to form the actinide compound, and a process of depositing a thin film of such an actinide compound, e.g., uranium mononitride, by subliming an actinide organometallic precursor, e.g., a uranium amide precursor, in the presence of an effectgive amount of a protic Lewis base, e.g., ammonia, within a reactor at temperatures and for time sufficient to form a thin film of the actinide compound, are disclosed.

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

    Science.gov (United States)

    Marston, Brad; Horowitz, Steven

    2010-03-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Landa, A; Soderlind, P

    2005-11-04

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

  3. Summary Report of Second Research Coordination Meeting on Prompt Fission Neutron Spectra of Major Actinides

    International Nuclear Information System (INIS)

    A summary is given of the Second Research Coordination Meeting on Prompt Fission Neutron Spectra of Actinides. Experimental data and modelling methods on prompt fission neutron spectra were reviewed. Extensive technical discussions held on theoretical methods to calculate prompt fission spectra. Detailed coordinated research proposals have been agreed. Summary reports of selected technical presentations at the meeting are given. The resulting work plan of the Coordinated Research Programme is summarized, along with actions and deadlines. (author)

  4. A review and assessment of some thermodynamic representations of solid solutions of the actinide oxides

    International Nuclear Information System (INIS)

    A review is presented of some of the published thermodynamic representations for binary, ternary and higher-order oxide systems of the actinide and lanthanide elements. These have been assessed by comparing calculated results with experimental values obtained from the literature. The incorporation of these models into the program SOL-GASMIX, which may be used to determine the phase relationships in a multicomponent system, is also described. (author)

  5. Detecting isotopic ratio outliers

    International Nuclear Information System (INIS)

    An alternative method is proposed for improving isotopic ratio estimates. This method mathematically models pulse-count data and uses iterative reweighted Poisson regression to estimate model parameters to calculate the isotopic ratios. This computer-oriented approach provides theoretically better methods than conventional techniques to establish error limits and to identify outliers. 6 refs., 3 figs., 3 tabs

  6. Microbial Transformations of Actinides and Other Radionuclides

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-01-07

    Microorganisms can affect the stability and mobility of the actinides and other radionuclides released from nuclear fuel cycle and from nuclear fuel reprocessing plants. Under appropriate conditions, microorganisms can alter the chemical speciation, solubility and sorption properties and thus could increase or decrease the concentrations of radionuclides in solution in the environment and the bioavailability. Dissolution or immobilization of radionuclides is brought about by direct enzymatic action or indirect non-enzymatic action of microorganisms. Although the physical, chemical, and geochemical processes affecting dissolution, precipitation, and mobilization of radionuclides have been extensively investigated, we have only limited information on the effects of microbial processes and biochemical mechanisms which affect the stability and mobility of radionuclides. The mechanisms of microbial transformations of the major and minor actinides U, Pu, Cm, Am, Np, the fission products and other radionuclides such as Ra, Tc, I, Cs, Sr, under aerobic and anaerobic conditions in the presence of electron donors and acceptors are reviewed.

  7. Interaction of actinide cations with synthetic polyelectrolytes

    International Nuclear Information System (INIS)

    The binding of Am+3, Th+4 and UO2+2 to polymaleic acid, polyethylenemaleic acid and polymethylvinylethermaleic acid has been measured by a solvent extraction technique at 250C and either 0.02 or 0.10 M ionic strength. The solutions were buffered over a pH range such that the percent of carboxylate groups ionized ranged from 25 to 74%. The binding was described by two constants, β1 and β2, which were evaluated after correction for complexation of the actinide cations by acetate and hydrolysis. For comparable degrees of ionization, all three polyelectrolytes showed similar binding strengths. In general, these results indicated that the binding of actinides to these synthetic polyelectrolytes is basically similar to that of natural polyelectrolytes such as humic and fulvic acids. (orig.)

  8. Actinide and fission product separation and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1991-07-01

    The first international information exchange meeting on actinide and fission product separation and transmutation, took place in Mito in Japan, on 6-8 November 1990. It starts with a number of general overview papers to give us some broad perspectives. Following that it takes a look at some basic facts about physics and about the quantities of materials it is talking about. Then it proceeds to some specific aspects of partitioning, starting with evolution from today commercially applied processes and going on to other possibilities. At the end of the third session it takes a look at the significance of partitioning and transmutation of actinides before it embarks on two sessions on transmutation, first in reactors and second in accelerators. The last session is designed to throw back into the discussion the main points which need to be looked at when considering future work in this area. (A.L.B.)

  9. Actinides: from heavy fermions to plutonium metallurgy

    International Nuclear Information System (INIS)

    The actinide elements mark the emergence of 5f electrons. The f electrons possess sufficiently unusual characteristics that their participation in atomic binding often result in dramatic changes in properties. This provides an excellent opportunity to study the question of localization of electrons; a question that is paramount in predicting the physical and chemical properties of d and f electron transition metals. The transition region between localized (magnetic) and itinerant (often superconducting) behavior provides for many interesting phenomena such as structural instabilities (polymorphism), spin fluctuations, mixed valences, charge density waves, exceptional catalytic activity and hydrogen storage. This region offers most interesting behavior such as that exhibited by the actinide compounds UBe13 and UPt3. Both compounds are heavy-fermion superconductors in which both magnetic and superconducting behavior exist in the same electrons. The consequences of f-electron bonding (which appears greatest at Plutonium) show dramatic effects on phase stability, alloying behavior, phase transformations and mechanical behavior

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

    International Nuclear Information System (INIS)

    A joint research program involving the United States and the United Kingdom was initiated about four years ago for the purpose of studying the fuel behavior of higher actinides using in-core irradiation in the fast reactor at Dounreay, Scotland. Simultaneously, determination of integral cross sections of a wide variety of higher actinide isotopes (physics specimens) was proposed. Coincidental neutron flux and energy spectral measurements were to be made using vanadium encapsulated dosimetry materials in the immediate region of the fuel pellets and physics samples. The higher actinide samples chosen for the fuel study were 241Am and 244Cm in the forms of Am2O3, Cm2O3, and Am6Cm(RE)7O21, where (RE) represents a mixture of lanthanides. Milligram quantities of actinide oxides of 248Cm, 246Cm, 244Cm, 243Cm, 243Am, 241Am, 244Pu, 242Pu, 241Pu, 240Pu, 239Pu, 238Pu, 237Np, 238U, 236U, 235U, 234U, 233U, 232Th, 230Th, and 231Pa were encapsulated to obtain nuclear cross section and reaction rate data for these materials

  11. Actinide and fission product partitioning and transmutation

    International Nuclear Information System (INIS)

    The fourth international information exchange meeting on actinide and fission product partitioning and transmutation, took place in Mito City in Japan, on 111-13 September 1996. The proceedings are presented in six sessions: the major programmes and international cooperation, the partitioning and transmutation programs, feasibility studies, particular separation processes, the accelerator driven transmutation, and the chemistry of the fuel cycle. (A.L.B.)

  12. Actinide and fission product partitioning and transmutation

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1997-07-01

    The fourth international information exchange meeting on actinide and fission product partitioning and transmutation, took place in Mito City in Japan, on 111-13 September 1996. The proceedings are presented in six sessions: the major programmes and international cooperation, the partitioning and transmutation programs, feasibility studies, particular separation processes, the accelerator driven transmutation, and the chemistry of the fuel cycle. (A.L.B.)

  13. Synthesis and Evaluation of new Polyfunctional Molecules for Group Actinide Extraction

    International Nuclear Information System (INIS)

    The aim of this project is to design new extracting molecules for spent nuclear fuel reprocessing. In order to minimize the long-term residual radiotoxicity of the waste, the GANEX process is an option based on homogeneous recycling of actinides. All actinides (U, Np, Pu, Am, Cm), present in a highly acidic aqueous solution, would be extracted together and separated from fission products (especially from lanthanides) using liquid-liquid extraction. In this context, twenty new bi-topic ligands constituted of a nitrogen poly-aromatic unit functionalized by amide groups were synthesized. Liquid-liquid extraction tests with these ligands dissolved alone in the organic phase show that N, N, N', N'-tetra-alkyl-6, 6''(2, 2':6', 2''-terpyridine)-diamides are able to selectively extract actinides at different oxidation states (Np(V et VI), U(VI), Pu(IV), Am(III), Cm(III)) from an aqueous solution 3M HNO3. Nevertheless, actinides(III) are poorly extracted. According to crystallographic structures of complexes with Nd(III) and U(VI) determined by X-rays diffraction, these ligands are penta-dentate. In solution (methanol), complexes stoichiometries (1:1) of Nd(III), U(VI) and Pu(IV) were determined by electro-spray ionization mass spectrometry. Stability constants, evaluated by UV-visible spectrophotometry in MeOH/H2O solutions, confirm the selectivity of ligands toward actinides(III) with respect to lanthanides(III). Associate to nuclear magnetic resonance experiments and DFT calculations (Density Functional Theory), a better knowledge of their coordination mode was achieved. (author)

  14. Successive change regularity of actinide properties with atomic number

    International Nuclear Information System (INIS)

    The development and achievements on chemistry of actinide elements are summarised. The relations of properties of actinides to their electronic configurations of valence electronic shells are discussed. Some anomalies of solid properties, the radius contraction, the stable state effect of f7n-orbits (n = 0, 1, 2) and the tetrad effect of oxidation states, etc., with atomic number (Z) are described. 31 figures appended show directly the successive change regularity of actinide properties with Z

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

    Energy Technology Data Exchange (ETDEWEB)

    Haire, R.G.

    1985-01-01

    The actinide elements form a unique series of metals. The variation in their physial properties combined with the varying availability of the different elements offers a challenge to the preparative scientist. This article provides a brief review of selected methods used for preparing ..mu..g to kg amounts of the actinide metals and the properties of these metals. In addition, some recent studies on selected actinide metals are discussed. 62 refs.

  16. Synthesis and evaluation structure/extracting and complexing properties of new bi-topic ligands for group actinides extraction

    International Nuclear Information System (INIS)

    The aim of this project is to design and study new extractants for spent nuclear fuel reprocessing. To decrease the long-term radiotoxicity of the waste, the GANEX process is an option to homogeneously recycle actinides. All actinides (U, Np, Pu, Am, Cm) would be extracted together from a highly acidic media and separated from fission products (especially from lanthanides). In this context, fourteen new bi-topic ligands constituted of a nitrogen poly-aromatic unit from the dipyridyl-phenanthroline and dipyridyl-1,3,5-triazine families and functionalized by amid groups were synthesized. Extraction studies performed with some of these ligands confirmed their interest to selectively separate actinides at different oxidation states from an aqueous solution 3M HNO3. To determine the influence of ligands structure on cation complexation, a study in a homogenous media (MeOH/H2O) has been carried out. Electro-spray ionization mass spectrometry have been used to characterize the complexes stoichiometries formed with several cations (Eu3+, Nd3+, Am3+, Pu4+ and NpO2+). Stability constants, evaluated by UV-Visible spectrophotometry, confirm the selectivity of these ligands toward actinides. Lanthanides and actinides complexes have also been characterized in the solid state by infra-red spectroscopy and X-Ray diffraction. Associated to nuclear magnetic resonance experiments and DFT calculations (Density Functional Theory), a better knowledge of their coordination mode was achieved. (author)

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

    Science.gov (United States)

    Souček, P.; Cassayre, L.; Eloirdi, R.; Malmbeck, R.; Meier, R.; Nourry, C.; Claux, B.; Glatz, J.-P.

    2014-04-01

    A chlorination route is being investigated for recovery of actinides from actinide-aluminium alloys, which originate from pyrochemical recovery of actinides from spent metallic nuclear fuel by electrochemical methods in molten LiCl-KCl. In the present work, the most important steps of this route were experimentally tested using U-Pu-Al alloy prepared by electrodeposition of U and Pu on solid aluminium plate electrodes. The investigated processes were vacuum distillation for removal of the salt adhered on the electrode, chlorination of the alloy by chlorine gas and sublimation of the AlCl3 formed. The processes parameters were set on the base of a previous thermochemical study and an experimental work using pure UAl3 alloy. The present experimental results indicated high efficiency of salt distillation and chlorination steps, while the sublimation step should be further optimised.

  18. Hydrothermal decomposition of actinide(IV oxalates: a new aqueous route towards reactive actinide oxide nanocrystals

    Directory of Open Access Journals (Sweden)

    Walter Olaf

    2016-09-01

    Full Text Available The hydrothermal decomposition of actinide(IV oxalates (An= Th, U, Pu at temperatures between 95 and 250 °C is shown to lead to the production of highly crystalline, reactive actinide oxide nanocrystals (NCs. This aqueous process proved to be quantitative, reproducible and fast (depending on temperature. The NCs obtained were characterised by X-ray diffraction and TEM showing their size to be smaller than 15 nm. Attempts to extend this general approach towards transition metal or lanthanide oxalates failed in the 95–250 °C temperature range. The hydrothermal decomposition of actinide oxalates is therefore a clean, flexible and powerful approach towards NCs of AnO2 with possible scale-up potential.

  19. Isotopic composition and neutronics of the Okelobondo natural reactor

    Science.gov (United States)

    Palenik, Christopher Samuel

    The Oklo-Okelobondo and Bangombe uranium deposits, in Gabon, Africa host Earth's only known natural nuclear fission reactors. These 2 billion year old reactors represent a unique opportunity to study used nuclear fuel over geologic periods of time. The reactors in these deposits have been studied as a means by which to constrain the source term of fission product concentrations produced during reactor operation. The source term depends on the neutronic parameters, which include reactor operation duration, neutron flux and the neutron energy spectrum. Reactor operation has been modeled using a point-source computer simulation (Oak Ridge Isotope Generation and Depletion, ORIGEN, code) for a light water reactor. Model results have been constrained using secondary ionization mass spectroscopy (SIMS) isotopic measurements of the fission products Nd and Te, as well as U in uraninite from samples collected in the Okelobondo reactor zone. Based upon the constraints on the operating conditions, the pre-reactor concentrations of Nd (150 ppm +/- 75 ppm) and Te (<1 ppm) in uraninite were estimated. Related to the burnup measured in Okelobondo samples (0.7 to 13.8 GWd/MTU), the final fission product inventories of Nd (90 to 1200 ppm) and Te (10 to 110 ppm) were calculated. By the same means, the ranges of all other fission products and actinides produced during reactor operation were calculated as a function of burnup. These results provide a source term against which the present elemental and decay abundances at the fission reactor can be compared. Furthermore, they provide new insights into the extent to which a "fossil" nuclear reactor can be characterized on the basis of its isotopic signatures. In addition, results from the study of two other natural systems related to the radionuclide and fission product transport are included. A detailed mineralogical characterization of the uranyl mineralogy at the Bangombe uranium deposit in Gabon, Africa was completed to improve

  20. The 10B(n,α)7Li reaction in PWR coolants: calculations of the effect on coolant pH and on decreases in 10B isotopic fractions

    International Nuclear Information System (INIS)

    Boron is used as a chemical shim in PWRs for reactivity control and is added in the form of boric acid to the primary coolant. The 10B(n,α)7Li reaction leads to a continuous increase in 7Li in the primary coolant and to a continuous decrease in 10B the isotope of boron responsible for control of reactivity. The rate of increase in coolant pH due to 7Li production is calculated for the Sizewell 'B' PWR to enable judgements to be made on the frequency of sampling and removal of lithium required to maintain the pH of the primary coolant within the desired limits. Calculations are contrasted for the cases of natural boron and 100% 10B chemical shims, for both a normal cycle and an extended 18 month cycle. Calculations of 10B depletion over 30 years of operation as a function of the quantity of boron discharged to waste are also presented. 10B isotopic fractions are calculated for the reactor coolant (RC), boric acid tanks (BATs) and refuelling water storage tank (RWST) assuming rapid mixing of BAT and RC boron for tritium control and other reasons. Such predictions enable assessments of the reactor physics implications of 10B consumption to be made. (author)

  1. Uncertainties in fission-product decay-heat calculations

    Energy Technology Data Exchange (ETDEWEB)

    Oyamatsu, K.; Ohta, H.; Miyazono, T.; Tasaka, K. [Nagoya Univ. (Japan)

    1997-03-01

    The present precision of the aggregate decay heat calculations is studied quantitatively for 50 fissioning systems. In this evaluation, nuclear data and their uncertainty data are taken from ENDF/B-VI nuclear data library and those which are not available in this library are supplemented by a theoretical consideration. An approximate method is proposed to simplify the evaluation of the uncertainties in the aggregate decay heat calculations so that we can point out easily nuclei which cause large uncertainties in the calculated decay heat values. In this paper, we attempt to clarify the justification of the approximation which was not very clear at the early stage of the study. We find that the aggregate decay heat uncertainties for minor actinides such as Am and Cm isotopes are 3-5 times as large as those for {sup 235}U and {sup 239}Pu. The recommended values by Atomic Energy Society of Japan (AESJ) were given for 3 major fissioning systems, {sup 235}U(t), {sup 239}Pu(t) and {sup 238}U(f). The present results are consistent with the AESJ values for these systems although the two evaluations used different nuclear data libraries and approximations. Therefore, the present results can also be considered to supplement the uncertainty values for the remaining 17 fissioning systems in JNDC2, which were not treated in the AESJ evaluation. Furthermore, we attempt to list nuclear data which cause large uncertainties in decay heat calculations for the future revision of decay and yield data libraries. (author)

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

    Science.gov (United States)

    Schulz, Wallace W.

    1976-01-01

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

  3. Actinides AMS at CIRCE and 236U and Pu measurements of structural and environmental samples from in and around a mothballed nuclear power plant

    International Nuclear Information System (INIS)

    Accelerator mass spectrometry (AMS) is presently the most sensitive technique for the measurement of long-lived actinides, e.g. 236U and 239Pu. A new actinide line is in operation at the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy. Using the actinide line a uranium mass sensitivity of around 4 μg has been reached measuring with a 16-strip silicon detector, and a 239Pu background level of below 0.1 fg has been obtained. In this work we also discuss preliminary results for environmental and structural samples from in and around the Garigliano nuclear power plant (GNPP), presently in the decommissioning phase. Measurements on environmental samples from the vicinity of the plant allow the assessment of contamination, if any, over the years. Measurements of structural samples from the plant are relevant to the optimization of the decommissioning program for the GNPP.

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

    Energy Technology Data Exchange (ETDEWEB)

    Radulescu, Georgeta [ORNL

    2010-06-01

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

  5. Advanced Aqueous Separation Systems for Actinide Partitioning

    Energy Technology Data Exchange (ETDEWEB)

    Nash, Ken [Washington State Univ., Pullman, WA (United States); Martin, Leigh [Idaho National Lab. (INL), Idaho Falls, ID (United States); Lumetta, Gregg [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2015-04-02

    One of the most challenging aspects of advanced processing of used nuclear fuel is the separation of transplutonium actinides from fission product lanthanides. This separation is essential if actinide transmutation options are to be pursued in advanced fuel cycles, as lanthanides compete with actinides for neutrons in both thermal and fast reactors, thus limiting efficiency. The separation is difficult because the chemistry of Am3+ and Cm3+ is nearly identical to that of the trivalent lanthanides (Ln3+). The prior literature teaches that two approaches offer the greatest probability of devising a successful group separation process based on aqueous processes: 1) the application of complexing agents containing ligand donor atoms that are softer than oxygen (N, S, Cl-) or 2) changing the oxidation state of Am to the IV, V, or VI state to increase the essential differences between Am and lanthanide chemistry (an approach utilized in the PUREX process to selectively remove Pu4+ and UO22+ from fission products). The latter approach offers the additional benefit of enabling a separation of Am from Cm, as Cm(III) is resistant to oxidation and so can easily be made to follow the lanthanides. The fundamental limitations of these approaches are that 1) the soft(er) donor atoms that interact more strongly with actinide cations than lanthanides form substantially weaker bonds than oxygen atoms, thus necessitating modification of extraction conditions for adequate phase transfer efficiency, 2) soft donor reagents have been seen to suffer slow phase transfer kinetics and hydro-/radiolytic stability limitations and 3) the upper oxidation states of Am are all moderately strong oxidants, hence of only transient stability in media representative of conventional aqueous separations systems. There are examples in the literature of both approaches having been described. However, it is not clear at present that any extant process is sufficiently robust for application at the scale

  6. Preparations and mechanism of hydrolysis of ([8]annulene)actinide compounds

    International Nuclear Information System (INIS)

    The mechanism of hydrolysis for bis[8]annulene actinide and lanthanide complexes has been studied in detail. The uranium complex, uranocene, decomposes with good pseudo-first order kinetics (in uranocene) in 1 M degassed solutions of H2O in THF. Decomposition of a series of aryl-substituted uranocenes demonstrates that the hydrolysis rate is dependent on the electronic nature of the substituent (Hammett rho value = 2.1, r2 = 0.999), with electron-withdrawing groups increasing the rate. When D2O is substituted for H2O, kinetic isotope effects of 8 to 14 are found for a variety of substituted uranocenes. These results suggest a pre-equilibrium involving approach of a water molecule to the central metal, followed by rate determining proton transfer to the eight membered ring and rapid decomposition to products. Each of the four protonations of the complex has a significant isotope effect. The product ratio of cyclooctatriene isomers formed in the hydrolysis varies, depending on the central metal of the complex. However, the general mechanism of hydrolysis, established for uranocene, can be extended to the hydrolysis and alcoholysis of all the [8]annulene complexes of the lanthanides and actinides

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

    Energy Technology Data Exchange (ETDEWEB)

    Moore, R.M. Jr.

    1985-07-01

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

  8. Programme and Abstracts. 38. Journees des Actinides together with the 7. School on the Physics and Chemistry of the Actinides

    International Nuclear Information System (INIS)

    Journees des Actinides (JdA) is a traditional informal actinide forum, including physics, chemistry, and materials research. It regularly brings together experts from fields involved, taking place in a very informal way, emphasizing exchanges and discussions on current issues in actinide science. At the 38th JdA (10-15 April 2008; Wroclaw, Poland) scientific communications on the following topics on physics and chemistry of the actinides were presented: (a) inorganic and organometallic chemistry; (b) strongly correlated behaviour, superconductivity, quantum criticality; (c) materials science; (d) theory, electronic structure; (e) nuclear fuel cycle, environment

  9. Isotope and nuclear chemistry division. Annual report, FY 1987. Progress report, October 1986-September 1987

    International Nuclear Information System (INIS)

    This report describes progress in the major research and development programs carried out in FY 1987 by the Isotope and Nuclear Chemistry Division. The report includes articles on radiochemical weapons diagnostics and research and development; other unclassified weapons research; stable and radioactive isotope production and separation; chemical biology and nuclear medicine; element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced concepts and technology; and atmospheric chemistry

  10. Actinide inventory in Herndon’s georeactor operating throughout geologic time

    International Nuclear Information System (INIS)

    Highlights: • Actinide inventory of Herndon’s georeactor was analyzed by using a modified TRITON sequence in SCALE6. • The georeactor can function as a converter reactor, with a conversion efficiency of approximately 0.9 over billions of years. • Dominant mechanisms that dictate the variations of nuclide concentrations over geologic time were identified. - Abstract: Herndon proposed a nuclear fission reactor at the center of the Earth to explain changes in the geomagnetic field and the 3He/4He ratios observed from deep mantle sources. This study investigated the neutronic properties of the planetary-scale reactor by performing rigorous depletion simulations over geologic time by using a modified TRITON sequence in SCALE6. We also conducted analytical calculations of the rates of change of various actinides in the reactor core to identify the primary mechanisms involved in the nuclear system as a function of the operating time. The sound agreement between analytical and TRITON calculations on the predicted variations of the amounts of important actinides revealed that (1) the hypothetical nuclear georeactor is a fast-spectrum converter reactor burning only 235U; (2) the efficiency of fuel conversion approaches 0.9, and can be sustained for billions of years based on the cycle of 238U/239Pu/235U, rather than of 238U/239Pu or 232Th/233U; and (3) under appropriate conditions, the georeactor can operate at a constant power of 3 TW for up to 6.5 billion years

  11. Trace analysis of actinides in the environment using resonance ionization mass spectrometry; Spurenanalyse von Aktiniden in der Umwelt mittels Resonanzionisations-Massenspektrometrie

    Energy Technology Data Exchange (ETDEWEB)

    Raeder, Sebastian

    2011-04-12

    In this work the resonant ionization of neutral atoms using laser radiation was applied and optimized for ultra-trace analysis of the actinides thorium, uranium, neptunium and plutonium. The sensitive detection of these actinides is a challange for the monitoring and quantification of radioactive releases from nuclear facilities. Using resonance ionization spectroscopy combined with a newly developed quadrupole-mass-spectrometer, numerous energy levels in the atomic structure of these actinides could be identified. With this knowledge efficient excitation schemes for the mentioned actinides could be identified and characterised. The applied in-source-ionization ensures for a high detection efficiency due to the good overlap of laser radiation with the atomic beam and allows therefore for a low sample consumption which is required for the analysis of radio nuclides. The selective excitation processes in the resonant ionization method supresses unwanted contaminations and was optimized for analytical detection of ultra-trace amounts in environmental samples as well as for determination of isotopic compositions. The efficient in-source-ionization combined with high power pulsed laser radiation allows for detections efficiency up to 1%. For plutonium detection limits in the range of 10{sup 4}-10{sup 5} atoms could be demonstrated for synthetic samples as well as for first environmental samples. The usage of narrow bandwidth continuous wave lasers in combination with a transversal overlap of the laser radiation and the free propagating atomic beam enable for resolving individual isotopic shifts of the resonant transitions. This results in a high selectivity against dominant neighboring isotopes but with a significant loss in detection efficiency. For the ultra-trace isotope {sup 236}U a detection limit down to 10{sup -9} for the isotope ratio N ({sup 236}U)/N ({sup 238}U) could be determined.

  12. Structure of early actinides(V) in acidic solutions

    Energy Technology Data Exchange (ETDEWEB)

    Di Giandomenico, M.V.; Le Naour, C.; Simoni, E. [CNRS/Univ. Paris-Sud, Inst. de Physique Nucleaire, Orsay (France); Guillaumont, D.; Moisy, P.; Den Auwer, C. [CEA Marcoule, DHN/DRCP/SCPS, Bagnols sur Ceze (France); Hennig, C. [Forschungszentrum Rossendorf, Dresden (Germany); Conradson, S.D. [Los Alamos National Lab., Los Alamos, NM (United States)

    2009-07-01

    Protactinium occupies a key position in the actinide series between thorium and uranium. In aqueous acidic solution, it is stable at oxidation state (V), occurring either as an oxocation or as a naked ion, depending on the media. Very few structural information on the hydration sphere of Pa(V) in acidic medium is available, in particular in hydrofluoric acid. Combined EXAFS and theoretical calculations have been used in this work to characterize the protactinium coordination sphere at various HF concentrations. The correlation of the XAFS data with quantum chemical calculations provides complementary structural and electronic models from ab initio techniques. At HF concentrations from 0.5 to 0.05 M, both theoretical calculations and EXAFS data suggest that the protactinium coordination sphere is mainly composed of fluoride ions. At the lowest HF concentration, the occurrence of a monooxo bond is observed with EXAFS, in agreement with the literature. A comparison of these data with related neptunium(V) and plutonium(V) diooxocations in perchloric acid is also presented. (orig.)

  13. Structure of early actinides(V) in acidic solutions

    International Nuclear Information System (INIS)

    Protactinium occupies a key position in the actinide series between thorium and uranium. In aqueous acidic solution, it is stable at oxidation state (V), occurring either as an oxocation or as a naked ion, depending on the media. Very few structural information on the hydration sphere of Pa(V) in acidic medium is available, in particular in hydrofluoric acid. Combined EXAFS and theoretical calculations have been used in this work to characterize the protactinium coordination sphere at various HF concentrations. The correlation of the XAFS data with quantum chemical calculations provides complementary structural and electronic models from ab initio techniques. At HF concentrations from 0.5 to 0.05 M, both theoretical calculations and EXAFS data suggest that the protactinium coordination sphere is mainly composed of fluoride ions. At the lowest HF concentration, the occurrence of a monooxo bond is observed with EXAFS, in agreement with the literature. A comparison of these data with related neptunium(V) and plutonium(V) diooxocations in perchloric acid is also presented. (orig.)

  14. Formal oxidation potentials of actinide couples in K10P2W17O61 solutions

    International Nuclear Information System (INIS)

    The formal oxidation potentials of the M(VI)/M(V), M(V)/M(IV), and M(IV)/M(III) couples for actinides from U to No and of the M(IV)/M(III) couples for some actinides in 1 M H+ or 1 M Na+ (pH ∼5-5.5) solutions containing K10P2W17O61 were calculated from the data on stability of complexes of f element ions with the unsaturated heteropolytungstate anion P2W17O 6110-. In some cases, the previously accepted values were subjected to major revision, especially the potentials of the An(V)/An(IV) couples. Problems arising in measuring the potentials of the couples involving Np(III) and Pu(III) which react with the heteropolyanion to form a heteropoly blue are discussed. The potentials of some M(III)/M(II) couples are estimated

  15. Prospects of subcritical molten salt reactor for minor actinides incineration in closed fuel cycle

    Energy Technology Data Exchange (ETDEWEB)

    Alekseev, Pavel N.; Balanin, Andrey L.; Dudnikov, Anatoly A.; Fomichenko, Petr A.; Nevinitsa, Vladimir A.; Frolov, Aleksey A.; Lubina, Anna S.; Sedov, Aleksey A.; Subbotin, Aleksey S.; Blandinsky, Viktor Yu. [Nuclear Research Centre ' ' Kurchatov Institute' ' , Moscow (Russian Federation)

    2015-09-15

    A subcritical molten salt reactor is proposed for minor actinides (separated from spent fuel VVER-1000 light water reactor) incineration and for {sup 233}U conversion from {sup 232}Th. Here the subcritical molten salt reactor with fuel composition of heavy nuclide fluorides in molten LiF - NaF - KF salt and with external neutron source, based on 1 GeV proton accelerator and molten salt cooled tungsten target is considered. The paper presents the results of parametrical analysis of equilibrium nuclide composition of molten salt reactor with minor actinides feed in dependence of core dimensions, average neutron flux and external neutron source intensity. Reactor design is defined; requirements to external neutron source are posed; heavy nuclides equilibrium and fuel cycle main parameters are calculated.

  16. Odd–even effect in fragment angular momentum in low-energy fission of actinides

    Indian Academy of Sciences (India)

    B S Tomar; R Tripathi; A Goswami

    2007-01-01

    Quantitative explanation for the odd–even effect on fragment angular momenta in the low-energy fission of actinides have been provided by taking into account the single particle spin of the odd proton at the fragment's scission point deformation in the case of odd- fragments along with the contribution from the population of angular momentum bearing collective vibrations of the fissioning nucleus at scission point. The calculated fragment angular momenta have been found to be in very good agreement with the experimental data for fragments in the mass number region of 130–140. The odd–even effect observed in the fragment angular momenta in the low-energy fission of actinides has been explained quantitatively for the first time.

  17. Actinide management with commercial fast reactors

    International Nuclear Information System (INIS)

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

  18. Actinide management with commercial fast reactors

    Science.gov (United States)

    Ohki, Shigeo

    2015-12-01

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

  19. Supercritical fluid extraction studies on actinides

    International Nuclear Information System (INIS)

    Uranyl nitrate and plutonium in its Pu (III) as well Pu (IV) form loaded onto a tissue paper was extracted completed from paper, glass, stainless steel as well as teflon matrices using modified SC-CO2. A further investigation on recovery of actinides independent of their drying period is expected to culminate into developing an universal procedure to handle Pu bearing waste for its recovery irrespective of its drying history and oxidation states. Such endeavors ultimately lead to the potential utility of the SFE technology for efficient nuclear waste management

  20. Recent progress in actinide borate chemistry

    OpenAIRE

    Wang, S.; Alekseev, E .V.; Depmeier, W.; Albrecht-Schmitt, T.E.

    2011-01-01

    The use of molten boric acid as a reactive flux for synthesizing actinide borates has been developed in the past two years providing access to a remarkable array of exotic materials with both unusual structures and unprecedented properties. [ThB(5)O(6)(OH)(6)][BO(OH)(2)]·2.5H(2)O possesses a cationic supertetrahedral structure and displays remarkable anion exchange properties with high selectivity for TcO(4)(-). Uranyl borates form noncentrosymmetric structures with extraordinarily rich topol...

  1. Actinide management with commercial fast reactors

    Energy Technology Data Exchange (ETDEWEB)

    Ohki, Shigeo [Japan Atomic Energy Agency, 4002, Narita-cho, O-arai-machi, Higashi-Ibaraki-gun, Ibaraki 311-1393 (Japan)

    2015-12-31

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

  2. Fission cross section measurements for minor actinides

    Energy Technology Data Exchange (ETDEWEB)

    Fursov, B. [IPPE, Obninsk (Russian Federation)

    1997-03-01

    The main task of this work is the measurement of fast neutron induced fission cross section for minor actinides of {sup 238}Pu, {sup 242m}Am, {sup 243,244,245,246,247,248}Cm. The task of the work is to increase the accuracy of data in MeV energy region. Basic experimental method, fissile samples, fission detectors and electronics, track detectors, alpha counting, neutron generation, fission rate measurement, corrections to the data and error analysis are presented in this paper. (author)

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2015-09-15

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

  4. MOLECULAR SPECTROSCPY AND REACTIONS OF ACTINIDES IN THE GAS PHASE AND CRYOGENIC MATRICES

    Energy Technology Data Exchange (ETDEWEB)

    Heaven, Michael C.; Gibson, John K.; Marcalo, Joaquim

    2009-02-01

    In this chapter we review the spectroscopic data for actinide molecules and the reaction dynamics for atomic and molecular actinides that have been examined in the gas phase or in inert cryogenic matrices. The motivation for this type of investigation is that physical properties and reactions can be studied in the absence of external perturbations (gas phase) or under minimally perturbing conditions (cryogenic matrices). This information can be compared directly with the results from high-level theoretical models. The interplay between experiment and theory is critically important for advancing our understanding of actinide chemistry. For example, elucidation of the role of the 5f electrons in bonding and reactivity can only be achieved through the application of experimentally verified theoretical models. Theoretical calculations for the actinides are challenging due the large numbers of electrons that must be treated explicitly and the presence of strong relativistic effects. This topic has been reviewed in depth in Chapter 17 of this series. One of the goals of the experimental work described in this chapter has been to provide benchmark data that can be used to evaluate both empirical and ab initio theoretical models. While gas-phase data are the most suitable for comparison with theoretical calculations, there are technical difficulties entailed in generating workable densities of gas-phase actinide molecules that have limited the range of species that have been characterized. Many of the compounds of interest are refractory, and problems associated with the use of high temperature vapors have complicated measurements of spectra, ionization energies, and reactions. One approach that has proved to be especially valuable in overcoming this difficulty has been the use of pulsed laser ablation to generate plumes of vapor from refractory actinide-containing materials. The vapor is entrained in an inert gas, which can be used to cool the actinide species to room

  5. Contribution to the physical modeling of the actinide characterization by electron probe microanalysis

    International Nuclear Information System (INIS)

    Electron probe microanalysis (EPMA) is used to quantify with a high accuracy the amount of different elements present on a sample of unknown composition. EPMA is largely used to quantify the amount of actinides present in fresh and irradiated fuels, to manage waste disposal and to date rocks. However, quantitative EPMA is not always possible to achieve for these materials due to the lack of suitable reference standards for the radionuclides. To overcome this difficulty, standard-less methods of analysis are employed with mean of virtual calculated standards. These calculated standards are generally obtained from empirical formulae based on experimental extrapolations or from theoretical calculations that require physical parameters which are poorly known as it is the case for the X-ray production cross section. The accurate knowledge of these cross sections is required in many applications such as in particle transport code and in Monte Carlo simulations. The computer simulations are widely used in the medical field and particularly in medical imaging and in electron beam therapy. In the field of astronomy, these data are used to perform simulations that predict the compositions of stars and galactic clouds, and the formation of planetary systems. In the present work, L- and M-shell absolute x-ray production cross sections were determined experimentally for elements lead, thorium and uranium by electron impact using ultrathin self-supporting targets with thickness varying from 0.2 to 8 nm. The measured cross sections have been compared, with the distorted-wave Born approximation (DWBA) calculated by Bote et al. and with the predictions of analytical formulae widely used in practical applications. For the conversion of inner-shell ionization cross sections into x-ray production cross sections, atomic relaxation parameters were extracted from the literature. The predictions of the DWBA calculations are in excellent agreement with our measured x-ray production cross

  6. A multi-layer, closed-loop system for continuous measurement of CO2 concentrations and its isotopic signature in forest soils as a basis for CO2 efflux calculation and for revealing its controls

    Science.gov (United States)

    Jochheim, Hubert; Wirth, Stephan

    2015-04-01

    We present a setup of measurement devices that allows the application of the soil CO2 gradient approach for CO2 efflux calculation in combination with the analysis of isotopic signature (δ13C). Vertical profiles of CO2 concentrations in air-filled pores of soil were measured using miniature NDIR sensors within a 16-channel closed-loop system where equilibrium with soil air can be achieved using hydrophobic, gas-permeable porous polypropylene tubes circulating gas using peristaltic pumps. A 16-position multiplexer allows the connection to an isotopic CO2 analyser. This setup was applied at two ICP Forest intensive monitoring sites, a beech and a pine forest on sandy soils located in Brandenburg, Germany. CO2 concentrations in air-filled pores of soils were measured on top of soil surface, below the humus layer, and in 10cm, 20cm, 30cm and 100 cm depths every 30 min. At both sites, soil moisture and temperature were measured continuously in the respective soil depths in identical time intervals. Isotopic signatures of soil CO2 was detected by measurement campaigns. After two years of measurements, our results provided evidence for distinct seasonal dynamics and vertical gradients of soil CO2 concentration and δ13C values. Varying impacts of soil temperature and moisture on CO2 concentration were revealed, highlighting its impact on soil physical and soil biological controls. Higher levels of CO2 concentration and a more distinct seasonal dynamics were detected at the beech site compared to the pine site. The collected data provide a suitable database for calculation of CO2 efflux and modelling of soil respiration.

  7. QCT calculation of reactions of F+LiH→LiF+H and F+LiD→LiF+D: product polarization and isotope effects

    International Nuclear Information System (INIS)

    Using the quasi-classical trajectory (QCT) method, the product polarization at the collision energy of 46 kcal/mol is investigated for the reactions of F+LiH (v = 0, j = 0)→LiF+H and F+LiD (v = 0, j = 0)→LiF+D on the 2A' ground state potential energy surface (PES)[J. Chem. Phys. 106(1997)1013]. The distribution of P(θr), which represents the K and J' correlation, the dihedral angle distribution of K-K'-J' P(φr), the angular distribution P(θr, φr) and the four PDDCSs[(2π/σ)(dσ00/dωt), (2π/σ)(dσ20/dωt), (2π/σ)(dσ22+/dωt), (2π/σ)(dσ21-/dωt)] are presented and discussed. In addition, isotope effects are investigated. The results indicate that at the collision energy of 46 kcal/mol, with isotopic mass substitution, the orientation degree of LiF perpendicular to the scattering degree becomes stronger while the polarization degree of LiF perpendicular to K keeps almost changeless. In addition, the angular distribution of LiF strongly prefers forward scattering. (authors)

  8. Actinide Solubility and Speciation in the WIPP

    Energy Technology Data Exchange (ETDEWEB)

    Reed, Donald T. [Los Alamos National Laboratory

    2015-11-02

    The presentation begins with the role and need for nuclear repositories (overall concept, international updates (Sweden, Finland, France, China), US approach and current status), then moves on to the WIPP TRU repository concept (design, current status--safety incidents of February 5 and 14, 2014, path forward), and finally considers the WIPP safety case: dissolved actinide concentrations (overall approach, oxidation state distribution and redox control, solubility of actinides, colloidal contribution and microbial effects). The following conclusions are set forth: (1) International programs are moving forward, but at a very slow and somewhat sporadic pace. (2) In the United States, the Salt repository concept, from the perspective of the long-term safety case, remains a viable option for nuclear waste management despite the current operational issues/concerns. (3) Current model/PA prediction (WIPP example) are built on redundant conservatisms. These conservatisms are being addressed in the ongoing and future research to fill existing data gaps--redox control of plutonium by Fe(0, II), thorium (analog) solubility studies in simulated brine, contribution of intrinsic and biocolloids to the mobile concentration, and clarification of microbial ecology and effects.

  9. Strategies for Application of Isotopic Uncertainties in Burnup Credit

    Energy Technology Data Exchange (ETDEWEB)

    Gauld, I.C.

    2002-12-23

    Uncertainties in the predicted isotopic concentrations in spent nuclear fuel represent one of the largest sources of overall uncertainty in criticality calculations that use burnup credit. The methods used to propagate the uncertainties in the calculated nuclide concentrations to the uncertainty in the predicted neutron multiplication factor (k{sub eff}) of the system can have a significant effect on the uncertainty in the safety margin in criticality calculations and ultimately affect the potential capacity of spent fuel transport and storage casks employing burnup credit. Methods that can provide a more accurate and realistic estimate of the uncertainty may enable increased spent fuel cask capacity and fewer casks needing to be transported, thereby reducing regulatory burden on licensee while maintaining safety for transporting spent fuel. This report surveys several different best-estimate strategies for considering the effects of nuclide uncertainties in burnup-credit analyses. The potential benefits of these strategies are illustrated for a prototypical burnup-credit cask design. The subcritical margin estimated using best-estimate methods is discussed in comparison to the margin estimated using conventional bounding methods of uncertainty propagation. To quantify the comparison, each of the strategies for estimating uncertainty has been performed using a common database of spent fuel isotopic assay measurements for pressurized-light-water reactor fuels and predicted nuclide concentrations obtained using the current version of the SCALE code system. The experimental database applied in this study has been significantly expanded to include new high-enrichment and high-burnup spent fuel assay data recently published for a wide range of important burnup-credit actinides and fission products. Expanded rare earth fission-product measurements performed at the Khlopin Radium Institute in Russia that contain the only known publicly-available measurement for {sup 103

  10. Study of the mechanism of the dissolution of actinide's dioxides (UO2, NpO2 PuO2, AmO2) by chemical or electrochemical redox reactions in aqueous acid medium

    International Nuclear Information System (INIS)

    The study of the mechanism of the dissolution of MO2 type actinide's oxides (with M = U,Np,Pu,Am) has been realized. Three basic tools have been employed: 1/ thermodynamic calculations, 2/ electrochemistry of the oxides in carbon paste electrodes (CPE), 3/ isotopic labelling (18O) followed by the measurement of the MO22+ entities by RAMAN spectroscopy. The thermodynamic study demonstrates that: 1/ the dissolution of MO2 oxides leading to MIV ions in acidic non complexing medium is impossible: these oxides are thus strictly insoluble in these conditions, 2/ the dissolution of MO2 oxides leading to M III, M V and M VI aquo ions is possible and the range of potential corresponding to these transformations have been calculated. The results of the thermodynamic study are supported by those obtained by electrochemistry. Quantitative transformations: MO2(solid) → MO22+(solution) or MO2(solid) → M3(solution) are observable. The knowledge of the reactional chemical path has been improved in the case of the oxidizing dissolution (MO2(solid) → MO22+(solution), in the course of the experiment where 18O labelling of actinyl's oxygen (MO22+) was realized: the species M16O22+, M16,18O22+ and M18,18O22+ were detected after reaction by RAMAN spectroscopy. This study demonstrated that the first step of an oxidizing dissolution of an actinide's oxide of the MO2 type consist in the conversion of M IV O2 into an M V (MO2+) species on the surface of the oxide

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

    International Nuclear Information System (INIS)

    Complexation of trivalent actinides with DTPA (diethylenetriamine pentaacetic acid) was studied as a function of pcH and temperature in (Na,H)Cl medium of 0.1 M ionic strength. Formation constants of both complexes AnHDTPA- and AnDTPA2- (where An stands for Am, Cm, and Cf) were determined by TRLFS, CE-ICP-MS, spectrophotometry, and solvent extraction. The values of formation constants obtained from the different techniques are coherent and consistent with reinterpreted literature data, showing a higher stability of Cf complexes than Am and Cm complexes. The effect of temperature indicates that formation constants of protonated and non protonated complexes are exothermic with a high positive entropic contribution. DFT calculations were also performed on the An/DTPA system. Geometry optimizations were conducted on AnDTPA2- and AnHDTPA- considering all possible protonation sites. For both complexes, one and two water molecules in the first coordination sphere of curium were also considered. DFT calculations indicate that the lowest energy structures correspond to protonation on oxygen that is not involved in An-DTPA bonds and that the structures with two water molecules are not stable. (authors)

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

    Energy Technology Data Exchange (ETDEWEB)

    Heiken, J.H.; Lindberg, H.A. (eds.)

    1984-05-01

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

  13. Isotope and Nuclear Chemistry Division annual report, FY 1984

    International Nuclear Information System (INIS)

    This report describes progress in the major research and development programs carried out in FY 1984 by the Isotope and Nuclear Chemistry Division. It covers radiochemical diagnostics of weapons tests; weapons radiochemical diagnostics research and development; other unclassified weapons research; stable and radioactive isotope production, separation, and applications (including biomedical applications); element and isotope transport and fixation; actinide and transition metal chemistry; structural chemistry, spectroscopy, and applications; nuclear structure and reactions; irradiation facilities; advanced analytical techniques: development and applications; atmospheric chemistry and transport; and earth and planetary processes. 287 refs

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

    International Nuclear Information System (INIS)

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

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

    Energy Technology Data Exchange (ETDEWEB)

    Lumetta, Gregg J.; Addleman, Raymond S.; Hay, Benjamin P.; Hubler, Timothy L.; Levitskaia, Tatiana G.; Sinkov, Sergey I.; Snow, Lanee A.; Warner, Marvin G.; Latesky, Stanley L.

    2006-11-17

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

  16. Thermodynamics and Structure of Actinide(IV) Complexes with Nitrilotriacetic Acid

    International Nuclear Information System (INIS)

    Nitrilotriacetic acid, commonly known as NITA (N(CH2CO2H)3), can be considered a representative of the polyamino-carboxylic family. The results presented in this paper describe the thermodynamical complexation and structural investigation of An(IV) complexes with NTA in aqueous solution. In the first part, the stability constants of the An(IV) complexes (An = Pu, Np, U, and Th) have been determined by spectrophotometry. In the second part, the coordination spheres of the actinide cation in these complexes have been described using extended X-ray absorption fine structure spectroscopy and compared to the solid-state structure of (Hpy)2[U(NTA)2].H2O. These data are further compared to quantum chemical calculations, and their evolution across the actinide series is discussed. In particular, an interpretation of the role of the nitrogen atom in the coordination mode is proposed. These results are considered to be model behavior of polyamino-carboxylic ligands such as diethylenetriamine pentaacetic acid, which is nowadays the best candidate for a chelating agent in the framework of actinide decorporation for the human body. (authors)

  17. Use of animal studies for assessing intakes of inhaled actinide-bearing dusts

    International Nuclear Information System (INIS)

    This paper reviews the methodology used in the execution and interpretation of animal studies (mostly conducted at NRPB) designed to provide guidance on limits of intake and the effectiveness of chest monitoring for persons exposed to various uranium, plutonium, americium, and thorium bearing dusts. The lung retention and transportability characteristics of the actinides in humans have been predicted by combining the absorption rates into blood calculated from the animal studies with particle transport rates from the alveolar region of the human lung. This approach is compatible with the application of the new ICRP respiratory tract model. The results of the animal experiments demonstrate the diversity of the absorption rates for the different chemical forms of the actinides and their disparity from the default values proposed by ICRP for Type F, M, and S compounds in the absence of specific data. The predicted lung retention kinetics of the actinides in humans provide the basis for assessing the validity of chest monitoring; for this purpose the most recent ICRP values for doses per unit intake and deposition in the alveolar region of the lungs have been taken into account. The results show that for some dusts, the data can be interpreted with confidence, while for others the method is impracticable or has considerable uncertainty. Overall, the results support the ICRP recommendation that material specific information is to be preferred for setting limits on intake and interpreting monitoring data. The paper concludes with suggestions for further work. (author). 44 refs., 4 figs., 6 tabs

  18. Isotopic dependence of isomeric states in heavy nuclei

    International Nuclear Information System (INIS)

    High-spin K-isomer states, which are usually assumed as two quasiparticle high-spin configurations states, were observed in heavy nuclei 250,256Fm, 252,254No, 266Hs and 270,271Ds. In order to calculate the energies of 2qp isomer states in even-even nuclei, the two-center shell model is used for finding the single-particle levels at the ground state of nucleus. The shape parameterization used in this model effectively includes many even multipolarities. The dependence of the parameters of Is and I2 terms on A and N - Z were modified for the correct description of the ground state spins of odd actinides. The microscopical corrections and quadrupole parameters of deformation calculated with the two-center shell model are close to those obtained with the microscopic-macroscopic approaches of P. Moller et al. and A.Sobiczewski et al. The calculated values of Qa are in reasonable agreement with measured values. The calculated two-quasiparticle energies are in good agreement with the available experimental data. In the even isotope chains of Fm and No the calculated E2qp for high spin K-isomer states are minimal for 250Fm and 252No. In 242,244Fm the K-isomer states with K ≥ 6 are above 1.38 MeV that is larger than the energies of the K-isomer states in 252,254No. In order to observe these states in the neutron-deficient Fm isotopes, one should produce these isotopes with the cross sections similar to those for the nuclei 252,254No. Calculating the potential energy surface near the ground state, one can not exclude the existence of shallow potential minima which can be related to the shape isomers. The possibility of existence of these minima is discussed within the microscopic-macroscopic model. We found the indications for the low-lying shape isomers in 264,266Sg and 268,270Hs The alpha-decay between the isomer states and between the ground states can have similar properties that shields the observation of isomeric states. The population of the isomer states in the

  19. Evaluation of average neutron resonance parameters of actinides with the account of experimental resolution and discrimination threshold. Final report for the period 15 December 1996 - 14 December 1997

    International Nuclear Information System (INIS)

    New evaluation of average resonance parameters for 32 isotopes of the actinide region (229Th-252Cf) was completed. Obtained values of average level spacings produce a smooth systematics of the main level density parameter. The results were included into the Starter File of the Reference Input Parameter Library (segment Average Neutron Resonances) and officially released on 15 May 1998. The numerical results are available from the Internet (http://iaeand.iaea.or.at/ripl) and on CD-ROM. (author)

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

    Science.gov (United States)

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

    1979-01-01

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

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

    Science.gov (United States)

    Veliscek-Carolan, Jessica

    2016-11-15

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

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

    Science.gov (United States)

    Veliscek-Carolan, Jessica

    2016-11-15

    This review summarises the methods currently available to extract radioactive actinide elements from solutions of spent nuclear fuel. This separation of actinides reduces the hazards associated with spent nuclear fuel, such as its radiotoxicity, volume and the amount of time required for its' radioactivity to return to naturally occurring levels. Separation of actinides from environmental water systems is also briefly discussed. The actinide elements typically found in spent nuclear fuel include uranium, plutonium and the minor actinides (americium, neptunium and curium). Separation methods for uranium and plutonium are reasonably well established. On the other hand separation of the minor actinides from lanthanide fission products also present in spent nuclear fuel is an ongoing challenge and an area of active research. Several separation methods for selective removal of these actinides from spent nuclear fuel will be described. These separation methods include solvent extraction, which is the most commonly used method for radiochemical separations, as well as the less developed but promising use of adsorption and ion-exchange materials. PMID:27427893

  3. Fission decay properties of ultra neutron-rich uranium isotopes

    Indian Academy of Sciences (India)

    L Satpathy; S K Patra; R K Choudhury

    2008-01-01

    The fission decay of highly neutron-rich uranium isotopes is investigated which shows interesting new features in the barrier properties and neutron emission characteristics in the fission process. 233U and 235U are the nuclei in the actinide region in the beta stability valley which are thermally fissile and have been mainly used in reactors for power generation. The possibility of occurrence of thermally fissile members in the chain of neutron-rich uranium isotopes is examined here. The neutron number = 162 or 164 has been predicted to be magic in numerous theoretical studies carried out over the years. The series of uranium isotopes around it with = 154-172 are identified to be thermally fissile on the basis of the fission barrier and neutron separation energy systematics; a manifestation of the close shell nature of = 162 (or 164). We consider here the thermal neutron fission of a typical representative 249U nucleus in the highly neutron-rich region. Semiempirical study of fission barrier height and width shows that 250U nucleus is stable against spontaneous fission due to increase in barrier width arising out of excess neutrons. On the basis of the calculation of the probability of fragment mass yields and the microscopic study in relativistic mean field theory, this nucleus is shown to undergo exotic decay mode of thermal neutron fission (multi-fragmentation fission) whereby a number of prompt scission neutrons are expected to be simultaneously released along with the two heavy fission fragments. Such properties will have important implications in stellar evolution involving -process nucleosynthesis.

  4. Actinide separation chemistry in nuclear waste streams and materials

    International Nuclear Information System (INIS)

    The separation of actinide elements from various waste materials, produced either in nuclear fuel cycles or in past nuclear weapons production, represents a significant issue facing developed countries. Improvements in the efficiencies of the separation processes can be expected to occur as a result of better knowledge of the elements in these complex matrices. The Nuclear Science Committee of the OECD/NEA has established a task force of experts in actinide separation chemistry to review current and developing separation techniques and chemical processes. The report consist of eight chapters. In Chapter 1 the importance of actinide separation chemistry in the fields of waste management and its background are summarized.In Chapter 2 the types of waste streams are classified according to their relative importance, by physical form and by source of actinides. The basic data of actinide chemical thermodynamics, such as oxidation states, hydrolysis, complexation, sorption, Gibbs energies of formation, and volatility, were collected and are presented in Chapter 3. Actinide analyses related to separation processes are also mentioned in this chapter. The state of the art of actinide separation chemistry is classified in three groups, including hydrometallurgy, pyrochemical process and process based on fields, and is described in Chapter 4 along with the relationship of kinetics to separations. In Chapter 5 basic chemistry research needs and the inherent limitation on separation processes are discussed. Prioritization of research and development is discussed in Chapter 6 in the context of several attributes of waste management problems. These attributes include: mass or volume of waste; concentration of the actinide in the waste; expected difficulty of treating the wastes; short-term hazard of the waste; long-term hazard of the waste; projected cost of treatment; amount of secondary waste. Based on the priority, recommendations were made for the direction of future research

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2010-01-01

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

  6. Distribution of actinides in SFR1; Aktinidfoerdelning i SFR1

    Energy Technology Data Exchange (ETDEWEB)

    Ingemansson, Tor [ALARA Engineering, Skultuna (Sweden)

    2000-02-01

    The amount of actinides in the Swedish repository for intermediate level radioactive wastes has been estimated. The sources for the actinides are mainly the purification filters of the reactors and the used fuel pools. Defect fuel elements are the originating source of the actinides. It is estimated that the 12 Swedish reactors, in total, have had 2.2 kg of fuel dissolved in their systems since start-up. About 880 g of this amount has been brought to the intermediate-level repository.

  7. Status report on actinide and fission product transmutation studies

    International Nuclear Information System (INIS)

    The management of radioactive waste is one of the key issues in today's political and public discussions on nuclear energy. One of the fields that looks into the future possibilities of nuclear technology is the neutronic transmutation of actinides and of some most important fission products. Studies on transmutation of actinides are carried out in various countries and at an international level. This status report which gives an up-to-date general overview of current and planned research on transmutation of actinides and fission products in non-OECD countries, has been prepared by a Technical Committee meeting organized by the IAEA in September 1995. 168 refs, 16 figs, 34 tabs

  8. Review of actinide nitride properties with focus on safety aspects

    Energy Technology Data Exchange (ETDEWEB)

    Albiol, Thierry [CEA Cadarache, St Paul Lez Durance Cedex (France); Arai, Yasuo [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    2001-12-01

    This report provides a review of the potential advantages of using actinide nitrides as fuels and/or targets for nuclear waste transmutation. Then a summary of available properties of actinide nitrides is given. Results from irradiation experiments are reviewed and safety relevant aspects of nitride fuels are discussed, including design basis accidents (transients) and severe (core disruptive) accidents. Anyway, as rather few safety studies are currently available and as many basic physical data are still missing for some actinide nitrides, complementary studies are proposed. (author)

  9. Actinide interactions at microbial interfaces: an interdisciplinary challenge

    International Nuclear Information System (INIS)

    An overview on the current state of knowledge of microbial actinide interaction processes is presented. Several detailed examples of the interaction of aerobic soil bacteria (Pseudomonas, Bacillus and Deinococcus strains) with uranium and plutonium are discussed. Details of the nature of the bacterial functional groups involved in the interfacial actinide interaction process are reported. Based on time-resolved laser-induced fluorescence spectroscopy (TRLFS) and synchrotron X-ray absorption spectroscopy (XANES and EXAFS) studies, molecular-level mechanistic details of the different interaction processes are discussed. Areas of this emerging field in actinide research are outlined where additional information and integrated interdisciplinary research is required

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

    Energy Technology Data Exchange (ETDEWEB)

    Lumetta, Gregg J.; Braley, Jenifer C.; Sinkov, Sergey I.; Carter, Jennifer C.

    2012-08-22

    This report describes work conducted at the Pacific Northwest National Laboratory (PNNL) in Fiscal Year (FY) 2012 under the auspices of the Sigma Team for Minor Actinide Separation, funded by the U.S. Department of Energy Office of Nuclear Energy. Researchers at PNNL and Argonne National Laboratory (ANL) are investigating a simplified solvent extraction system for providing a single-step process to separate the minor actinide elements from acidic high-level liquid waste (HLW), including separating the minor actinides from the lanthanide fission products.

  11. Characterization of partitioning relevant lanthanide and actinide complexes by NMR spectroscopy; Charakterisierung von partitioningrelevanten Lanthaniden- und Actinidenkomplexen mittels NMR-Spektroskopie

    Energy Technology Data Exchange (ETDEWEB)

    Adam, Christian

    2016-01-15

    In the present work the interaction of N-donor ligands, such as 2,6-Bis(5,6-dipropyl-1,2,4-triazin-3-yl)pyridine (nPrBTP) and 2,6-Bis(5-(2,2-dimethylpropyl)1H-pyrazol)-3-yl-pyridine (C5-BPP), with trivalent lanthanide and actinide ions was studied. Ligands of this type show a high selectivity for the separation of trivalent actinide ions over lanthanides from nitric acid solutions. However, the reason for this selectivity, which is crucial for future partitioning and transmutation strategies for radioactive wastes, is still unknown. So far, the selectivity of some N-donor ligands is supposed to be an effect of an increased covalency in the actinide-ligand bond, compared to the lanthanide compounds. NMR spectroscopy on paramagnetic metal complexes is an excellent tool for the elucidation of bonding modes. The overall paramagnetic chemical shift consists of two contributions, the Fermi Contact Shift (FCS), due to electron spin delocalisation through covalent bonds, and the Pseudo Contact Shift (PCS), which describes the dipolar coupling of the electron magnetic moment and the nuclear spin. By assessing the FCS share in the paramagnetic shift, the degree of covalency in the metal-ligand bond can be gauged. Several methods to discriminate FCS and PCS have been used on the data of the nPrBTP- and C5-BPP-complexes and were evaluated regarding their applicability on lanthanide and actinide complexes with N-donor ligands. The study comprised the synthesis of all Ln(III) complexes with the exceptions of Pm(III) and Gd(III) as well as the Am(III) complex as a representative of the actinide series with both ligands. All complexes were fully characterised ({sup 1}H, {sup 13}C and {sup 15}N spectra) using NMR spectroscopy. By isotope enrichment with the NMR-active {sup 15}N in positions 8 and 9 in both ligands, resonance signals of these nitrogen atoms were detected for all complexes. The Bleaneymethod relies on different temperature dependencies for FCS (T{sup -1}) and PCS (T

  12. Macroscopic multigroup constants for accelerator driven system core calculation

    International Nuclear Information System (INIS)

    The high-level wastes stored in facilities above ground or shallow repositories, in close connection with its nuclear power plant, can take almost 106 years before the radiotoxicity became of the order of the background. While the disposal issue is not urgent from a technical viewpoint, it is recognized that extended storage in the facilities is not acceptable since these ones cannot provide sufficient isolation in the long term and neither is it ethical to leave the waste problem to future generations. A technique to diminish this time is to transmute these long-lived elements into short-lived elements. The approach is to use an Accelerator Driven System (ADS), a sub-critical arrangement which uses a Spallation Neutron Source (SNS), after separation the minor actinides and the long-lived fission products (LLFP), to convert them to short-lived isotopes. As an advanced reactor fuel, still today, there is a few data around these type of core systems. In this paper we generate macroscopic multigroup constants for use in calculations of a typical ADS fuel, take into consideration, the ENDF/BVI data file. Four energy groups are chosen to collapse the data from ENDF/B-VI data file by PREPRO code. A typical MOX fuel cell is used to validate the methodology. The results are used to calculate one typical subcritical ADS core. (author)

  13. Cryogenic gamma detectors enable direct detection of 236U and minor actinides for non-destructive assay

    International Nuclear Information System (INIS)

    We demonstrate the utility of a superconducting transition edge sensor (TES) γ-ray detector with high energy resolution and low Compton background for nondestructive assay (NDA) of a uranium sample from reprocessed nuclear fuel. We show that TES γ-detectors can separate low-energy actinide γ-emissions from the background and nearby lines, even from minor isotopes whose signals are often obscured in NDA with conventional Ge detectors. Superconducting γ-detectors may therefore bridge the gap between high-accuracy destructive assay (DA) and easier-to-use NDA. (author)

  14. Solidification of simulated actinides by natural zircon

    Institute of Scientific and Technical Information of China (English)

    YANG Jian-Wen; LUO Shang-Geng

    2004-01-01

    Natural zircon was used as precursor material to produce a zircon waste form bearing 20wt% simulated actinides (Nd2O3 and UO2) through a solid state reaction by a typical synroc fabrication process. The fabricated zircon waste form has relatively good physical properties (density 5.09g/cm3, open porosity 4.0%, Vickers hardness 715kg/mm2). The XRD, SEM/EDS and TEM/EDS analyses indicate that there are zircon phases containing waste elements formed through the reaction. The chemical durability and radiation stability are determined by the MCC-1method and heavy ion irradiation; the results show that the zircon waste form is highly leach resistance and relatively stable under irradiation (amorphous dose 0.7dpa). From this study, the method of using a natural mineral to solidify radioactive waste has proven to be feasible.

  15. Actinide elements in aquatic and terrestrial environments

    International Nuclear Information System (INIS)

    Progress is reported in terrestrial ecology studies with regard to plutonium in biota from the White Oak Creek forest; comparative distribution of plutonium in two forest ecosystems; an ecosystem model of plutonium dynamics; actinide element metabolism in cotton rats; and crayfish studies. Progress is reported in aquatic studies with regard to transuranics in surface waters, frogs, benthic algae, and invertebrates from pond 3513; and radioecology of transuranic elements in cotton rats bordering waste pond 3513. Progress is also reported in stability of trivalent plutonium in White Oak Lake water; chemistry of plutonium, americium, curium, and uranium in pond water; uranium, thorium, and plutonium in small mammals; and effect of soil pretreatment on the distribution of plutonium

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

    Energy Technology Data Exchange (ETDEWEB)

    Mattsson, Ann Elisabet

    2012-01-01

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

  17. Sm isotope composition and Sm/Eu ratio determination in an irradiated 153Eu sample by ion exchange chromatography-quadrupole inductively coupled plasma mass spectrometry combined with double spike isotope dilution technique

    International Nuclear Information System (INIS)

    Within the framework of the research undertaken by the French Atomic Energy Commission on transmutation of long-lived radionuclides, targets of highly enriched actinides and fission products were irradiated in the fast neutron reactor Phenix. Precise and accurate measurements of the isotopic and elemental composition of the enriched elements are therefore required. In order to obtain the uncertainties of several per mil and to reduce handling time and exposure to analyst on radioactive material, the on-line coupling of ion exchange chromatography with quadrupole inductively coupled plasma mass spectrometry has been associated with the technique of the double spike isotope dilution. We present in this paper the results obtained on an irradiated sample of Europium oxide powder (enriched at 99.13% in 153Eu). After irradiation of around 5 mg of Eu2O3 powder the theoretical calculations predict the formation of several micrograms of gadolinium and samarium isotopes. In relation to the very high activity of the sample after irradiation and the very low quantity of Sm formed, the on-line ion exchange chromatography separation of Gd, Sm and Eu before Sm isotope ratio measurements has been developed for the quantification of the 152Sm/153Eu ratio. These on-line measurements were associated with the double spike isotope dilution technique after calibration of a 147Sm/151Eu spike solution. The external reproducibility of Sm isotopic ratios was determined to be around 0.5% (2 σ) resulting in a final uncertainty on the 152Sm/153Eu ratio of around 1% (2 σ). These on-line measurements present therefore a robust and high-throughput alternative to the thermal-ionisation mass spectrometry technique used so far in combination with off-line chromatographic separation, particularly in nuclear applications where characterisation of high activity sample solutions is required. (authors)

  18. The reduced transition probabilities for excited states of rare-earths and actinide even-even nuclei

    International Nuclear Information System (INIS)

    The theoretical B(E2) ratios have been calculated on DF, DR and Krutov models. A simple method based on the work of Arima and Iachello is used to calculate the reduced transition probabilities within SU(3) limit of IBA-I framework. The reduced E2 transition probabilities from second excited states of rare-earths and actinide even–even nuclei calculated from experimental energies and intensities from recent data, have been found to compare better with those calculated on the Krutov model and the SU(3) limit of IBA than the DR and DF models

  19. The reduced transition probabilities for excited states of rare-earths and actinide even-even nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Ghumman, S. S. [Department of Physics, Sant Longowal Institute of Engineering and Technology (Deemed University), Longowal, Sangrur-148106, Punjab, India s-ghumman@yahoo.com (India)

    2015-08-28

    The theoretical B(E2) ratios have been calculated on DF, DR and Krutov models. A simple method based on the work of Arima and Iachello is used to calculate the reduced transition probabilities within SU(3) limit of IBA-I framework. The reduced E2 transition probabilities from second excited states of rare-earths and actinide even–even nuclei calculated from experimental energies and intensities from recent data, have been found to compare better with those calculated on the Krutov model and the SU(3) limit of IBA than the DR and DF models.

  20. Pyrometallurgical processes for recovery of actinide elements

    Energy Technology Data Exchange (ETDEWEB)

    Battles, J.E.; Laidler, J.J.; McPheeters, C.C.; Miller, W.E.

    1994-01-01

    A metallic fuel alloy, nominally U-20-Pu-lOZr, is the key element of the Integral Fast Reactor (IFR) fuel cycle. Metallic fuel permits the use of an innovative, simple pyrometallurgical process, known as pyroprocessing, (the subject of this report), which features fused salt electrorefining of the spent fuel. Electrorefining separates the actinide elements from fission products, without producing a separate stream of plutonium. The plutonium-bearing product is contaminated with higher actinides and with a minor amount of rare earth fission products, making it diversion resistant while still suitable as a fuel material in the fast spectrum of the IFR core. The engineering-scale demonstration of this process will be conducted in the refurbished EBR-II Fuel Cycle Facility, which has entered the start-up phase. An additional pyrometallurgical process is under development for extracting transuranic (TRU) elements from Light Water Reactor (LWR) spent fuel in a form suitable for use as a feed to the IFR fuel cycle. Four candidate extraction processes have been investigated and shown to be chemically feasible. The main steps in each process are oxide reduction with calcium or lithium, regeneration of the reductant and recycle of the salt, and separation of the TRU product from the bulk uranium. Two processes, referred to as the lithium and salt transport (calcium reductant) processes, have been selected for engineering-scale demonstration, which is expected to start in late 1993. An integral part of pyroprocessing development is the treatment and packaging of high-level waste materials arising from the operations, along with the qualification of these waste forms for disposal in a geologic repository.

  1. Pyrometallurgical processes for recovery of actinide elements

    International Nuclear Information System (INIS)

    A metallic fuel alloy, nominally U-20-Pu-lOZr, is the key element of the Integral Fast Reactor (IFR) fuel cycle. Metallic fuel permits the use of an innovative, simple pyrometallurgical process, known as pyroprocessing, (the subject of this report), which features fused salt electrorefining of the spent fuel. Electrorefining separates the actinide elements from fission products, without producing a separate stream of plutonium. The plutonium-bearing product is contaminated with higher actinides and with a minor amount of rare earth fission products, making it diversion resistant while still suitable as a fuel material in the fast spectrum of the IFR core. The engineering-scale demonstration of this process will be conducted in the refurbished EBR-II Fuel Cycle Facility, which has entered the start-up phase. An additional pyrometallurgical process is under development for extracting transuranic (TRU) elements from Light Water Reactor (LWR) spent fuel in a form suitable for use as a feed to the IFR fuel cycle. Four candidate extraction processes have been investigated and shown to be chemically feasible. The main steps in each process are oxide reduction with calcium or lithium, regeneration of the reductant and recycle of the salt, and separation of the TRU product from the bulk uranium. Two processes, referred to as the lithium and salt transport (calcium reductant) processes, have been selected for engineering-scale demonstration, which is expected to start in late 1993. An integral part of pyroprocessing development is the treatment and packaging of high-level waste materials arising from the operations, along with the qualification of these waste forms for disposal in a geologic repository

  2. In-situ monitoring of actinides and rare earth elements by electrothermal hollow cathode discharge spectrometry

    International Nuclear Information System (INIS)

    This report describes an Electrothermal Hollow Cathode Discharge Spectrometry (ET-HCDS) source being constructed for the analytical determination of actinides and rare earth elements. This work was initiated with the support of the Office of Safeguards and Security; the Buried Waste Integrated Demonstration began funding work in this area in mid-FY1992 and the work is continuing into FY1993 with funds from both sources. Special features of this instrument should permit it to be used for the determination of individual isotopic species, which is important for safeguard's materials control and accountancy. ET-HCDS can be achieved using compact instrumentation suitable for use in field laboratories. The technique is capable of determining a suite of environmentally-important species, such as the actinides and the heavy metals, in a variety of physical forms (e.g., in solution, as found on air particulates, or in soils). ET-HCDS should be capable of very sensitive analyses and should require very small samples (e.g., microgram). Since ET-HCDS is possible in an air atmosphere (at reduced pressures), it may be useful for the real-time determination of hazardous materials, both radioactive and non radioactive, contained in dusts released during waste retrieval operations; ET-HCDS should also be useful for the rapid and sensitive analysis of metals in soils

  3. Calculation of the absorbed dose for contamination in skin imparted by beta radiation through the Varskin code modified for 122 isotopes of interest for nuclear medicine, nuclear plants and research; Calculo de dosis absorbida para contaminacion en piel impartida por radiacion beta mediante el codigo Varskin modificado para 122 isotopos de interes para medicina nuclear, plantas nucleares e investigacion

    Energy Technology Data Exchange (ETDEWEB)

    Alvarez R, J.T

    1992-06-15

    In this work the implementation of a modification of the Varskin code for calculation of absorbed dose by contamination in skin imparted by external radiation fields generated by beta emitting is presented. The necessary data for the execution of the code are: isotope, dose depth, isotope activity, geometry type, source radio and time of integration of the isotope, being able to execute combinations of up to five radionuclides. This program it was implemented in Fortran 5 by means of the FFSKIN source program and the executable one in binary language BFFSKIN being the maximum execution time of 5 minutes. (Author)

  4. Nuclear Data for Reactor Physics: Cross sections and level densities in the actinide region

    Directory of Open Access Journals (Sweden)

    Bernstein L.

    2010-03-01

    Full Text Available Nuclear data in the actinide region are particularly important because they are basis behind all simulations of nuclear reactor core behaviour over both long time scales (fuel depletion and waste production and short time scales (accident scenarios. Nuclear reaction cross sections must be known as precisely as possible so that core reaction rates can be accurately calculated. Although cross section measurements in this region have been widely performed, for certain nuclei, particularly those with short half lives, direct measurements are either very difficult or impossible and thus reactor simulations must rely on theoretical calculations or extrapolations from neighbouring nuclei. The greatest uncertainty in theoretical cross section calculations comes from the lack of knowledge of level densities, for which predicted values can often be incorrect by a factor of two or more. Therefore there is a strong case for a systematic experimental study of level densities in the actinide region for the purpose of a providing a stringent test of theoretical cross section calculations for nuclei where experimental cross section data are available and b for providing better estimations of cross sections for nuclei in which no cross section data are available.

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

    Science.gov (United States)

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

    2015-10-01

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

  6. Neutron skin in Osmium isotopes

    International Nuclear Information System (INIS)

    Here we have made an attempt to calculate neutron skin thickness in rare earth even-even osmium isotopes. The selected isotopes ranges from 2-p to 2-n drip line. Neutron skin is an important feature of neutron rich nuclei. The ground state proton and neutron rms radii have been calculated using HFB approximation. A comparison of calculated radii have been done by using two different Skyrme parameterizations and two different basis

  7. An atomic beam source for actinide elements: concept and realization

    International Nuclear Information System (INIS)

    For ultratrace analysis of actinide elements and studies of their atomic properties with resonance ionization mass spectroscopy (RIMS), efficient and stable sources of actinide atomic beams are required. The thermodynamics and kinetics of the evaporation of actinide elements and oxides from a variety of metals were considered, including diffusion, desorption, and associative desorption. On this basis various sandwich-type filaments were studied. The most promising system was found to consist of tantalum as the backing material, an electrolytically deposited actinide hydroxide as the source of the element, and a titanium covering layer for its reduction to the metal. Such sandwich sources were experimentally proven to be well suited for the production of atomic beams of plutonium, curium, berkelium and californium at relatively low operating temperatures and with high and reproducible yields. (orig.)

  8. Distribution of actinide elements in sediments: leaching studies

    International Nuclear Information System (INIS)

    Previous investigations have shown that Fe and Mn oxides and organic matter can significantly influence the behavior of Pu and other actinides in the environment. A sequential leaching procedure has been developed in order to investigate the solid phase distribution of the actinides in riverine and marine sediments. Seven different sedimentary fractions are defined by this leaching experiment: an exchangeable metals fraction, an organic fraction, a carbonate fraction, a Mn oxide fraction, an amorphous Fe fraction, a crystalline Fe oxide fraction and a lattice-held or residual fraction. There is also the option of including a metal sufide fraction. A preliminary experiment, analyzing only the metals and not the actinide elements, indicates that this leaching procedure (with some modifications) is a viable procedure. The subsequent data should result in information concerning the geochemical history and behavior of these actinide elements in the environment

  9. Element Partitioning in Glass-Ceramic Designed for Actinides Immobilization

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    <正>Glass-ceramics were designed for immobilization of actinides. In order to immobilizing more wastes in the matrix and to develop the optimum formulation for the glass-ceramic, it is necessary to study the

  10. Advanced techniques for actinide spectroscopy (ATAS 2012). Abstract book

    International Nuclear Information System (INIS)

    The abstract book of the International workshop on advanced techniques for actinide spectroscopy (ATAS 2012) include contributions concerning the following issues: environmental applications, NMR spectroscopy, vibrational spectroscopy, X-ray spectroscopy and theory, technical application: separation processes, emission spectroscopy.

  11. In-situ mineralization of actinides with phytic acid

    International Nuclear Information System (INIS)

    A new approach to the remediation of actinide contamination is described. A hydrolytically unstable organophosphorus compound, phytic acid, is introduced into the contaminated environment. In the short term (up to several hundred years), phytate acts as a cation exchanger to absorb mobile actinide ions from ground waters. Ultimately, phytate decomposes to release phosphate and promote the formation of insoluble phosphate mineral phases, considered an ideal medium to immobilize actinides, as it forms compounds with the lowest solubility of any candidate mineral species. This overview will discuss the rate of hydrolysis of phytic acid, the formation of lanthanide/actinide phosphate mineral forms, the cation exchange behavior of insoluble phytate, and results from laboratory demonstration of the application to soils from the Fernald site

  12. Advanced techniques for actinide spectroscopy (ATAS 2012). Abstract book

    Energy Technology Data Exchange (ETDEWEB)

    Foerstendorf, Harald; Mueller, Katharina; Steudtner, Robin (eds.)

    2012-07-01

    The abstract book of the International workshop on advanced techniques for actinide spectroscopy (ATAS 2012) include contributions concerning the following issues: environmental applications, NMR spectroscopy, vibrational spectroscopy, X-ray spectroscopy and theory, technical application: separation processes, emission spectroscopy.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2008-09-01

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

  14. Improved methods for Feynman path integral calculations of vibrational-rotational free energies and application to isotopic fractionation of hydrated chloride ions.

    Science.gov (United States)

    Mielke, Steven L; Truhlar, Donald G

    2009-04-23

    We present two enhancements to our methods for calculating vibrational-rotational free energies by Feynman path integrals, namely, a sequential sectioning scheme for efficiently generating random free-particle paths and a stratified sampling scheme that uses the energy of the path centroids. These improved methods are used with three interaction potentials to calculate equilibrium constants for the fractionation behavior of Cl(-) hydration in the presence of a gas-phase mixture of H(2)O, D(2)O, and HDO. Ion cyclotron resonance experiments indicate that the equilibrium constant, K(eq), for the reaction Cl(H(2)O)(-) + D(2)O right harpoon over left harpoon Cl(D(2)O)(-) + H(2)O is 0.76, whereas the three theoretical predictions are 0.946, 0.979, and 1.20. Similarly, the experimental K(eq) for the Cl(H(2)O)(-) + HDO right harpoon over left harpoon Cl(HDO)(-) + H(2)O reaction is 0.64 as compared to theoretical values of 0.972, 0.998, and 1.10. Although Cl(H(2)O)(-) has a large degree of anharmonicity, K(eq) values calculated with the harmonic oscillator rigid rotator (HORR) approximation agree with the accurate treatment to within better than 2% in all cases. Results of a variety of electronic structure calculations, including coupled cluster and multireference configuration interaction calculations, with either the HORR approximation or with anharmonicity estimated via second-order vibrational perturbation theory, all agree well with the equilibrium constants obtained from the analytical surfaces.

  15. The isotopic distribution conundrum.

    Science.gov (United States)

    Valkenborg, Dirk; Mertens, Inge; Lemière, Filip; Witters, Erwin; Burzykowski, Tomasz

    2012-01-01

    Although access to high-resolution mass spectrometry (MS), especially in the field of biomolecular MS, is becoming readily available due to recent advances in MS technology, the accompanied information on isotopic distribution in high-resolution spectra is not used at its full potential, mainly because of lack of knowledge and/or awareness. In this review, we give an insight into the practical problems related to calculating the isotopic distribution for large biomolecules, and present an overview of methods for the calculation of the isotopic distribution. We discuss the key events that triggered the development of various algorithms and explain the rationale of how and why the various isotopic-distribution calculations were performed. The review is focused around the developmental stages as briefly outlined below, starting with the first observation of an isotopic distribution. The observations of Beynon in the field of organic MS that chlorine appeared in a mass spectrum as two variants with odds 3:1 lie at the basis of the first wave of algorithms for the calculation of the isotopic distribution, based on the atomic composition of a molecule. From here on, we explain why more complex biomolecules such as peptides exhibit a highly complex isotope pattern when assayed by MS, and we discuss how combinatorial difficulties complicate the calculation of the isotopic distribution on computers. For this purpose, we highlight three methods, which were introduced in the 1980s. These are the stepwise procedure introduced by Kubinyi, the polynomial expansion from Brownawell and Fillippo, and the multinomial expansion from Yergey. The next development was instigated by Rockwood, who suggested to decompose the isotopic distribution in terms of their nucleon count instead of the exact mass. In this respect, we could claim that the term "aggregated" isotopic distribution is more appropriate. Due to the simplification of the isotopic distribution to its aggregated counterpart

  16. Rare Earth element (REE) incorporation in natural calcite. Upper limits for actinide uptake in a secondary phase

    Energy Technology Data Exchange (ETDEWEB)

    Stipp, S.L.S.; Christensen, J.T.; Waight, T.E. [Geological Inst., Univ. of Copenhagen (Denmark); Lakshtanov, L.Z. [Geological Inst., Univ. of Copenhagen (Denmark); Inst. of Experimental Mineralogy, Russian Academy of Science, Chernogolovka (Russian Federation); Baker, J.A. [School of Earth Sciences, Victoria Univ. of Wellington (New Zealand)

    2006-07-01

    Secondary minerals have the potential to sequester escaped actinides in the event of a radioactive waste repository failure, but currently, data to define their maximum uptake capacity are generally lacking. To estimate a maximum limit for solid solution in calcite, we took advantage of the behavioural similarities of the 4f-orbital lanthanides with some of the 5f-orbital actinides and used rare Earth element (REE) concentration as an analogue. A suite of 65 calcite samples, mostly pure single crystals, was assembled from a range of geological settings, ages and locations and analysed by isotope dilution MC-ICP-MS (multiple-collector inductively-coupled plasma mass spectroscopy). All samples were shown to contain significant lanthanide concentrations. The highest were in calcite formed from hydrothermal solutions and from carbonatite magma. Maximum total mole fraction of REE was 4.72 x 10{sup -4}, which represents one substituted atom for about 2000 Ca sites. In comparison, synthetic calcite, precipitated at growth rates slow enough to insure solid solution formation, incorporated 7.5 x 10{sup -4} mole fraction Eu(III). For performance assessment, we propose that 7.5 mmole substitution/kg calcite should be considered the upper limit for actinide incorporation in secondary calcite. The largest source of uncertainty in this estimate results from extrapolating lanthanide data to actinides. However, the data offer confidence that for waters in the hydrothermal temperature range, such as in the near-field, or at groundwater temperatures, such as in the far-field, if calcite formation is favoured and actinides are present, those with behaviour like the trivalent lanthanides, especially Am{sup 3+} and Cm{sup 3+}, will be incorporated. REE are abundant and widely distributed, and they have remained in calcite for millions of years. Thus, one can be certain that incorporated actinides will also remain immobilised in calcite formed in fractures and pore spaces, as long as

  17. Electronic structure and properties of rare earth and actinide intermetallics

    International Nuclear Information System (INIS)

    There are 188 contributions, experimental and theoretical, a few on rare earth and actinide elements but mostly on rare earth and actinide intermetallic compounds and alloys. The properties dealt with include 1) crystal structure, 2) magnetic properties and magnetic structure, 3) magnetic phase transformations and valence fluctuations, 4) electrical properties and superconductivity and their temperature, pressure and magnetic field dependence. A few papers deal with crystal growth and novel measuring methods. (G.Q.)

  18. Ultrasensitive detection of actinides and technetium by laser resonance ionization mass spectrometry

    International Nuclear Information System (INIS)

    The application of laser resonance ionization mass spectrometry for the detection of extremely small numbers of atoms has been explored in the very recent years. High sensitivity and unambiguity in element and isotope identification can be achieved by three-step photoionization of the elements in the atomic state followed by time-of-flight mass analysis. The laser system for photoionization consists of three dye lasers which are pumped simultaneously by a copper vapor laser. For mass determination a time-of-flight spectrometer with a mass resolution better than 1500 is used. By ionization via autoionizing states and by saturation in each excitation step a detection limit of about 107 atoms of actinides or of technetium in the sample has been obtained

  19. The effect of corrosion product colloids on actinide transport

    International Nuclear Information System (INIS)

    The near field of the proposed UK repository for ILW/LLW will contain containers of conditioned waste in contact with a cementious backfill. It will contain significant quantities of iron and steel, Magnox and Zircaloy. Colloids deriving from their corrosion products may possess significant sorption capacity for radioelements. If the colloids are mobile in the groundwater flow, they could act as a significant vector for activity transport into the far field. The desorption of plutonium and americium from colloidal corrosion products of iron and zirconium has been studied under chemical conditions representing the transition from the near field to the far field. Desorption Rd values of ≥ 5 x 106 ml g-1 were measured for both actinides on these oxides and hydroxides when actinide sorption took place under the near-field conditions and desorption took place under the far-field conditions. Desorption of the actinides occurred slowly from the colloids under far-field conditions when the colloids had low loadings of actinide and more quickly at high loadings of actinide. Desorbed actinide was lost to the walls of the experimental vessel. (author)

  20. Research on the actinide chemistry in Nuclear Fuel Cycle

    International Nuclear Information System (INIS)

    Fundamental technique to measure chemical behaviors and properties of lanthanide and actinide in radioactive waste is necessary for the development of pryochemical process. First stage, the electrochemical/spectroscopic integrated measurement system was designed and set up for spectro-electrochemical measurements of lanthanide and actinide ions in high temperature molten salt media. A compact electrochemical cell and electrode system was also developed for the minimization of reactants, and consequently minimization of radioactive waste generation. By applying these equipments, oxidation and reduction behavior of lanthanide and actinide ions in molten salt media have been made. Also, thermodynamic parameter values are determined by interpreting the results obtained from electrochemical measurements. Several lanthanide ions exhibited fluorescence properties in molten salt. Also, UV-VIS measurement provided the detailed information regarding the oxidation states of lanthanide and actinide ions in high temperature molten salt media. In the second stage, measurement system for physical properties at pyrochemical process such as viscosity, melting point and conductivity is established, and property database at different compositions of lanthanide and actinide is collected. And, both interactions between elements and properties with different potential are measured at binary composition of actinide-lanthanide in molten salt using electrochemical/spectroscopic integrated measurement system.

  1. Isotopic geology

    International Nuclear Information System (INIS)

    Born from the application to geology of nuclear physics techniques, the isotopic geology has revolutionized the Earth's sciences. Beyond the dating of rocks, the tracer techniques have permitted to reconstruct the Earth's dynamics, to measure the temperatures of the past (giving birth to paleoclimatology) and to understand the history of chemical elements thanks to the analysis of meteorites. Today, all domains of Earth sciences appeal more or less to the methods of isotopic geology. In this book, the author explains the principles, methods and recent advances of this science: 1 - isotopes and radioactivity; 2 - principles of isotope dating; 3 - radio-chronological methods; 4 - cosmogenic isotope chronologies; 5 - uncertainties and radio-chronological results; 6 - geochemistry of radiogenic isotopes; 7 - geochemistry of stable isotopes; 8 - isotopic geology and dynamical analysis of reservoirs. (J.S.)

  2. High-spin states in boson models with applications to actinide nuclei

    CERN Document Server

    Kuyucak, S

    1995-01-01

    We use the 1/N expansion formalism in a systematic study of high-spin states in the sd and sdg boson models with emphasis on spin dependence of moment of inertia and E2 transitions. The results are applied to the high-spin states in the actinide nuclei ^{232}Th, ^{234-238}U, where the need for g bosons is especially acute but until now, no realistic calculation existed. We find that the d-boson energy plays a crucial role in description of the high-spin data.

  3. Electronic structure, cohesive, and magnetic properties of the actinide-iridium Laves phases

    International Nuclear Information System (INIS)

    The electronic structure of the isostructural AIr2 systems (A = Th, Pa, U, Np, Pu, and Am) has been obtained by means of the scalar relativistic and fully relativistic linear muffin-tin orbital techniques. Ground-state properties such as lattice constants and onset of magnetic order have been calculated and compared with measured data. The hybridization between the actinide 5f and the ligand 5d states and the direct 5f wave-function overlap are found to be of comparable importance for the bandwidth of the itinerant 5f states. The anomalous paramagnetism of PuIr2 can be explained only by a fully relativistic treatment

  4. Calculation of the inventory and near-field release rates of radioactivity from neutron-activated metal parts discharged from the high flux isotope reactor and emplaced in solid waste storage area 6 at Oak Ridge National Laboratory

    International Nuclear Information System (INIS)

    Emplacement of contaminated reactor components involves disposal in lined and unlined auger holes in soil above the water table. The radionuclide inventory of disposed components was calculated. Information on the composition and weight of the components, as well as reasonable assumptions for the neutron flux fueling use, the time of neutron exposure, and radioactive decay after discharge, were employed in the inventory calculation. Near-field release rates of 152Eu, 154Eu, and 155Eu from control plates and cylinders were calculated for 50 years after emplacement. Release rates of the europium isotopes were uncertain. Two release-rate-limiting models were considered and a range of reasonable values were assumed for the time-to-failure of the auger-hole linear and aluminum cladding and europium solubility in SWSA-6 groundwater. The bounding europium radionuclide near-field release rates peaked at about 1.3 Ci/year total for /sup 152,154,155/Eu in 1987 for the lower bound, and at about 420 Ci/year in 1992 for the upper bound. The near-field release rates of 55Fe, 59Ni, 60Co, and 63Ni from stainless steel and cobalt alloy components, as well as of 10Be, 41Ca, and 55Fe from beryllium reflectors, were calculated for the next 100 years, assuming bulk waste corrosion was the release-rate-limiting step. Under the most conservative assumptions for the reflectors, the current (1986) total radionuclide release rate was calculated to be about 1.2 x 10-4 Ci/year, decreasing by 1992 to a steady release of about 1.5 x 10-5 Ci/year due primarily to 41Ca. 50 refs., 13 figs., 8 tabs

  5. Calculation of the inventory and near-field release rates of radioactivity from neutron-activated metal parts discharged from the high flux isotope reactor and emplaced in solid waste storage area 6 at Oak Ridge National Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Kelmers, A.D.; Hightower, J.R.

    1987-05-01

    Emplacement of contaminated reactor components involves disposal in lined and unlined auger holes in soil above the water table. The radionuclide inventory of disposed components was calculated. Information on the composition and weight of the components, as well as reasonable assumptions for the neutron flux fueling use, the time of neutron exposure, and radioactive decay after discharge, were employed in the inventory calculation. Near-field release rates of /sup 152/Eu, /sup 154/Eu, and /sup 155/Eu from control plates and cylinders were calculated for 50 years after emplacement. Release rates of the europium isotopes were uncertain. Two release-rate-limiting models were considered and a range of reasonable values were assumed for the time-to-failure of the auger-hole linear and aluminum cladding and europium solubility in SWSA-6 groundwater. The bounding europium radionuclide near-field release rates peaked at about 1.3 Ci/year total for /sup 152,154,155/Eu in 1987 for the lower bound, and at about 420 Ci/year in 1992 for the upper bound. The near-field release rates of /sup 55/Fe, /sup 59/Ni, /sup 60/Co, and /sup 63/Ni from stainless steel and cobalt alloy components, as well as of /sup 10/Be, /sup 41/Ca, and /sup 55/Fe from beryllium reflectors, were calculated for the next 100 years, assuming bulk waste corrosion was the release-rate-limiting step. Under the most conservative assumptions for the reflectors, the current (1986) total radionuclide release rate was calculated to be about 1.2 x 10/sup -4/ Ci/year, decreasing by 1992 to a steady release of about 1.5 x 10/sup -5/ Ci/year due primarily to /sup 41/Ca. 50 refs., 13 figs., 8 tabs.

  6. Measurement of fission cross-section of actinides at n_TOF for advanced nuclear reactors

    CERN Document Server

    Calviani, Marco; Montagnoli, G; Mastinu, P

    2009-01-01

    The subject of this thesis is the determination of high accuracy neutron-induced fission cross-sections of various isotopes - all of which radioactive - of interest for emerging nuclear technologies. The measurements had been performed at the CERN neutron time-of-flight facility n TOF. In particular, in this work, fission cross-sections on 233U, the main fissile isotope of the Th/U fuel cycle, and on the minor actinides 241Am, 243Am and 245Cm have been analyzed. Data on these isotopes are requested for the feasibility study of innovative nuclear systems (ADS and Generation IV reactors) currently being considered for energy production and radioactive waste transmutation. The measurements have been performed with a high performance Fast Ionization Chamber (FIC), in conjunction with an innovative data acquisition system based on Flash-ADCs. The first step in the analysis has been the reconstruction of the digitized signals, in order to extract the information required for the discrimination between fission fragm...

  7. Comparative food-chain behavior and distribution of actinide elements in and around a contaminated fresh-water pond

    International Nuclear Information System (INIS)

    The bioaccumulation of 233234U, 238U, 238Pu, 239240Pu, 241Am, and 244Cm in both native and introduced biota was studied at Pond 3513, a former low-level radioactive waste settling basin at Oak Ridge National Laboratory. This system, which was decommissioned in 1976 after more than 30 years use, contains approximately 5 Ci of 239240Pu; inventories of other actinide isotopes are considerably less. Significantly higher concentrations of actinides in fish that were allowed access to sediments indicated that sedimentary particulates may be the primary source of transuranics to biota in shallow fresh-water ecosystems. Our study determined habitat, in particular the degree of association of an organism with the sediment-water interface, to be the primary factor in controlling transuranic concentrations in aquatic biota. In most of the biological samples analyzed, excluding samples suspected of being contaminated by sediment, 241Am/239Pu, 244Cm/239Pu, and 238U/239Pu ratios were greater than the respective ratio in sediment while 233234U/238U, and 239240Pu/238Pu ratios were not different from the respective ratios in sediment. The relative uptake of actinides from contaminated sediment by aquatic and terrestrial biota at this site was U > Cm greater than or equal to Am > Pu. The relative extractability of actinides from shoreline sediment was U > Cm approx. = Am > Pu; we also observed the same relative ranking for sediment-water exchange in situ. Concentrations of transuranics in water, terrestrial vegetation, and vertebrate carcasses were less than 10% of the recommended public exposure maximum permissible concentration (MPC) of the ICRP

  8. Validation of SCALE (SAS2H) Isotopic Predictions for BWR Spent Fuel

    Energy Technology Data Exchange (ETDEWEB)

    Hermann, O.W.

    1998-01-01

    Thirty spent fuel samples obtained from boiling-water-reactor (BWR) fuel pins have been modeled at Oak Ridge National Laboratory using the SAS2H sequence of the SCALE code system. The SAS2H sequence uses transport methods combined with the depletion and decay capabilities of the ORIGEN-S code to estimate the isotopic composition of fuel as a function of its burnup history. Results of these calculations are compared with chemical assay measurements of spent fuel inventories for each sample. Results show reasonable agreement between measured and predicted isotopic concentrations for important actinides; however, little data are available for most fission products considered to be important for spent fuel concerns (e.g., burnup credit, shielding, source-term calculations, etc.). This work is a follow-up to earlier works that studied the ability to predict spent fuel compositions in pressurized-water-reactor (PWR) fuel pins. Biases and uncertainties associated with BWR isotopic predictions are found to be larger than those of PWR calculations. Such behavior is expected, as the operation of a BWR is significantly more complex than that of a PWR plant, and in general the design of a BWR has a more heterogeneous configuration than that of a PWR. Nevertheless, this work shows that the simple models employed using SAS2H to represent such complexities result in agreement to within 5% (and often less than 1%) or less for most nuclides important for spent fuel applications. On the other hand, however, the set of fuel samples analyzed represent a small subset of the BWR fuel population, and results reported herein may not be representative of the full population of BWR spent fuel.

  9. Validation of SCALE (SAS2H) isotopic predictions for BWR spent fuel

    Energy Technology Data Exchange (ETDEWEB)

    Hermann, O.W.; DeHart, M.D.

    1998-09-01

    Thirty spent fuel samples obtained from boiling-water-reactor (BWR) fuel pins have been modeled at Oak Ridge National Laboratory using the SAS2H sequence of the SCALE code system. The SAS2H sequence uses transport methods combined with the depletion and decay capabilities of the ORIGEN-S code to estimate the isotopic composition of fuel as a function of its burnup history. Results of these calculations are compared with chemical assay measurements of spent fuel inventories for each sample. Results show reasonable agreement between measured and predicted isotopic concentrations for important actinides; however, little data are available for most fission products considered to be important for spent fuel concerns (e.g., burnup credit, shielding, source-term calculations, etc.). This work is a follow-up to earlier works that studied the ability to predict spent fuel compositions in pressurized-water-reactor (PWR) fuel pins. Biases and uncertainties associated with BWR isotopic predictions are found to be larger than those of PWR calculations. Such behavior is expected, as the operation of a BWR is significantly more complex than that of a PWR plant, and in general the design of a BWR has a more heterogeneous configuration than that of a PWR. Nevertheless, this work shows that the simple models employed using SAS2H to represent such complexities result in agreement to within 5% (and often less than 1%) or less for most nuclides important for spent fuel applications. On the other hand, however, the set of fuel samples analyzed represent a small subset of the BWR fuel population, and results reported herein may not be representative of the full population of BWR spent fuel.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    1995-12-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-08-15

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

  12. Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples

    Science.gov (United States)

    Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; Spencer, Khalil J.

    2016-06-01

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics "toolbox", especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods.

  13. Isotope and Nuclear Chemistry Division annual report, FY 1990, October 1, 1989--September 30, 1990

    International Nuclear Information System (INIS)

    This report describes some of the major research and development programs of the Isotope and Nuclear Chemistry Division during FY 1990. The report includes articles on weapons chemistry, environmental chemistry, actinide and transition metal chemistry, geochemistry, nuclear structure and reactions, biochemistry and nuclear medicine, materials chemistry, and INC Division facilities and laboratories

  14. A quantum chemistry study of actinide(III) and lanthanide(III) complexes with tridentate nitrogen ligands

    Energy Technology Data Exchange (ETDEWEB)

    Guillaumont, D

    2004-07-01

    The structure and bonding in large complexes of actinide(III) and lanthanide(III) with tridentate N-donor ligands and water molecules have been investigated through quantum chemistry calculations in order to characterize the nature of the lanthanide-ligand and actinide-ligand bonds. Calculations have been performed using relativistic density functional theory on [M(L)(H{sub 2}O){sub 6}]{sup 3+}, [M(L)(H{sub 2}O){sub 5}Cl]{sup 2+} and [M(H{sub 2}O){sub 9}]{sup 3+} clusters where M = La, Ce, Nd, U, Pu, Am or Cm and L = 2,2':6'2''ter-pyridine (Terpy) or 2,6-bis(5,6-di-methyl-1,2,4-triazine-3-yl)pyridine (MeBtp). The calculated evolution of the M-L bond as a function of the cation shows that lanthanide-ligand distances decrease with the diminution of the ionic radius, whereas the actinide-ligand distances increase from uranium to americium and are shorter than Ln-N distances. These trends are explained by the presence of covalent effects in the metal-ligand decreasing in the order U > Pu > Am {approx_equal} Cm {approx_equal} Ln. (author)

  15. Effects of humic substances on the migration of radionuclides: complexation of actinides with humic substances. A commission of the European Communities program

    International Nuclear Information System (INIS)

    The aim of the research program is to study the complexation behavior of actinide ions with humic substances in natural aquifer systems and hence to quantify the effect of humic substances on the actinide migration. In the present research program the complexation of actinide ions with humic substances will be described thermodynamically. This description will be based on a simple model which will allow an easy introduction of the resulting reaction constants into geochemical modeling of actinide migration. To achieve the desired goal, the program is divided into three task; complexation reactions of actinide ions with well characterized reference and site-specific humic and fulvic acids, competition reactions with major cations in natural groundwaters, and validation of the complexation data in natural aquatic systems by comparison of calculation with spectroscopic experiment. This program is a continuation of the activities of the colloid and complexation (COCO) group in the second phase of the CEC-MIRAGE project. (authors). 39 refs., 5 figs., 4 tabs

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

    Energy Technology Data Exchange (ETDEWEB)

    Kenneth L. Nash

    2009-09-22

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

  17. Simultaneous analysis of matter radii, transition probabilities, and excitation energies of Mg isotopes by angular-momentum-projected configuration-mixing calculations

    Science.gov (United States)

    Shimada, Mitsuhiro; Watanabe, Shin; Tagami, Shingo; Matsumoto, Takuma; Shimizu, Yoshifumi R.; Yahiro, Masanobu

    2016-06-01

    We perform simultaneous analysis of (1) matter radii, (2) B (E 2 ;0+→2+) transition probabilities, and (3) excitation energies, E (2+) and E (4+) , for Mg-4024 by using the beyond-mean-field (BMF) framework with angular-momentum-projected configuration mixing with respect to the axially symmetric β2 deformation with infinitesimal cranking. The BMF calculations successfully reproduce all of the data for rm,B (E 2 ) , and E (2+) and E (4+) , indicating that it is quite useful for data analysis; particularly for low-lying states. We also discuss the absolute value of the deformation parameter β2 deduced from measured values of B (E 2 ) and rm. This framework makes it possible to investigate the effects of β2 deformation, the change in β2 due to restoration of rotational symmetry, β2 configuration mixing, and the inclusion of time-odd components by infinitesimal cranking. Under the assumption of axial deformation and parity conservation, we clarify which effect is important for each of the three measurements and propose the kinds of BMF calculations that are practical for each of the three kinds of observables.

  18. Laser isotope separation of gadolinium

    International Nuclear Information System (INIS)

    Basic studies on laser isotope separation of gadolinium were performed. Spectroscopic data were obtained such as isotope shifts and hyperfine structures using an atomic beam. Enrichment of 157Gd up to 80% was observed by three-step photoionization experiment using linearly polarized dye lasers. Design of an separation system was discussed by the help of computer calculation of excitation dynamics. (author)

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

    International Nuclear Information System (INIS)

    Chemical experiments were performed to examine the usefulness of heavy ion transfer reactions in producing new, neutron-rich actinide nuclides. A general quasi-elastic to deep-inelastic mechanism is proposed, and the utility of this method as opposed to other methods (e.g. complete fusion) is discussed. The relative merits of various techniques of actinide target synthesis are discussed. A description is given of a target system designed to remove the large amounts of heat generated by the passage of a heavy ion beam through matter, thereby maximizing the beam intensity which can be safely used in an experiment. Also described is a general separation scheme for the actinide elements from protactinium (Z=91) to mendelevium (Z=101), and fast specific procedures for plutonium, americium and berkelium. The cross sections for the production of several nuclides from the bombardment of 248Cm with 18O, 86Kr and 136Xe projectiles at several energies near and below the Coulomb barrier were determined. The results are compared with yields from 48Ca and 238U bombardments of 248Cm. Simple extrapolation of the product yields into unknown regions of charge and mass indicates that the use of heavy ion transfer reactions to produce new, neutron-rich above-target species is limited. The substantial production of neutron-rich below-target species, however, indicates that with very heavy ions like 136Xe and 238U the new species 248Am, 249Am and 247Pu should be produced with large cross sections from a 248Cm target. A preliminary, unsuccessful attempt to isolate 247Pu is outlined. The failure is probably due to the half life of the decay, which is calculated to be less than 3 minutes. The absolute gamma ray intensities from 251Bk decay, necessary for calculating the 251Bk cross section, are also determined

  20. Interaction of actinides with amino acids: from peptides to proteins

    International Nuclear Information System (INIS)

    Structural information on complexes of actinides with molecules of biological interest is required to better understand the mechanisms of actinides transport in living organisms, and can contribute to develop new decorporation treatments. Our study is about Th(IV), Np(IV), Pu(IV) and uranyl(VI) cations, which have a high affinity for some protein domains, and Fe(III), which is the natural cation of these biological systems. In this work, chelation of actinides has been brought to light with UV-visible-Near Infra Red spectroscopy, NMR, EPR, and ultrafiltration. Determination of the structure of the complexation site has been undertaken with Exafs measurements, and of the tertiary structure of the protein with SANS measurements. The first approach was to describe the interaction modes between actinides and essential chemical functions of proteins. Thus, the Ac-AspAspProAspAsp-NH2 peptide was studied as a possible chelate of actinides. Polynuclear species with μ-oxo or μ-hydroxo bridges were identified. The iron complex is binuclear, and the actinide ones have a higher nuclearity. The second approach was to study a real case of complexation of actinide with a protein: transferrin. Results show that around physiological ph a mononuclear complex is formed with Np(IV) and Pu(IV), while transferrin does not complex Th(IV) in the same conditions. Characteristic distances of M-transferrin complexes (M = Fe, Np, Pu) were determined. Moreover, the protein seems to be in its close conformation with Pu(IV), and in its open form with Np(IV) and UO22+. (author)

  1. Actinide production in 136Xe bombardments of 249Cf

    International Nuclear Information System (INIS)

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

  2. Determination of uranium, thorium and plutonium isotopes by ICP-MS

    International Nuclear Information System (INIS)

    Quantitative and isotopic measurement of actinide elements is required in many circumstances in the nuclear industry. For example, determination of very low levels of these alpha emitters in human urine samples is used to assess the internal committed dose for nuclear workers. Quantifying actinide isotopes in radioactive waste from nuclear processing and nuclear facility decommissioning provides important information for waste management. Accurate determination of the uranium isotopic ratios in reactor fuels provides fuel burnup information. Inductively coupled plasma mass spectrometry (ICP-MS) has been used for the determination of Th, U, and Pu in various samples including urine, nuclear waste, and nuclear fuel in our laboratory. In order to maximize the capability of the technique and ensure quality analyses, ICP-MS was used to analyze samples directly, or after pre-treatment to separate complicated matrices or to concentrate the analyte(s). High-efficiency sample introduction techniques were investigated. Spectral interferences to minor isotopes caused by peak tails and hydride ions of major actinide isotopes were studied in detail using solutions prepared with light and heavy waters. The quality of the isotopic ratio measurement was monitored using standard reference materials. (author)

  3. The decay heat of fission products and actinides of the SNR-300

    International Nuclear Information System (INIS)

    The report describes the computer code RASPA, which calculates the build-up and decay of fission products and actinides. The verification of the code and its library has been performed by comparison with theoretical and experimental results of other authors, whereby a good agreement has been achieved. Furthermore, an error analysis has shown, that the error of the calculated decay heat, which is induced by uncertainties of nuclear data, is less than 10 % up to decay times of one month. The results of calculations of the time dependent decay heat and the gamma source strength in various zones of the cores Mark-Ia and Mark-II of the SNR-300 are documented and discussed in detail

  4. A counter-intuitive approach to calculating non-exchangeable 2H isotopic composition of hair: treating the molar exchange fraction fE as a process-related rather than compound-specific variable

    Science.gov (United States)

    Landwehr, J.M.; Meier-Augenstein, W.; Kemp, H.F.

    2011-01-01

    Hair is a keratinous tissue that incorporates hydrogen from material that an animal consumes but it is metabolically inert following synthesis. The stable hydrogen isotope composition of hair has been used in ecological studies to track migrations of mammals as well as for forensic and archaeological purposes to determine the provenance of human remains or the recent geographic life trajectory of living people. Measurement of the total hydrogen isotopic composition of a hair sample yields a composite value comprised of both metabolically informative, non-exchangeable hydrogen and exchangeable hydrogen, with the latter reflecting ambient or sample preparation conditions. Neither of these attributes is directly measurable, and the non-exchangeable hydrogen composition is obtained by estimation using a commonly applied mathematical expression incorporating sample measurements obtained from two distinct equilibration procedures. This commonly used approach treats the fraction of exchangeable hydrogen as a mixing ratio, with a minimal procedural fractionation factor assumed to be close or equal to 1. Instead, we propose to use full molar ratios to derive an expression for the non-exchangeable hydrogen composition explicitly as a function of both the procedural fractionation factor α and the molar hydrogen exchange fraction fE. We apply these derivations in a longitudinal study of a hair sample and demonstrate that the molar hydrogen exchange fraction fE should, like the procedural fractionation factor α, be treated as a process-dependent parameter, i.e. a reaction-specific constant. This is a counter-intuitive notion given that maximum theoretical values for the molar hydrogen exchange fraction fE can be calculated that are arguably protein-type specific and, as such, fE could be regarded as a compound-specific constant. We also make some additional suggestions for future approaches to determine the non-exchangeable hydrogen composition of hair and the use of

  5. Studies on Neutron, Photon (Bremsstrahlung and Proton Induced Fission of Actinides and Pre-Actinides

    Directory of Open Access Journals (Sweden)

    H. Naik

    2015-08-01

    Full Text Available We present the yields of various fission products determined in the reactor neutron, 3.7-18.1 MeV quasi-mono energetic neutron, 8-80 MeV bremsstrahlung and 20-45 MeV proton induced fission of 232Th and 238U using radiochemical and off-line beta or gamma ray counting. The yields of the fission products in the bremsstrahlung induced fission natPb and 209Bi with 50- 70 MeV and 2.5 GeV based on off-line gamma ray spectrometric technique were also presented. From the yields of fission products, the mass chains yields were obtained using charge distribution correction. From the mass yield distribution, the peak-to-valley (P/V ratio was obtained. The role of excitation energy on the peak-to-valley ratio and fine structure such as effect of shell closure proximity and even-odd effect of mass yield distribution were examined. The higher yields of the fission products around A=133-134, 138-140 and 143-144 and their complementary products explained from the nuclear structure effect and role of standard I and II mode of asymmetric fission. In the neutron, photon (bremsstrahlung and proton induced fission, the asymmetric mass distribution for actinides (Th, U and symmetric distribution for pre-actinides (Pb, Bi were explained from different type of potential fission barrier

  6. Photofission of actinide and pre-actinide nuclei in the quasideuteron and delta energy regions

    CERN Document Server

    Berman, B L; Cole, P L; Dodge, W R; Feldman, G; Sanabria, J C; Kolb, N; Pywell, R E; Vogt, J; Nedorezov, V; Sudov, A; Kezerashvili, G Ya

    1999-01-01

    The photofission cross sections for the actinide nuclei sup 2 sup 3 sup 2 Th, sup 2 sup 3 sup 3 sup , sup 2 sup 3 sup 5 sup , sup 2 sup 3 sup 8 U, and sup 2 sup 3 sup 7 Np have been measured from 68 to 264 MeV and those for the pre-actinide nuclei sup 1 sup 9 sup 7 Au and sup N sup A sup T Pb from 122 to 222 MeV at the Saskatchewan Accelerator Laboratory, using monoenergetic tagged photons and novel parallel-plate avalanche detectors for the fission fragments. The aim of the experiment was to obtain a comprehensive and self-consistent data set and to investigate previous anomalous results in this energy region. The fission probability for transuranic nuclei is expected to be close to unity here. However, important discrepancies have been confirmed for sup 2 sup 3 sup 7 Np and sup 2 sup 3 sup 2 Th, compared with sup 2 sup 3 sup 8 U, which have serious implications for the inferred total photoabsorption strengths, and hence call into question the 'Universal Curve' for photon absorption at these energies. High-s...

  7. Simultaneous analysis of matter radii, transition probabilities, and excitation energies of Mg isotopes by angular-momentum-projected configuration-mixing calculations

    CERN Document Server

    Shimada, Mitsuhiro; Tagami, Shingo; Matsumoto, Takuma; Shimizu, Yoshifumi R; Yahiro, Masanobu

    2016-01-01

    We perform simultaneous analysis of (1) matter radii, (2) $B(E2; 0^+ \\rightarrow 2^+ )$ transition probabilities, and (3) excitation energies, $E(2^+)$ and $E(4^+)$, for $^{24-40}$Mg by using the beyond mean-field (BMF) framework with angular-momentum-projected configuration mixing with respect to the axially symmetric $\\beta_2$ deformation with infinitesimal cranking. The BMF calculations successfully reproduce all of the data for $r_{\\rm m}$, $B(E2)$, and $E(2^+)$ and $E(4^+)$, indicating that it is quite useful for data analysis, particularly for low-lying states. We also discuss the absolute value of the deformation parameter $\\beta_2$ deduced from measured values of $B(E2)$ and $r_{\\rm m}$. This framework makes it possible to investigate the effects of $\\beta_2$ deformation, the change in $\\beta_2$ due to restoration of rotational symmetry, $\\beta_2$ configuration mixing, and the inclusion of time-odd components by infinitesimal cranking. Under the assumption of axial deformation and parity conservation,...

  8. Lithium and magnesium isotopes fractionation by zone melting

    Science.gov (United States)

    Akimov, D. V.; Egorov, N. B.; Dyachenko, A. N.; Pustovalova, M. P.; Podoinikov, I. R.

    2016-06-01

    The process of changing isotopic composition of the lithium and magnesium salts was studied by using the process of zone melting. It was founded in the paper that the process of separation of the lithium isotopes is more effective than for magnesium isotopes when the conditions of process were the same. The coefficients of isotopes separation were calculated and have the next value: α = 1.006 for 26Mg isotope and α = 1.0022 for 6Li isotope.

  9. The actinides-a beautiful ending of the Periodic Table

    Energy Technology Data Exchange (ETDEWEB)

    Johansson, Boerje [Condensed Matter Theory Group, Department of Physics, Uppsala University, Box 530, S-751 21 Uppsala (Sweden); Applied Materials Physics, Department of Materials Science and Engineering, Royal Institute of Technology, Brinellvaegen 23, SE-100 44 Stockholm (Sweden)], E-mail: borje.johansson@fysik.uu.se; Li, Sa [Applied Materials Physics, Department of Materials Science and Engineering, Royal Institute of Technology, Brinellvaegen 23, SE-100 44 Stockholm (Sweden); Department of Physics, Virginia Commonwealth University, Richmond, VA 23284 (United States)

    2007-10-11

    The 5f elements, actinides, show many properties which have direct correspondence to the 4f transition metals, the lanthanides. The remarkable similarity between the solid state properties of compressed Ce and the actinide metals is pointed out in the present paper. The {alpha}-{gamma} transition in Ce is considered as a Mott transition, namely, from delocalized to localized 4f states. An analogous behavior is also found for the actinide series, where the sudden volume increase from Pu to Am can be viewed upon as a Mott transition within the 5f shell as a function of the atomic number Z. On the itinerant side of the Mott transition, the earlier actinides (Pa-Pu) show low symmetry structures at ambient conditions; while across the border, the heavier elements (Am-Cf) present the dhcp structure, an atomic arrangement typical for the trivalent lanthanide elements with localized 4f magnetic moments. The reason for an isostructural Mott transition of the f electron in Ce, as opposed to the much more complicated cases in the actinides, is identified. The strange appearance of the {delta}-phase (fcc) in the phase diagram of Pu is another consequence of the border line behavior of the 5f electrons. The path leading from {delta}-Pu to {alpha}-Pu is identified.

  10. Rapid determination of alpha emitters using Actinide resin.

    Science.gov (United States)

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

    2004-01-01

    The European Commission has recently published the recommended radiological protection criteria for the clearance of building and building rubble from the dismantling of nuclear installations. Radionuclide specific clearance levels for actinides are very low (between 0.1 and 1 Bq g(-1)). The prevalence of natural radionuclides in rubble materials makes the verification of these levels by direct alpha counting impossible. The capability of Actinide resin (Eichrom Industries, Inc.) for extracting plutonium and americium from rubble samples has been tested in this work. Besides a strong affinity for actinides in the tri, tetra and hexavalent oxidation states, this extraction chromatographic resin presents an easy recovery of absorbed radionuclides. The retention capability was evaluated on rubble samples spiked with certified radionuclide standards (239Pu and 241Am). Samples were leached with nitric acid, passed through a chromatographic column containing the resin and the elution fraction was measured by LSC. Actinide retention varies from 60% to 80%. Based on these results, a rapid method for the verification of clearance levels for actinides in rubble samples is proposed. PMID:15177360

  11. Development of the Chalmers Grouped Actinide Extraction Process

    Directory of Open Access Journals (Sweden)

    Halleröd Jenny

    2015-12-01

    Full Text Available Several solvents for Grouped ActiNide EXtraction (GANEX processes have been investigated at Chalmers University of Technology in recent years. Four different GANEX solvents; cyclo-GANEX (CyMe4- -BTBP, 30 vol.% tri-butyl phosphate (TBP and cyclohexanone, DEHBA-GANEX (CyMe4-BTBP, 20 vol.% N,N-di-2(ethylhexyl butyramide (DEHBA and cyclohexanone, hexanol-GANEX (CyMe4-BTBP, 30 vol.% TBP and hexanol and FS-13-GANEX (CyMe4-BTBP, 30 vol.% TBP and phenyl trifluoromethyl sulfone (FS-13 have been studied and the results are discussed and compared in this work. The cyclohexanone based solvents show fast and high extraction of the actinides but a somewhat poor diluent stability in contact with the acidic aqueous phase. FS-13-GANEX display high separation factors between the actinides and lanthanides and a good radiolytic and hydrolytic stability. However, the distribution ratios of the actinides are lower, compared to the cyclohexanone based solvents. The hexanol-GANEX is a cheap solvent system using a rather stable diluent but the actinide extraction is, however, comparatively low.

  12. Opportunities for isotope discoveries at FRIB

    Science.gov (United States)

    Baumann, T.; Hausmann, M.; Sherrill, B. M.; Tarasov, O. B.

    2016-06-01

    Expected production yields of the Facility for Rare Isotope Beams (FRIB) were calculated for a wide range of rare isotopes using the code LISE++ and planned performance parameters (Tarasov and Bazin, 2008; Bollen et al., 2011 [2]). A comparison between isotope discoveries of the last decade and expected particle yields indicates the range of isotopes that can likely be detected at FRIB. This paper will highlight recent isotope discoveries at NSCL's Coupled Cyclotron Facility and deduce how far the limits could be pushed with the Facility for Rare Isotope Beams.

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

    CERN Document Server

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

    2014-01-01

    Potential energy surfaces (PES's) of actinide nuclei are characterized by a two-humped barrier structure. At large deformations beyond the second barrier, the occurrence of a third one was predicted by macroscopic-microscopic model calculations in the 1970s but contradictory results were later obtained with a number of different models. In this paper, triple-humped barriers in actinide nuclei are investigated with covariant density functional theory (CDFT). Calculations are performed using the multidimensionally-constrained relativistic mean field (MDC-RMF) model, with functionals PC-PK1 and DD-ME2 in the particle-hole channel, while pairing correlations are treated in the BCS approximation with a separable and finite range pairing force. Two-dimensional PES's of $^{226,228,230,232}$Th and $^{232,234,236,238}$U are mapped and the third minima on these surfaces are located. In a second step the one-dimensional potential energy curves along the fission path are analyzed in detail and the energies of the second ...

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

    Directory of Open Access Journals (Sweden)

    Abdul Waris

    2008-03-01

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

  15. Stainless steel-zirconium alloy waste forms for metallic fission products and actinides during treatment of spent nuclear fuel

    International Nuclear Information System (INIS)

    Stainless steel-zirconium waste form alloys are being developed for the disposal of metallic wastes recovered from spent nuclear fuel using an electrometallurgical process developed by Argonne National Laboratory. The metal waste form comprises the fuel cladding, noble metal fission products and other metallic constituents. Two nominal waste form compositions are being developed: (1) stainless steel-15 wt% zirconium for stainless steel-clad fuels. The noble metal fission products are the primary source of radiation and their contribution to the waste form radioactivity has been calculated. The disposition of actinide metals in the waste alloys is also being explored. Simulated waste form alloys were prepared to study the baseline alloy microstructures and the microstructural distribution of noble metals and actinides, and to evaluate corrosion performance

  16. The characteristics of actinide nuclei production and accumulation accompanied with long-term utilization of nuclear energy

    Energy Technology Data Exchange (ETDEWEB)

    Yamana, Hajime [Kyoto Univ., Kumatori, Osaka (Japan). Research Reactor Inst.

    1997-03-01

    Aiming at quantitative and qualitative assessment of actinide-nuclides, which would accumulate through a long-term utilization of nuclear energy, a convenient calculation method for such assessment was proposed. The nuclides, Pu, Np, Am and Cm were used as the subject and the period of utilization of nuclear energy was supposed as 200 years to make integral assessment for different scenarios of nuclear energy utilization. The standard reactors supposed here were light water reactor charged with concentrated uranium, 1/3 MOX core light reactor and fast breeder reactor. Four kinds of scenarios; LWR(UOX), LWR(UOX+MOX), Pu Recycling FBR and MA Recycling FBR Scenarios were compared and quantitative results concerning those actinide nuclides including multi-recycling effects were obtained. From the aspect of long continuous production of poisonous substance, the most important problem was the production of {sup 241}Am followed by the presence of a large amount of plutonium. (M.N.)

  17. The efficacy of denaturing actinide elements as a means of decreasing materials attractiveness

    Energy Technology Data Exchange (ETDEWEB)

    Hase, K.R.; Bathke, C.G. [Los Alamos National Laboratory: P.O. Box 1663, Los Alamos, NM 87545 (United States); Ebbinghaus, B.B.; Sleaford, B.W.; Robel, M. [Lawrence Livermore National Laboratory: P.O. Box 808, Livermore, CA 94551 (United States); Collins, B.A.; Prichard, A.W. [Pacific Northwest National Laboratory: P.O. Box 999, Richland, WA 99352 (United States)

    2013-07-01

    This study considers the concept of denaturing as applied to the actinide elements present in spent fuel as a means to reduce materials attractiveness. Highly attractive materials generally have low values of bare critical mass, heat content, and dose. To denature an attractive element, its spent-fuel isotopic composition (isotopic vector) is intentionally modified by introducing sufficient quantities of a significantly less attractive isotope to dilute the concentration of a highly attractive isotope so that the overall attractiveness of the element is reduced. The authors used FOM (Figure of Merit) formula as the material attractiveness metric for their parametric determination of the attractiveness of the Pu and U. Materials attractiveness needs to be considered in three distinct phases in the process to construct a nuclear explosive device (NED): the acquisition phase, processing phase, and utilization phase. The results show that denaturing uranium with {sup 238}U is actually an effective means of reducing the attractiveness. For uranium with a large minority of {sup 235}U, a mixture of 80% {sup 238}U to 20% {sup 235}U is required to reduce the attractiveness to low. For uranium with a large concentration of {sup 233}U, a mixture of 88% {sup 238}U to 12% {sup 233}U is required to reduce the attractiveness to low. The results also show that denaturing plutonium with {sup 238}Pu is less effective than denaturing uranium with {sup 238}U. Using {sup 238}Pu as the denaturing agent would require 80% or more by mass in order to reduce the attractiveness to low. No amount of {sup 240}Pu is enough to reduce the plutonium attractiveness below medium. The combination of {sup 238}Pu and {sup 240}Pu would require approximately 70% {sup 238}Pu and 25% {sup 240}Pu by mass to reduce the plutonium attractiveness to low.

  18. 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

    International Nuclear Information System (INIS)

    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 241Am and 237Np 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 241Am isomeric branching ratio were precisely measured at thermal energy point. (author)

  19. Actinide consumption: Nuclear resource conservation without breeding

    Energy Technology Data Exchange (ETDEWEB)

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

    1991-01-01

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

  20. Actinide consumption: Nuclear resource conservation without breeding

    International Nuclear Information System (INIS)

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