WorldWideScience

Sample records for calculating actinide isotope

  1. Actinide isotopes compositions and neutrons emission rate calculations for irradiated research reactors fuel

    International Nuclear Information System (INIS)

    the availability of burn-up data is an essential first step in any systematic approach to the enhancement of safety, economics and performance of research reactors. A computer program has been designed to solve the system of equations describing the depletion, decay and production of uranium, plutonium and transplutonium nuclides. monte Carlo code was used to calculate the effective one group microscopic cross sections averaged over ETRR-1 fuel cell. the compositions of actinide isotopes, burn-up and neutrons emission rate have been calculated as a function of irradiation time and cooling time. results indicate that the amount of plutonium produced and neutrons emission rate are strongly dependent on the fuel burn-up

  2. Actinide isotopic analysis systems

    International Nuclear Information System (INIS)

    This manual provides instructions and procedures for using the Lawrence Livermore National Laboratory's two-detector actinide isotope analysis system to measure plutonium samples with other possible actinides (including uranium, americium, and neptunium) by gamma-ray spectrometry. The computer program that controls the system and analyzes the gamma-ray spectral data is driven by a menu of one-, two-, or three-letter options chosen by the operator. Provided in this manual are descriptions of these options and their functions, plus detailed instructions (operator dialog) for choosing among the options. Also provided are general instructions for calibrating the actinide isotropic analysis system and for monitoring its performance. The inventory measurement of a sample's total plutonium and other actinides content is determined by two nondestructive measurements. One is a calorimetry measurement of the sample's heat or power output, and the other is a gamma-ray spectrometry measurement of its relative isotopic abundances. The isotopic measurements needed to interpret the observed calorimetric power measurement are the relative abundances of various plutonium and uranium isotopes and americium-241. The actinide analysis system carries out these measurements. 8 figs

  3. 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....

  4. Generation of an actinide isotopes cross section set for fast reactor calculations using data from ENDL and ENDF/B-IV

    International Nuclear Information System (INIS)

    A Bondarenko format 25-group cross section set of actinide isotopes was generated for the fuel cycle evaluation and the incineration study in fast reactor systems. Evaluated Nuclear Data Library of Lawrence Livermore Laboratory (U.S.) was used as the source data. The actinide isotopes treated are the following 28: Th-232, U-233, U-234, U-235, U-236, U-237, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, Pu-243, Am-241, Am-242, Am-243, Cm-242, Cm-243, Cm-245, Cm-246, Cm-247, Cm-248, Bk-249, Cf-249, Cf-250, Cf-251, Cf-252 and a pseudo-fission product. ENDF/B-IV was used for U-238. The set was then collapsed to one energy group using a large LMFBR core spectrum for the comparison with other one-group sets. (author)

  5. 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

  6. Radiochemical studies of neutron deficient actinide isotopes

    International Nuclear Information System (INIS)

    The production of neutron deficient actinide isotopes in heavy ion reactions was studied using alpha, gamma, x-ray, and spontaneous fission detection systems. A new isotope of berkelium, 242Bk, was produced with a cross-section of approximately 10 μb in reactions of boron on uranium and nitrogen on thorium. It decays by electron capture with a half-life of 7.0 +- 1.3 minutes. The alpha-branching ratio for this isotope is less than 1% and the spontaneous fission ratio is less than 0.03%. Studies of (Heavy Ion, pxn) and (Heavy Ion, αxn) transfer reactions in comparison with (Heavy ion, xn) compound nucleus reactions revealed transfer reaction cross-sections equal to or greater than the compound nucleus yields. The data show that in some cases the yield of an isotope produced via a (H.I.,pxn) or (H.I.,αxn) reaction may be higher than its production via an xn compound nucleus reaction. These results have dire consequences for proponents of the ''Z1 + Z2 = Z/sub 1+2/'' philosophy. It is no longer acceptable to assume that (H.I.,pxn) and (H.I.,αxn) product yields are of no consequence when studying compound nucleus reactions. No evidence for spontaneous fission decay of 228Pu, 230Pu, 232Cm, or 238Cf was observed indicating that strictly empirical extrapolations of spontaneous fission half-life data is inadequate for predictions of half-lives for unknown neutron deficient actinide isotopes

  7. Radiochemical studies of neutron deficient actinide isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Williams, K.E.

    1978-04-01

    The production of neutron deficient actinide isotopes in heavy ion reactions was studied using alpha, gamma, x-ray, and spontaneous fission detection systems. A new isotope of berkelium, /sup 242/Bk, was produced with a cross-section of approximately 10 ..mu..b in reactions of boron on uranium and nitrogen on thorium. It decays by electron capture with a half-life of 7.0 +- 1.3 minutes. The alpha-branching ratio for this isotope is less than 1% and the spontaneous fission ratio is less than 0.03%. Studies of (Heavy Ion, pxn) and (Heavy Ion, ..cap alpha..xn) transfer reactions in comparison with (Heavy ion, xn) compound nucleus reactions revealed transfer reaction cross-sections equal to or greater than the compound nucleus yields. The data show that in some cases the yield of an isotope produced via a (H.I.,pxn) or (H.I.,..cap alpha..xn) reaction may be higher than its production via an xn compound nucleus reaction. These results have dire consequences for proponents of the ''Z/sub 1/ + Z/sub 2/ = Z/sub 1+2/'' philosophy. It is no longer acceptable to assume that (H.I.,pxn) and (H.I.,..cap alpha..xn) product yields are of no consequence when studying compound nucleus reactions. No evidence for spontaneous fission decay of /sup 228/Pu, /sup 230/Pu, /sup 232/Cm, or /sup 238/Cf was observed indicating that strictly empirical extrapolations of spontaneous fission half-life data is inadequate for predictions of half-lives for unknown neutron deficient actinide isotopes.

  8. 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...

  9. Actinide and fission product evolution benchmarking with Vandellos II (PWR-Spain) measured isotopic values with considering all the burn-up history with consecutive calculation

    International Nuclear Information System (INIS)

    At this study, isotopic evolution of the sample E58-263 of assembly WZR0058 of Vandellos Unit II (PWR-Spain) is calculated with MONTEBURNS code system. The sample was exposed with different neutron spectrum because of its different core location at fuel different cycles. At fuel calculation, all fuel cycle burn-up history of Use sample is 1 considered consecutively by using the 'remove' and 'add' option of the MONTEBURNS code. The calculated results are compared with fuel measurement and with cycle by cycle calculation methodology results.

  10. HTGR actinide burner feasibility studies: Calculation scheme related considerations

    International Nuclear Information System (INIS)

    At the CEA, the actinides burner version of the prismatic block-type reactor is currently investigated, including studies about the design proposed by General Atomics. The purpose of this paper is essentially to evaluate the capability of the deterministic methods to calculate a wide range of core configurations. In the first part of the paper, the analysis is carried out on the 'Deep Burner' fuel element geometry. The fuel element calculations are performed with both Transport code APOLLO2 and Monte-Carlo code TRIPOLI4. This preliminary analysis shows the reliability of the deterministic code APOLLO2 to calculate heterogeneous fuel element configurations (fuel element loaded with plutonium and minor actinides). In the second part, the analysis deals with the core geometry in order to estimate the impact of some physical assumptions on the fine fuel isotopic depletion. Due to the strong spectrum transient in the core, it turns out that the transuranic mass balances in a GT-MHR cannot be estimated easily from fuel element calculations but rather need the use of a core modeling approach taking into account the presence of the graphite reflectors. Two different methods based on a fine core Diffusion calculation in CRONOS2 and a simplified Transport calculation in APOLLO2 are investigated in this paper. (authors)

  11. Characterization of Tank 48H Samples for Alpha Activity and Actinide Isotopics

    International Nuclear Information System (INIS)

    This document reports the total alpha activity and actinide isotopic results for samples taken from Tank 48H prior to the addition of sodium tetraphenylborate and MST in Batch number-sign 1 of the ITP process. This information used to determine the quantity of MST for Batch number-sign 1 of the ITP process and the total actinide content in the tank for dose calculations

  12. 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

  13. Minor Actinide Transmutation Performance in Fast Reactor Metal Fuel. Isotope Ratio Change in Actinide Elements upon Low-Burnup Irradiation

    International Nuclear Information System (INIS)

    Metal fuel alloys containing 5 wt% or less minor actinide (MA) and rare earth (RE) were irradiated in the fast reactor Phénix. After nondestructive postirradiation tests, a chemical analysis of the alloys irradiated for 120 effective full power days was carried out by the inductively coupled plasma - mass spectrometry (ICP-MS) technique. From the analysis results, it was determined that the discharged burnups of U-19Pu-10Zr, U-19Pu-10Zr-2MA-2RE, and U-19Pu-10Zr-5MA were 2.17, 2.48, and 2.36 at.%, respectively. Actinide isotope ratio analyses before and after the irradiation experiment revealed that Pu, Am, and Cm nuclides added to U-Pu-Zr alloy and irradiated up to 2.0 - 2.5 at.% burnups in a fast reactor are transmuted properly as predicted by ORIGEN2 calculations. (author)

  14. 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%

  15. 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)

  16. 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.

  17. The contrasting fission potential-energy structure of actinides and mercury isotopes

    CERN Document Server

    Ichikawa, Takatoshi; Möller, Peter; Sierk, Arnold J

    2012-01-01

    Fission-fragment mass distributions are asymmetric in fission of typical actinide nuclei for nucleon number $A$ in the range $228 \\lnsim A \\lnsim 258$ and proton number $Z$ in the range $90\\lnsim Z \\lnsim 100$. For somewhat lighter systems it has been observed that fission mass distributions are usually symmetric. However, a recent experiment showed that fission of $^{180}$Hg following electron capture on $^{180}$Tl is asymmetric. An earlier experiment has shown fission of $^{198}$Hg and nearby nuclei is symmetric, but with hints of asymmetric yield distributions up to about 10 MeV above the saddle-point energy. We calculate potential-energy surfaces for a typical actinide nucleus and for 12 even isotopes in the range $^{178}$Hg--$^{200}$Hg, demonstrating the radical differences between actinide and mercury potential surfaces. We discuss these differences and how the changing potential-energy structure along the mercury isotope chain affects the observed (a)symmetry of the fission fragments. We show that the ...

  18. 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.

  19. MCNPX calculation of the reactivity worth of actinides OSMOSE samples

    International Nuclear Information System (INIS)

    Highlights: • Improvement the neutronic predictions through reactivity worth calculations. • MCNPx code with the nuclear data library ENDF/B-VII has been used for calculations. • The results show a good agreement within a relative error less than ±8.2%. - Abstract: Improving neutronic prediction is a very important step in designing advanced reactors and reactor fuel. There are three main critical reactor facilities of the CEA Cadarache. These reactor facilities are EOLE, MINERVE and MASURCA. The MINERVE reactor is used within the frame work of what is known as OSMOSE project. The OSMOSE program aims at improving neutronic predictions of advanced nuclear fuels through measurements in the MINERVE reactor on samples containing separated actinides. In the present work, the reactivity worth of OSMOSE samples have been calculated using the most recent Monte Carlo N Transport code MCNPX using the most recent nuclear cross-section data library ENDF/B-VII. The calculations are applied to the three core configurations R1-UO2, R2-UO2 and R1-MOX. The present work is performed to improve and/or measure the degree of validity of the previous obtained results of the REBUS and DRAGON codes. Also, our study is extended to include the experimental results for the sake of comparison. The comparison between the previously calculated values using DRAGON and the present results for the effective multiplication factor keff has a deviation less than ±0.3% for the three core configurations. Furthermore, the results of the reactivity worth of the present work show a good agreement with the experimental results within a relative error less than ±8.2%

  20. Theoretical studies of nuclear shapes for some lanthanide and actinide isotopes

    International Nuclear Information System (INIS)

    In the framework of geometric collective model (GCM) quantum phase transition between spherical and deformed shapes of doubly even nuclei are investigated. The model is formulated, it contains two kinetic energy terms and a potential given as a six term polynomial in two deformation parameters. The validity of the model is examined for the case of lanthanide chains Nd / Sm / Gd / Dy with neutron number N = 84 - 100 and actinide chains Th / U with neutron number N = 134 - 148. The parameters of the model were obtained by performing a computer simulated search program in order to obtain a minimum root mean square deviations between the calculated and the experimental excitation energies. Calculated potential energy surfaces (PES 's) describing all deformation effects of each nucleus are extracted. Our systematic studies on lanthanide and actinide chains have revealed a shape transition from spherical vibrator to axially deformed rotor when moving from the lighter to heavier isotopes.It is shown that the proposed model describes the collective structure effectively and illustratively, exhibiting the systematic nuclear shape changes. Collective properties are illustrated by the PES. The abnormal behavior of the two - neutron separation energies of our lanthanide nuclei as a function of neutron number around neutron number 90 is calculated. Nonlinear behavior is observed which indicate that shape phase transition is occurred in this region. The calculated reduced B(E2) transition probabilities of the low states of the ground state band in the nuclei 150Nd / 152Sm / 154Gd / 156Dy are analyzed and compared to the prediction of vibrational U(5) and rotational SU(3) limits of interacting boson model calculations.

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

    International Nuclear Information System (INIS)

    We are developing superconducting transition-edge sensor (TES) microcalorimeters that are optimized for rapid isotopic analysis of trace actinide samples by Q-spectroscopy. By designing mechanically robust TESs and simplified detector assembly methods, we have developed a detector for Q-spectroscopy of actinides that can be assembled in minutes. We have characterized the effects of each simplification and present the results. Finally, we show results of isotopic analysis of plutonium samples with Q-spectroscopy detectors and compare the results to mass spectrometry

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

    Science.gov (United States)

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

    2015-06-01

    We are developing superconducting transition-edge sensor (TES) microcalorimeters that are optimized for rapid isotopic analysis of trace actinide samples by Q-spectroscopy. By designing mechanically robust TESs and simplified detector assembly methods, we have developed a detector for Q-spectroscopy of actinides that can be assembled in minutes. We have characterized the effects of each simplification and present the results. Finally, we show results of isotopic analysis of plutonium samples with Q-spectroscopy detectors and compare the results to mass spectrometry.

  3. Simulation of fuel cycles with minor actinide management using a fast burnup calculation tool

    International Nuclear Information System (INIS)

    The paper presents a fast and flexible burnup model for fuel cycle simulations which is based on the description of the one-group cross-sections as analytic functions of the isotopic composition. This was accomplished by multi-dimensional regression based on the results of numerous core calculations. The developed model is able to determine the spent fuel composition in reasonable CPU time, and was integrated into a simplified fuel cycle model containing Gas Cooled Fast Reactors (GFR) and conventional light water reactors (LWRs). The fuel cycle simulations revealed an advantageous effect of increased minor actinide content in the GFR core on the fuel utilization parameters. In order to explore the processes that lay behind this effect the neutronics balance of the GFR was investigated in equilibrium cycle conditions. (author)

  4. The Dirac equation in electronic structure calculations: Accurate evaluation of DFT predictions for actinides

    Energy Technology Data Exchange (ETDEWEB)

    Wills, John M [Los Alamos National Laboratory; Mattsson, Ann E [Sandia National Laboratories

    2012-06-06

    Brooks, Johansson, and Skriver, using the LMTO-ASA method and considerable insight, were able to explain many of the ground state properties of the actinides. In the many years since this work was done, electronic structure calculations of increasing sophistication have been applied to actinide elements and compounds, attempting to quantify the applicability of DFT to actinides and actinide compounds and to try to incorporate other methodologies (i.e. DMFT) into DFT calculations. Through these calculations, the limits of both available density functionals and ad hoc methodologies are starting to become clear. However, it has also become clear that approximations used to incorporate relativity are not adequate to provide rigorous tests of the underlying equations of DFT, not to mention ad hoc additions. In this talk, we describe the result of full-potential LMTO calculations for the elemental actinides, comparing results obtained with a full Dirac basis with those obtained from scalar-relativistic bases, with and without variational spin-orbit. This comparison shows that the scalar relativistic treatment of actinides does not have sufficient accuracy to provide a rigorous test of theory and that variational spin-orbit introduces uncontrolled errors in the results of electronic structure calculations on actinide elements.

  5. The contrasting fission potential-energy structure of actinides and mercury isotopes

    OpenAIRE

    Ichikawa, Takatoshi; Iwamoto, Akira; Möller, Peter; Sierk, Arnold J.

    2012-01-01

    Fission-fragment mass distributions are asymmetric in fission of typical actinide nuclei for nucleon number $A$ in the range $228 \\lnsim A \\lnsim 258$ and proton number $Z$ in the range $90\\lnsim Z \\lnsim 100$. For somewhat lighter systems it has been observed that fission mass distributions are usually symmetric. However, a recent experiment showed that fission of $^{180}$Hg following electron capture on $^{180}$Tl is asymmetric. We calculate potential-energy surfaces for a typical actinide ...

  6. 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...

  7. Actinide isotopic analysis system for Los Alamos Plutonium-Handling Facility

    International Nuclear Information System (INIS)

    This paper reports that inventory measurement of a sample's total plutonium and other actinides content by non-destructive assay is an important component of safeguarding special nuclear material. Gamma-ray spectromety measurements of relative isotopic abundances, coupled with a calorimetry measurement, can determine sample SNM content for inventory measurement. The Actinide Isotopic Analysis System (AIAS) is a newly developed two-detector gamma-ray spectrometry-based system that will determine isotopic ratios of Pu and U, Np, and Am abundances relative to plutonium for the Nuclear Material Storage Facility at Los Alamos National Laboratory. spectral analysis is performed using Multiple Group analysis (MGA) program or a customized version of the Group Analysis (GRPANL) computer program. The system can measure samples containing reactor grade plutonium, weapons grade plutonium, and plutonium enriched in either 238Pu or 242Pu (>50%). Software that controls the system is driven by a user-friendly menu of options

  8. 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

  9. An easy method for the determination of Ra isotopes and actinide alpha emitters from the same water sample

    International Nuclear Information System (INIS)

    Radium isotopes and actinide α emitters are easily determined from the same water sample. The Ra fraction is obtained by coprecipitation with Ba, while a Fe coprecipitation is used for the actinides. Both fractions are measured with a gas-flow proportional counter. Additionally the isotopic Ra composition is obtained by measuring at two or three different times the α activity from the Ra-fraction. The method is applied to rain water and drinking water samples. (author)

  10. Calculations of the actinide transmutation with HELIOS for fuels of light water reactors

    International Nuclear Information System (INIS)

    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 keff 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% Δk/k, which was also among other participants. For the isotopic concentrations: 241Pu, 242 Pu and 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 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 and Innovative Fuel Cycles of the Nuclear

  11. Density functional theory calculations of the redox potentials of actinide(VI)/actinide(V) couple in water

    International Nuclear Information System (INIS)

    The measured redox potential of an actinide at an electrode surface involves the transfer of a single electron from the electrode surface on to the actinide center. Before electron transfer takes place, the complexing ligands and molecules of solvation need to become structurally arranged such that the electron transfer is at its most favorable. Following the electron transfer, there is further rearrangement to obtain the minimum energy structure for the reduced state. As such, there are three parts to the total energy cycle required to take the complex from its ground state oxidized form to its ground state reduced form. The first part of the energy comes from the structural rearrangement and solvation energies of the actinide species before the electron transfer or charge transfer process; the second part, the energy of the electron transfer; the third part, the energy required to reorganize the ligands and molecules of solvation around the reduced species. The time resolution of electrochemical techniques such as cyclic voltammetry is inadequate to determine to what extent bond and solvation rearrangement occurs before or after electron transfer; only for a couple to be classed as reversible is it fast in terms of the experimental time. Consequently, the partitioning of the energy theoretically is of importance to obtain good experimental agreement. Here we investigate the magnitude of the instantaneous charge transfer through calculating the fast one electron reduction energies of AnO2(H2O)n2+, where An = U, Np, and Pu, for n = 4-6, in solution without inclusion of the structural optimization energy of the reduced form. These calculations have been performed using a number of DFT functionals, including the recently developed functionals of Zhao and Truhlar. The results obtained for calculated electron affinities in the aqueous phase for the AnO2(H2O)52+/+ couples are within 0.04 V of accepted experimental redox potentials, nearly an order of magnitude

  12. 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.

  13. 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

  14. 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

  15. Actinides ultra traces detection and isotopic ratio measurements by mass spectrometry

    International Nuclear Information System (INIS)

    We present the mass spectrometry techniques used in the frame of the environmental monitoring of the centres of CEA, and non proliferation programmes, for the detection of ultra-traces of actinides (U and Pu), and for measurement of the corresponding isotopic ratios. They are plasma source (ICP-MS), thermo-ionization (TIMS), and secondary ions (SINS) mass spectrometry techniques. As the analyzed samples contain only tiny amounts of nuclear materials, from the femto-gram (10-15 g) to the pico-gram (10-12 g) range, these instruments must present excellent performances in terms of sensitivity and precision on isotopic ratio measurements. We describe the methodological and instrumental developments carried out on the spectrometers to obtain instrumental detection limits below the femto-gram. (authors)

  16. Fission cross section calculations for Pa isotopes

    International Nuclear Information System (INIS)

    Based on the recently measured cross-section values for the neutron-induced fission of 231Pa and our experience gained with other isotopes, new self consistent neutron cross section calculations for n+231Pa have been performed up to 30 MeV. The results are quite different to the existing evaluations, especially above the first chance fission threshold. (authors)

  17. 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)

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

    International Nuclear Information System (INIS)

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

  19. Calculational benchmark comparisons for a low sodium void worth actinide burner core design

    International Nuclear Information System (INIS)

    Recently, a number of low void worth core designs with non-conventional core geometries have been proposed. Since these designs lack a good experimental and computational data base, benchmark calculations are useful for the identification of possible biases in performance characteristics predictions. In this paper, a simplified benchmark model of a metal fueled, low void worth actinide burner design is detailed: and two independent neutronic performance evaluations are compared. Calculated performance characteristics are evaluated for three spatially uniform compositions (fresh uranium/plutonium, batch-averaged uranium/transuranic, and batch-averaged uranium/transuranic with fission products) and a regional depleted distribution obtained from a benchmark depletion calculation. For each core composition, the flooded and voided multiplication factor, power peaking factor, sodium void worth (and its components), flooded Doppler coefficient and control rod worth predictions are compared. In addition, the burnup swing, average discharge burnup, peak linear power, and fresh fuel enrichment are calculated for the depletion case. In general, remarkably good agreement is observed between the evaluations. The mot significant difference in predicted performance characteristics is a 0.3-05% Δk/(kk') bias in the sodium void worth. Significant differences in the transmutation rate of higher actinides are also observed; however, these differences do not cause discrepancies in the performance predictions

  20. Calculational benchmark comparisons for a low sodium void worth actinide burner core design

    International Nuclear Information System (INIS)

    Recently, a number of low void worth core designs with non-conventional core geometries have been proposed. Since these designs lack a good experimental and computational database, benchmark calculations are useful for the identification of possible biases in performance characteristics predictions. In this paper, a simplified benchmark model of a metal fueled, low void worth actinide burner design is detailed; and two independent neutronic performance evaluations are compared. Calculated performance characteristics are evaluated for three spatially uniform compositions (fresh uranium/plutonium, batch-averaged uranium/transuranic, and batch-averaged uranium/transuranic with fission products) and a regional depleted distribution obtained from a benchmark depletion calculation. For each core composition, the flooded and voided multiplication factor, power peaking factor, sodium void worth (and its components), flooded Doppler coefficient and control rod worth predictions are compared. In addition, the burnup swing, average discharge burnup, peak linear power, and fresh fuel enrichment are calculated for the depletion case. In general, remarkably good agreement is observed between the evaluations. The most significant difference is predicted performance characteristics is a 0.3--0.5% Δk/(kk) bias in the sodium void worth. Significant differences in the transmutation rate of higher actinides are also observed; however, these differences do not cause discrepancies in the performing predictions

  1. 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.)

  2. Ultra-low level (pg/L) actinide determinations and superior isotope ratio precisions by quadrupole ICP-MS

    International Nuclear Information System (INIS)

    A very high sensitivity, quadrupole-based inductively coupled plasma mass spectrometer (ICP-MS) has been developed and employed to measure very low concentrations (pg/L) of various actinides in solution. The detection capabilities of the instrument are shown using a variety of sample introduction methods, including simple direct sample nebulization, higher efficiency sample nebulization, and column preconcentration. This allowed three sigma detection limits in the range from 33 to 0.07 pg/L to be achieved, using short integration times, for a number of actinides. In addition, the improved sensitivity allowed isotope ratio measurements to be undertaken with good precision, (0.05 to 0.2%) at low concentrations (0.5 to 5 microg/L), without requiring long acquisition times. The results of isotope ratio measurements on silver, lead, and NIST natural lead standard SRM 981 will be reported

  3. 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.

  4. Relativistic calculations of isotope shifts in highly charged ions

    OpenAIRE

    Tupitsyn, I. I.; Shabaev, V. M.; Lopez-Urrutia, J. R. Crespo; Draganic, I.; Orts, R. Soria; Ullrich, J.

    2003-01-01

    The isotope shifts of forbidden transitions in Be- and B-like argon ions are calculated. It is shown that only using the relativistic recoil operator can provide a proper evaluation of the mass isotope shift, which strongly dominates over the field isotope shift for the ions under consideration. Comparing the isotope shifts calculated with the current experimental uncertainties indicates very good perspectives for a first test of the relativistic theory of the recoil effect in middle-Z ions.

  5. 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)

  6. 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.

  7. 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.

  8. Progress in theoretical calculation of transactinium isotope nuclear data

    International Nuclear Information System (INIS)

    Considerable progress has been made in effective use of nuclear theory for evaluation purposes. During the past few years, a number of basic improvements have developed in nuclear models commonly used for data evaluation. Actinide data evaluation can also use such improvements, but in the actinide region a further complication arises from the presence of fission competition. Nevertheless, systematic prescriptions for calculating even predicting neutron cross sections within an extended actinide region are available. Many efforts in several laboratorie are currently devoted to improving nuclear codes to be used for evaluation purposes. However at the present time numerous basic parameters associated with the neutron-induced fission process as well as neutron and gamma-ray competition have to be predetermined as input. Systematic studies of the behaviour of these parameters have been initiated with the aim of finding general trends hopefully useful for extrapolation in cases where direct information is lacking. Such trends can emerge from suitable examination of a large number of coherent experimental data, coherent theoretical results, or a combination these. This seems at the present time to be the most promising means for improving the actinide data evaluation. The aim of this paper is only to review briefly some of the main improvements either achieved or under way. The concern will be theoretical aspects useful for evaluating actinide data in the restricted incident neutron energy range from 10 KeV to 20 MeV. It is intended to focus on examples of systematics and on some improvements expected from microscopic methods under development

  9. 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

  10. Calculation of the isotope cluster for polypeptides by probability grouping.

    Science.gov (United States)

    Olson, Matthew T; Yergey, Alfred L

    2009-02-01

    This paper presents a novel theoretical basis for accurately calculating the isotope cluster of polypeptides. In contrast to previous approaches to this problem, which consider exhaustive or near exhaustive combinations of isotopic species, the program, Neutron Cluster, groups probabilities to yield highly accurate information without elucidating any fine structure within a nominal mass unit. This is a fundamental difference from any previously described algorithm for calculating the isotope cluster. As a result of this difference, the accurate isotope clusters for high molecular weight polypeptides can be calculated rapidly without any pruning. When applied to isotope enriched polypeptides, the algorithm introduces "grouping error", which is described, quantified, and avoided by using probability partitioning. PMID:19026561

  11. Actinide solubility in deep groundwaters - estimates for upper limits based on chemical equilibrium calculations

    International Nuclear Information System (INIS)

    A chemical equilibrium model is used to estimate maximum upper concentration limits for some actinides (Th, U, Np, Pu, Am) in groundwaters. Eh/pH diagrams for solubility isopleths, dominant dissolved species and limiting solids are constructed for fixed parameter sets including temperature, thermodynamic database, ionic strength and total concentrations of most important inorganic ligands (carbonate, fluoride, phosphate, sulphate, chloride). In order to assess conservative conditions, a reference water is defined with high ligand content and ionic strength, but without competing cations. In addition, actinide oxides and hydroxides are the only solid phases considered. Recommendations for 'safe' upper actinide solubility limits for deep groundwaters are derived from such diagrams, based on the predicted Eh/pH domain. The model results are validated as far as the scarce experimental data permit. (Auth.)

  12. Realistic shell-model calculations for Sn isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Covello, A. [Napoli Federico-2 Univ. (Italy). Dipt. di Scienze Fisiche]|[Istituto Nazionale di Fisica Nucleare, Padua (Italy); Andreozzi, F. [Napoli Federico-2 Univ. (Italy). Dipt. di Scienze Fisiche]|[Istituto Nazionale di Fisica Nucleare, Padua (Italy); Coraggio, L. [Napoli Federico-2 Univ. (Italy). Dipt. di Scienze Fisiche]|[Istituto Nazionale di Fisica Nucleare, Padua (Italy); Gargano, A. [Napoli Federico-2 Univ. (Italy). Dipt. di Scienze Fisiche]|[Istituto Nazionale di Fisica Nucleare, Padua (Italy); Porrino, A. [Napoli Federico-2 Univ. (Italy). Dipt. di Scienze Fisiche]|[Istituto Nazionale di Fisica Nucleare, Padua (Italy)

    1997-05-01

    We report on a shell-model study of the Sn isotopes in which a realistic effective interaction derived from the Paris free nucleon-nucleon potential is employed. The calculations are performed within the framework of the seniority scheme by making use of the chain-calculation method. This provides practically exact solutions while cutting down the amount of computational work required by a standard seniority-truncated calculation. The behavior of the energy of several low-lying states in the isotopes with A ranging from 122 to 130 is presented and compared with the experimental one. (orig.)

  13. 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.

  14. 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.

  15. OECD/NEA comparison calculations for an accelerator-driven minor actinide burner: analysis of preliminary results

    International Nuclear Information System (INIS)

    In the framework of the NEA Nuclear Science Committee, an international benchmark exercise for an accelerator-driven system is being undertaken. A model of a lead-bismuth cooled subcritical system driven by a beam of 1 GeV protons was chosen for the exercise. Except for the subassembly geometry, the design of the subcritical core is based on the ALMR reference design of a sodium-cooled actinide burner. To reduce the high pumping power for the lead-bismuth coolant, the reference subassembly was replaced by a subassembly with a smaller number of pins, and the fission power of the system was proportionally reduced. Lead-bismuth was chosen as target material to reflect the generally increased interest in this material for high-power spallation target applications. An interesting role of accelerator-driven systems is to burn actinide waste from reactors with conventional fuel cycles. The benchmark reactor is assumed to operate as a minor actinide burner in a 'double strata' fuel cycle scheme, featuring a fully closed fuel cycle with a top-up of pure minor actinides. Two fuel compositions for a start-up and an equilibrium core are considered, both differing considerably from normal U-Pu mixed oxide fuel compositions. Six organisations (ANL, CIEMAT, JAERI, KAERI, PSI/CEA and RIT) have contributed preliminary results for inclusion in this paper. The results are based on deterministic transport as well as Monte Carlo calculations using data from ENDF/B-VI, JENDL3.2 and JEF2.2. Significant difference in important neutronic parameters are observed. (authors)

  16. Burnup determination in irradiated fuel by means of isotopic analysis and comparison to CASMO calculations

    International Nuclear Information System (INIS)

    One of the traditional methods for determining the burnup of irradiated Light Water Reactor (LWR) fuel is the 148Nd method according to ASTM E-321. Probably one of the largest sources for systematic errors in this method is the assumed fission yield, requiring knowledge of the fraction of fissions occurring in different fissile nuclides. Another traditional method for burnup determination is based on the uranium and plutonium isotopic composition; however, this method is rarely used for LWR fuel due to its rather simplified and rough assumptions regarding the neutron spectrum and fission fractions. However, modern physics codes like CASMO and HELIOS are instead able to calculate the amount of fission products and actinides formed or consumed during reactor operation in a much more sophisticated way. Isotopic Dilution Analysis with chemical separation of elements of interest, followed by isotopic analysis with a Thermal Ionization Mass Spectrometer (TIMS) is a well established method for determining the content of selected isotopes in samples of dissolved irradiated fuel. This method normally provides very accurate and precise results. High Performance Liquid Chromatography (HPLC) for elemental separations, combined with Inductively Coupled Plasma Mass Spectrometry (ICP-MS) has become a much faster alternative. In general, this method is somewhat less precise. This disadvantage is at least partly compensated by the possibility of analyzing a larger number of nuclides and samples. The local pellet burnup of a well characterised fuel sample irradiated in the Swedish Boiling Water Reactor Forsmark 3 to about 60 MWd/kgU was determined. Weight ratios of neodymium isotopes relative to 238U, analysed by Isotope Dilution Analysis applying HPLC-ICP-MS as well as 235U and 239Pu abundance values were compared to corresponding values calculated by a single-assembly CASMO-4 simulation. Input data were generated by CASMO-4/POLCA7 core tracking calculations. The overall result

  17. 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.

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

    International Nuclear Information System (INIS)

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

  19. Actinide content and associated neutron emission of WWER-440 spent fuel - calculation and validation for safeguards purposes

    International Nuclear Information System (INIS)

    A major task of international nuclear material safeguards consists in the experimental determination of the characteristics of spent nuclear fuel. In this respect, passive neutron techniques take a prominent place. The paper describes both the actinide content and the passive neutron emission of spent WWER-440 fuel for a number of operational conditions. For validation purposes the results have been compared with those independently gained by other authors for the same type of fuel. The calculations are the basis for a true to fact interpretation of the primary measurement signal, i.e. for the inference from recorded neutron radiation regarding the properties of the spent nuclear fuel. (author)

  20. 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

  1. 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

  2. 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)

  3. Decay calculations on medium-level and actinide-containing wastes from the LWR fuel cycle. Pt. 1

    International Nuclear Information System (INIS)

    A number of basic data on medium-level and actinide-containing waste streams from the LWR fuel cycle were evaluated and the activity and thermal decay power were calculated for the nuclide inventories of cladding hulls and fuel assembly structural materials, for feed clarification sludge, medium-level aqueous process waste, low-level solid transuranium waste and for medium-level reactor operating waste. The activity as a function of decay time of the medium-level wastes decreases within 500 to 600 years by 1 to 3 orders of magnitude and is at the same time about 1 to 2 orders of magnitude lower than the activity of the high-level waste. The thermal decay power of the medium-level wastes decreases after 10 to 100 years by about 3 orders of magnitude and is about a factor of 10 to 100 less than that of high-level waste. In the very long term the residual activity (and thermal power) decreases only slowly due to the long halflives of the dominant actinides. The activity after more that 1000 years is about 1 to 2 orders of magnitude lower than that of high-level waste, the low-level transuranium waste by a factor 10 to 4, respectively. The activity per unit volume of the packaged waste of the medium-level and actinide-containing wastes because of the bigger volume of the conditioned wastes is lower by 2 to 4 orders of magnitude up to about 500 years. After more than 1000 years the activities per unit volume are lower by a factor of 20 to 200 than that of high-level waste. (orig.)

  4. OECD/NEA Benchmark Calculations for an Accelerator-Driven Minor Actinide Burner

    International Nuclear Information System (INIS)

    Noticing the current interest in accelerator-driven systems as actinide waste burners, the OECD/NEA has organised an international benchmark exercise for evaluating the performance of computational tools and nuclear data for this type of system. The benchmark model simulates a lead-bismuth cooled sub-critical system driven by a beam of 1 GeV protons. The core design is similar to that of an ALMR, and the fuel composition is typical for a minor actinide burner in a 'double strata' fuel cycle. Lead-bismuth was chosen as target material. Since the intention was to validate data and codes in the energy region below 20 MeV, a predefined spallation neutron source was provided to the benchmark participants. The solutions from seven organisations (ANL, CIEMAT, KAERI, JAERI, PSI/CEA, RIT and SCK-CEN) are based on three different basic data libraries (ENDF/B-VI, JEF-2.2 and JENDL-3.2) and both deterministic and Monte Carlo reactor codes. Significant discrepancies are observed for important neutronic parameters such as initial keff, burn-up reactivity swing and flux distribution. Additional investigations of the basic nuclear data, the data processing methods and the approximations for the reactor simulation will be necessary to understand the origin of all observed discrepancies. (authors)

  5. Development of Todga extraction process for high-level liquid waste preliminary evaluation of actinide separation by calculation

    International Nuclear Information System (INIS)

    Extraction process for actinide separation from HLLW with N,N,N',N'-tetra-octyl-3-oxa-pentane-diamide (TODGA) was preliminarily evaluated by calculation of Am and Sr behaviors. Results of the calculation showed that it is possible to establish an extraction process with 0.1 M or 0.2 M TODGA in n-dodecane, where Am is extracted in a very high yield of more than 99.99% and Sr is kept in the aqueous phase in a yield of more than 99.95%. The solution volume required for the treatment of an unit amount of HLLW was also evaluated using data on extraction capacity as the first step for the estimation of the process scale. (author)

  6. 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

  7. 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

  8. Accelerating quantum instanton calculations of the kinetic isotope effects

    International Nuclear Information System (INIS)

    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

  9. ACTRAN: a code for depletion calculations in PWR cores aiming the production of minor actinide for using in ADS

    International Nuclear Information System (INIS)

    Despite of the renewed willing to accept nuclear power as a mean of mitigate the climate changing, to deal with the long lived waste still cause some concerning in relation to maintain in safety condition, during so many years. A technological solution to overcome this leg of time is to use a facility that burn these waste, besides to generate electricity. This is the idea built in the accelerator driven systems (ADS). This technology is being though to use some minor actinides (MAs) as fuel. This work presents a program to assess actinide concentrations, aiming a fertile-free fuel to be used in the future ADS technology. For that, use was made of a numerical code to solve the steady-state multigroup diffusion equation 3D to calculate the neutron fluxes, coupled it with a new code to solve, also numerically, depletion equations, named ACTRAN code. This paper shows the simulation of a PWR core during the residence time of the nuclear fuel, for three years, and after, for almost four hundred years, to assess the MAs production. The results show some insight in the best management to get a minimum amount of some MAs to use in the future generations of ADS. (author)

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

    International Nuclear Information System (INIS)

    A ThermoFisher 'Triton' multi-collector thermal ionization mass spectrometer (MC-TIMS) was evaluated for trace and ultra-trace level isotoperatioanalysis of actinides (uranium, plutonium, and americium), fission products and geolocators (strontium, cesium, and neodymium). Total efficiencies (atoms loaded to ions detected) of up to 0.5-2% for U, Pu, and Am, and 1-30% for Sr, Cs, and Nd can be reported employing resin bead load techniques onto flat ribbon Re filaments or resin beads loaded into a millimeter-sized cavity drilled into a Re rod. This results in detection limits of 4 atoms to 105 atoms) for 239-242+244Pu, 233+236U, 241-243Am, 89,90Sr, and 134,135,137Cs, and (le) 1 pg for natural Nd isotopes (limited by the chemical processing blank) using a secondary electron multiplier (SEM) or multiple-ion counters (MICs). Relative standard deviations (RSD) as small as 0.1% and abundance sensitivities of 1 x 106 or better using a SEM are reported here. Precisions of RSD ∼ 0.01-0.001% using a multi-collector Faraday cup array can be achieved at sub-nanogram concentrations for strontium and neodymium and are suitable to gain crucial geolocation information. The analytical protocols reported herein are of particular value for nuclear forensic and nuclear safeguard applications.

  11. 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.)

  12. Methods For The Calculation Of Pebble Bed High Temperature Reactors With High Burnup Plutonium And Minor Actinide Based Fuel

    International Nuclear Information System (INIS)

    The graphite moderated Modular High Temperature Pebble Bed Reactor enables very flexible loading strategies and is one candidate of the Generation IV reactors. For this reactor fuel cycles with high burnup (about 600 MWd/kg HM) based on plutonium (Pu) and minor actinides (MA) fuel will be investigated. The composition of this fuel is defined in the EU-PuMA-project which aims the reduction of high level waste. There exist nearly no neutronic full core calculations for this fuel composition with high burnup. Two methods (deterministic and Monte Carlo) will be used to determine the neutronics in a full core. The detailed results will be compared with respect to the influence on criticality and safety related parameters. (authors)

  13. 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.

  14. Reactivity effect breakdown calculations with deterministic and stochastic perturbations analysis – JEFF-3.1.1 to JEFF3.2T1 (BRC-2009) actinides application

    OpenAIRE

    Morillon B; Peneliau Y.

    2013-01-01

    JEFF-3.1.1 is the reference nuclear data library in CEA for the design calculations of the next nuclear power plants. The validation of the new neutronics code systems is based on this library and changes in nuclear data should be looked at closely. Some new actinides evaluation files at high energies have been proposed by CEA/Bruyères-le-Chatel in 2009 and have been integrated in JEFF3.2T1 test release. For the new release JEFF-3.2, CEA will build new evaluation files for the actinides, whic...

  15. Realistic shell-model calculations for neutron deficient Sn isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Andreozzi, F.; Coraggio, L.; Covello, A.; Gargano, A.; Kuo, T.T.; Li, Z.B.; Porrino, A. [Dipartimento di Scienze Fisiche, Universita di Napoli Federico II]|[Istituto Nazionale di Fisica Nucleare, Mostra d`Oltremare, Pad. 20, 80125 Napoli (Italy)]|[Department of Physics, SUNY, Stony Brook, New York 11794 (United States)

    1996-10-01

    We have performed shell-model calculations for {sup 102,103,104,105}Sn using two realistic effective interactions derived from the Bonn A and Paris nucleon-nucleon potentials, respectively. From the comparison of the calculated spectra of {sup 104}Sn and {sup 105}Sn with the experimental ones it turns out that the best agreement is obtained with the weaker tensor force potential (Bonn A). This agreement appears to be significantly better than for other nuclear regions, such as the {ital sd} shell, and thus encourages use of modern realistic potentials in shell-model calculations for medium- and heavy-mass nuclei. In addition, it supports confidence in our predictions of the spectra of the hitherto unknown isotopes {sup 102}Sn and {sup 103}Sn. {copyright} {ital 1996 The American Physical Society.}

  16. Realistic shell-model calculations for neutron deficient Sn isotopes

    International Nuclear Information System (INIS)

    We have performed shell-model calculations for 102,103,104,105Sn using two realistic effective interactions derived from the Bonn A and Paris nucleon-nucleon potentials, respectively. From the comparison of the calculated spectra of 104Sn and 105Sn with the experimental ones it turns out that the best agreement is obtained with the weaker tensor force potential (Bonn A). This agreement appears to be significantly better than for other nuclear regions, such as the sd shell, and thus encourages use of modern realistic potentials in shell-model calculations for medium- and heavy-mass nuclei. In addition, it supports confidence in our predictions of the spectra of the hitherto unknown isotopes 102Sn and 103Sn. copyright 1996 The American Physical Society

  17. 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.

  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. 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

  20. Development of windows based application for the calculation of atomic hyperfine spectrum of odd isotopes

    International Nuclear Information System (INIS)

    Windows based application has been developed for the calculation of atomic hyperfine spectrum of odd isotopes keeping in view of the needs of the atomic spectroscopists. The application can also calculate the hyperfine spectrum of another odd isotope if hyperfine structure constants of one isotope are known. Various features of the developed application are discussed. (author)

  1. Calculation characterization of spent fuel hazard related to partitioning and transmutation of minor actinides and fission products

    International Nuclear Information System (INIS)

    Radiotoxicity is one of important characteristics of radwaste hazard. Radiotoxicity of actinides and fission products from spent fuel of VVER-1000 reactor for processes of burnup, long-term storage, and transmutation is discussed. (author)

  2. Measured and calculated isotopes for a gadolinia lead test assembly

    International Nuclear Information System (INIS)

    The US Department of Energy, Duke Power Company, and the B and W Fuel Company participated in an extended burnup project to develop, irradiate, and examine an advanced fuel assembly design for pressurized water reactors. The assembly uses a urania-gadolinia (UO2-Gd2O3) burnable absorber fuel mixture along with other fuel performance and design features that enhance uranium utilization. Previous milestones in the gadolinia development of the extended burnup project include development and verification of a neutronics model, measurement of materials properties of gadolinia fuel, and a successful gadolinia lead test assembly (LTA) program. One LTA was discharged as planned after one cycle, four LTAs continued for two more cycles, and one LTA of these four underwent a fourth cycle and reached 58,310 MWd/ton U assembly-average burnup, a world record at the time. Hot-cell destructive examination of gadolinia and non-gadolinia fuel rods from the single-cycle LTA (406.2 effective full-power days irradiation) has been completed. The comparison of measured and calculated isotopics for this LTA is the subject of this paper. A comparison of measured and calculated power distributions is also given, because accurate prediction of core performance during power production is ultimately the most important test of a calculational model

  3. Decay calculations on medium-level and actinide-containing wastes from the LWR fuel cycle. Pt. 2

    International Nuclear Information System (INIS)

    1. The radiotoxicity index as inherent property of the radionuclide inventory was calculated for medium-level and actinide-containing wastes. The calculations were based on the annual limits of intake of the German Radiation Protection Ordinance as well as the new values of annual limits of intake from ICRP-30. The latter imply a higher rating of the toxicity of transuranium nuclides and a lower rating of Sr-90, Tc-99, and Ra-226. Thus, the annual radiotoxicity index is controlled by the transuranics after 10 to 100 years. 2. From the comparison of the radiotoxicity index of conditional and packed wastes with the same volume of uranium ore, it was evaluated that the relative radiotoxicity of the medium-level wastes decreases below the level of pitchblende after less than 100 years and below a 3% uranium ore after less than 2000 of decay. However, based on ICRP-30, the relative radiotoxicity index decreases below the level of pitchblende after 1000 years and decays to the level of the 3% uranium ore at about 105 years. 3. The comparison of the radiotoxicity concentration of the total disposal layer with a uranium ore deposit shows that the radiotoxicity concentration based on ICRP-30 of the self-heating wastes placed in single boreholes decays within 2000 years (high level waste within 3000 years) below the level of a uranium ore deposit of 0.2% uranium. The radiotoxicity concentration of the medium-level process waste and the alpha-waste disposed off in disposal chambers decreases to the level of a uranium ore deposit with 0.4 to 6% uranium after about 104 years, and 1% after about 105 years. (orig./HP)

  4. 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.)

  5. 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)

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

    Energy Technology Data Exchange (ETDEWEB)

    Stanbro, W.D. [comp.

    1997-03-01

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

  7. 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...

  8. Managing Inventories of Heavy Actinides

    International Nuclear Information System (INIS)

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

  9. 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

  10. 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.

  11. 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.

  12. 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

  13. 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.

  14. 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

  15. 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.

  16. 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

  17. Calculations of neutron and proton radii of cesium isotopes. Final report, April 23--September 30, 1993

    International Nuclear Information System (INIS)

    This task involved the calculation of neutron and proton radii of cesium isotopes. The author has written a computer code that calculates radii according to two models: Myers 1983 and FRDM 1992. Results of calculations in both these models for both cesium and francium isotopes are attached as figures. He is currently interpreting these results in collaboration with D. Vieira and J.R. Nix, and they expect to use the computer code for further studies of nuclear radii

  18. 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;

  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. Thermal-hydraulics of actinide burner reactors

    International Nuclear Information System (INIS)

    As a part of conceptual study of actinide burner reactors, core thermal-hydraulic analyses were conducted for two types of reactor concepts, namely (1) sodium-cooled actinide alloy fuel reactor, and (2) helium-cooled particle-bed reactor, to examine the feasibility of high power-density cores for efficient transmutation of actinides within the maximum allowable temperature limits of fuel and cladding. In addition, calculations were made on cooling of actinide fuel assembly. (author)

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

    International Nuclear Information System (INIS)

    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).

  2. 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).

  3. 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

  4. 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.)

  5. Dual-isotope separation technique for radioassay. Precision of calculated results affected by degree of separation

    International Nuclear Information System (INIS)

    The dual-isotope separation technique for radioassay is reviewed. An expression is derived describing the effect of counting errors on the precision of the calculated bound count rate in the dual-isotope technique. This mathematic model is tested in experiments using sodium iothalamate (I-125) as a marker in the Phadebas radiosorbent assay of cobalamin (Co-57). The coefficient of variation of results calculated on the basis of the dual-isotope technique is shown to be dependent on the amount of supernatant removed. The conclusion is that relatively large amounts of supernatant must be removed before counting if the dual-isotope technique is to give acceptable results. The experimental model is proposed as a simple test of the suitability of a projected dual-isotope system. (Auth.)

  6. 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)

  7. Reactivity effect breakdown calculations with deterministic and stochastic perturbations analysis - JEFF-3.1.1 to JEFF3.2T1 (BRC-2009) actinides application

    International Nuclear Information System (INIS)

    JEFF-3.1.1 is the reference nuclear data library in CEA for the design calculations of the next nuclear power plants. The validation of the new neutronics code systems is based on this library and changes in nuclear data should be looked at closely. Some new actinides evaluation files at high energies have been proposed by CEA/Bruyeres-le-Chatel in 2009 and have been integrated in JEFF3.2T1 test release. For the new release JEFF-3.2, CEA will build new evaluation files for the actinides, which should be a combination of the new evaluated data coming from BRC-2009 in the high energy range and improvements or new evaluations in the resolved and unresolved resonance range from CEA-Cadarache. To prepare the building of these new files, benchmarking the BRC-2009 library in comparison with the JEFF-3.1.1 library was very important. The crucial points to evaluate were the improvements in the continuum range and the discrepancies in the resonance range. The present work presents for a selected set of benchmarks the discrepancies in the effective multiplication factor obtained while using the JEFF-3.1.1 or JEFF-3.2T1 library with the deterministic code package ERANOS/PARIS and the stochastic code TRIPOLI- 4. They have both been used to calculate cross section perturbations or other nuclear data perturbations when possible. This has permitted to identify the origin of the discrepancies in reactivity calculations. In addition, this work also shows the importance of cross section processing validation. Actually, some fast neutron spectrum calculations have led to opposite tendencies between the deterministic code package and the stochastic code. Some particular nuclear data (MT=5 in ENDF terminology) seem to be incompatible with the current MERGE or GECCO processing codes. (authors)

  8. Reactivity effect breakdown calculations with deterministic and stochastic perturbations analysis – JEFF-3.1.1 to JEFF3.2T1 (BRC-2009 actinides application

    Directory of Open Access Journals (Sweden)

    Morillon B.

    2013-03-01

    Full Text Available JEFF-3.1.1 is the reference nuclear data library in CEA for the design calculations of the next nuclear power plants. The validation of the new neutronics code systems is based on this library and changes in nuclear data should be looked at closely. Some new actinides evaluation files at high energies have been proposed by CEA/Bruyères-le-Chatel in 2009 and have been integrated in JEFF3.2T1 test release. For the new release JEFF-3.2, CEA will build new evaluation files for the actinides, which should be a combination of the new evaluated data coming from BRC-2009 in the high energy range and improvements or new evaluations in the resolved and unresolved resonance range from CEA-Cadarache. To prepare the building of these new files, benchmarking the BRC-2009 library in comparison with the JEFF-3.1.1 library was very important. The crucial points to evaluate were the improvements in the continuum range and the discrepancies in the resonance range. The present work presents for a selected set of benchmarks the discrepancies in the effective multiplication factor obtained while using the JEFF-3.1.1 or JEFF-3.2T1 library with the deterministic code package ERANOS/PARIS and the stochastic code TRIPOLI-4. They have both been used to calculate cross section perturbations or other nuclear data perturbations when possible. This has permittted to identify the origin of the discrepancies in reactivity calculations. In addition, this work also shows the importance of cross section processing validation. Actually, some fast neutron spectrum calculations have led to opposite tendancies between the deterministic code package and the stochastic code. Some particular nuclear data (MT=5 in ENDF terminology seem to be incompatible with the current MERGE or GECCO processing codes.

  9. Reactivity effect breakdown calculations with deterministic and stochastic perturbations analysis - JEFF-3.1.1 to JEFF3.2T1 (BRC-2009) actinides application

    Science.gov (United States)

    Peneliau, Y.; Morillon, B.

    2013-03-01

    JEFF-3.1.1 is the reference nuclear data library in CEA for the design calculations of the next nuclear power plants. The validation of the new neutronics code systems is based on this library and changes in nuclear data should be looked at closely. Some new actinides evaluation files at high energies have been proposed by CEA/Bruyères-le-Chatel in 2009 and have been integrated in JEFF3.2T1 test release. For the new release JEFF-3.2, CEA will build new evaluation files for the actinides, which should be a combination of the new evaluated data coming from BRC-2009 in the high energy range and improvements or new evaluations in the resolved and unresolved resonance range from CEA-Cadarache. To prepare the building of these new files, benchmarking the BRC-2009 library in comparison with the JEFF-3.1.1 library was very important. The crucial points to evaluate were the improvements in the continuum range and the discrepancies in the resonance range. The present work presents for a selected set of benchmarks the discrepancies in the effective multiplication factor obtained while using the JEFF-3.1.1 or JEFF-3.2T1 library with the deterministic code package ERANOS/PARIS and the stochastic code TRIPOLI-4. They have both been used to calculate cross section perturbations or other nuclear data perturbations when possible. This has permittted to identify the origin of the discrepancies in reactivity calculations. In addition, this work also shows the importance of cross section processing validation. Actually, some fast neutron spectrum calculations have led to opposite tendancies between the deterministic code package and the stochastic code. Some particular nuclear data (MT=5 in ENDF terminology) seem to be incompatible with the current MERGE or GECCO processing codes.

  10. 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

  11. 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

  12. Radiochemical measurements of the formation cross sections of actinide isotopes in the reaction of 238U ions with 238U

    International Nuclear Information System (INIS)

    The method of high-pressure liquid chromatography was used to separate metal cations and anions. Thereby the influence of different parameters on the separation of lanthanides by cation exchange and extraction chromatography was systematically investigated. The results were used to optimize that separation cycle, in which the elements from Z = 26 to Z = 101 were separated taking into account especially the group of actinides. These separations and the subsequent spectroscopy of gamma radiation, alpha particles and spontaneous fission fragments were used to determine formation cross sections in heavy ion reactions as a function of the atomic charge and the mass number. The most important point was the investigation of the collision of 238U ions at different bombarding energies. On the basis of the measured formation cross sections conclusions can be drawn on the reaction mechanism and the excitation function of the formation of transplutonium elements. According to the results it seems to be reasonable to use transfer reactions between 238U and 238U or 248Cm to synthesize superheavy nuclei around Z = 114. Until now that has been tried only with the help of fusion reactions and the results were negative. (orig.)

  13. 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

  14. 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. PMID:26949835

  15. 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).

  16. Photochemistry of the actinides

    International Nuclear Information System (INIS)

    It has been found that all three major actinides have a useful variety of photochemical reactions which could be used to achieve a separations process that requires fewer reagents. Several features merit enumerating: (1) Laser photochemistry is not now as uniquely important in fuel reprocessing as it is in isotopic enrichment. The photochemistry can be successfully accomplished with conventional light sources. (2) The easiest place to apply photo-reprocessing is on the three actinides U, Pu, and Np. The solutions are potentially cleaner and more amenable to photoreactions. (3) Organic-phase photoreactions are probably not worth much attention because of the troublesome solvent redox chemistry associated with the photochemical reaction. (4) Upstream process treatment on the raffinate (dissolver solution) may never be too attractive since the radiation intensity precludes the usage of many optical materials and the nature of the solution is such that light transmission into it might be totally impossible

  17. 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.

  18. Heavy coolant fast neutron reactor BRUS-150 for minor actinides burning and U-233 build-up

    International Nuclear Information System (INIS)

    The present paper deals with the calculational research into the performance of fast reactor BRUS-150 cooled with liquid metal coolant eutectic lead-bismuth alloy with reference to minor actinides (Np, Am, Cm) transmutation and isotopic pure U 233 build up. (authors). 10 refs., 2 figs

  19. Efigie: a computer program for calculating end-isotope accumulation by neutron irradiation and radioactive decay

    International Nuclear Information System (INIS)

    Efigie is a program written in Fortran V which can calculate the concentration of radionuclides produced by neutron irradiation of a target made of either a single isotope or several isotopes. The program includes optimization criteria that can be applied when the goal is the production of a single nuclide. The effect of a cooling time before chemical processing of the target is also accounted for.(author)

  20. Comparison of statistical model calculations for stable isotope neutron capture

    Science.gov (United States)

    Beard, M.; Uberseder, E.; Crowter, R.; Wiescher, M.

    2014-09-01

    It is a well-observed result that different nuclear input models sensitively affect Hauser-Feshbach (HF) cross-section calculations. Less well-known, however, are the effects on calculations originating from nonmodel aspects, such as experimental data truncation and transmission function energy binning, as well as code-dependent aspects, such as the definition of level-density matching energy and the inclusion of shell correction terms in the level-density parameter. To investigate these aspects, Maxwellian-averaged neutron capture cross sections (MACS) at 30 keV have been calculated using the well-established statistical Hauser-Feshbach model codes talys and non-smoker for approximately 340 nuclei. For the same nuclei, MACS predictions have also been obtained using two new HF codes, cigar and sapphire. Details of these two codes, which have been developed to contain an overlapping set of identically implemented nuclear physics input models, are presented. It is generally accepted that HF calculations are valid to within a factor of 3. It was found that this factor is dependent on both model and nonmodel details, such as the coarseness of the transmission function energy binning and data truncation, as well as variances in details regarding the implementation of level-density parameter, backshift, matching energy, and giant dipole strength function parameters.

  1. Anthropogenic Actinides in the Environment

    International Nuclear Information System (INIS)

    The use of nuclear energy and the testing of nuclear weapons have led to significant releases of anthropogenic isotopes, in particular a number of actinide isotopes generally not abundant in nature. Most prominent amongst these are 239Pu, 240Pu, and 236U. The study of these actinides in nature has been an active field of study ever since. Measurements of actinides are applied to nuclear safeguards, investigating the sources of contamination, and as a tracer for a number of erosion and hydrology studies. Accelerator Mass Spectrometry (AMS) is ideally suited for these studies and generally offers higher sensitivities than competing techniques, like ICP-MS or decay counting. Recent advances in AMS allow the study of “minor” plutonium isotopes (241Pu, 242Pu, and 244Pu). Furthermore, 236U can now be measured at the levels expected from the global stratospheric fall-out of the atmospheric nuclear weapon tests in the 1950s and 1960s. Even the pre-anthropogenic isotope ratios could be within reach. However, the distribution and abundance levels of these isotopes are not well known yet. I will present an overview of the field, and in detail two recent studies on minor plutonium isotopes and 236U, respectively.(author)

  2. 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.

  3. Calculation of isotopic profile during band displacement on ion exchange resins

    International Nuclear Information System (INIS)

    A method has been developed to calculate the isotopic profile during band displacement on ion exchange resins using computer simulation. Persoz had utilized this technique earlier for calculating the isotopic profile during band displacement as well as frontal analysis. The present report deals with a simplification of the method used by Persoz by reducing the number of variables and making certain approximations where the separation factor is not far from unity. Calculations were made for the typical case of boron isotope separation. The results obtained by the modified method were found to be in very good agreement with those obtained by using an exact equation, at the same time requiring conside--rably less computer time. (author)

  4. Actinide recycle

    International Nuclear Information System (INIS)

    A multitude of studies and assessments of actinide partitioning and transmutation were carried out in the late 1970s and early 1980s. Probably the most comprehensive of these was a study coordinated by Oak Ridge National Laboratory. The conclusions of this study were that only rather weak economic and safety incentives existed for partitioning and transmuting the actinides for waste management purposes, due to the facts that (1) partitioning processes were complicated and expensive, and (2) the geologic repository was assumed to contain actinides for hundreds of thousands of years. Much has changed in the few years since then. A variety of developments now combine to warrant a renewed assessment of the actinide recycle. First of all, it has become increasingly difficult to provide to all parties the necessary assurance that the repository will contain essentially all radioactive materials until they have decayed. Assurance can almost certainly be provided to regulatory agencies by sound technical arguments, but it is difficult to convince the general public that the behavior of wastes stored in the ground can be modeled and predicted for even a few thousand years. From this point of view alone there would seem to be a clear benefit in reducing the long-term toxicity of the high-level wastes placed in the repository

  5. Exploratory coupled channels calculations for loosely bound carbon isotopes

    International Nuclear Information System (INIS)

    The loosely bound halo candidates 17C and 19C have been investigated in a neutron+core coupling model. A deformed Woods-Saxon potential is used for the neutron-core interaction and the coupled channels equations are solved with Sturmian expansions of the relative motion wave functions for experimental one-neutron separation energies. The r.m.s. matter radii, longitudinal momentum distributions, E1 strength functions, neutron stripping cross sections and electromagnetic dissociation cross sections are calculated. (K.A.)

  6. PHAST, Calculation of isotope equilibrium constants for geochemical models

    International Nuclear Information System (INIS)

    1 - Description of program or function: The geochemical part of the program has the capability to perform a wide range of chemical reaction calculations that include aqueous complexation, mineral equilibria, surface complexation, ion exchange, solid-solution equilibria, gas-phase equilibration, and general kinetic reactions. In addition, geochemical simulations, which include all of these types of reaction calculations plus mixing, irreversible reactions, and temperature variation, may be used to define initial and chemical boundary conditions for the reaction-transport simulations. Essentially, any modeling capability available in PHREEQC may be used to establish initial and boundary conditions for the reactive-transport simulation of PHAST. All spatially distributed properties are defined by zones that are rectangular prisms. Zones may overlap, in which case the order of definition is important because the last specification of a property for a cell or element will be the one used in the simulation. The units for input of properties may be a mixture of English and SI metric, however, all output data are SI metric with a user-selected time unit. The transport part of PHAST is written in Fortran 90 and the geochemical part is written in C. Both parts dynamically allocate any computer memory necessary for program execution. Little effort has been expended to minimize storage requirements. Consequently, depending on the size of the domain, the program may require relatively large amounts of memory for execution. In the application of PHAST, it is advisable to progress from simple to increasingly complicated simulations. First, the geochemical model PHREEQC should be used to evaluate chemical reactions by the use of reaction-path and then 1D-transport calculations. Second, PHAST should be used in flow-only mode to obtain an acceptable model of the flow system. Finally, PHAST should be used for reaction-transport calculations that combine the flow simulation with

  7. A full calculation of Zr and Sn isotopes in the Relativistic Mean Field theory

    CERN Document Server

    Geng, L S; Meng, J

    2003-01-01

    The ground-state properties of Zr and Sn isotopes are studied within the relativistic mean field theory. Zr and Sn isotopes have received tremendous attentions due to various reasons, including the predicted giant halos in neutron-rich Zr isotopes, the unique feature of being robust spherical in the region of $^{100}$Sn $\\sim$ $^{132}$Sn and the particular interest of Sn isotopes to nuclear astrophysics. Furthermore, four magic numbers, 40, 50, 82 and 126, make these two isotopes particularly important to test a microscopic model. In the present work, we carry out a full calculation of Zr and Sn isotopes from the proton drip line to the neutron drip line with deformation, pairing correlations and blocking effect for even-odd nuclei included. A quadrupole constrained calculation is performed to find the absolute minimum for each nucleus. All ground-state properties, including separation energies, odd-even staggering (OES), nuclear radii, deformations and single-particle spectra are analyzed and discussed in de...

  8. 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.

  9. 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.

  10. 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)

  11. 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 highly sensitive and advanced laser-based 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 applied for the chemical speciation of actinide in aqueous solutions and the quantitative analysis of actinide isotopes in spent nuclear fuels. In this report, results on the following subjects have been summarized. Development of TRLFS technology for the chemical speciation of actinides, Development of laser-induced photo-acoustic spectroscopy (LPAS) system, Application of LIBD technology to investigate dynamic behaviors of actinides dissolution reactions, Development of nanoparticle analysis technology in groundwater using LIBD, Chemical speciation of plutonium complexes by using a LWCC system, Development of LIBS technology for the quantitative analysis of actinides, Evaluation on the chemical reactions between actinides and humic substances, Spectroscopic speciation of uranium-ligand complexes in aqueous solution, Chemical speciation of actinides adsorbed on metal oxides surfaces

  12. 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.

  13. Calculation of reduced partition function ratios of isotopically substituted molecules on a quantum chemical base

    International Nuclear Information System (INIS)

    By means of the semiempirical quantum chemical MINDO/3- and MNDO-MO-methods it is possible to perform calculations for use in evaluation or interpretation of isotope effects to such an extent that would not be rationally fossible by corresponding experiments. But only the calculated reduced partition function ratios of isotopically substituted molecules can be applied with sufficient reliability for discussions. The temperature dependence of the reduced partition function ratios of over 100 molecules, ions, and radicals regarding the H/D, 12C/13C-, 14N/15N-, 16O/18O-, 28Si/30Si-, 32S/34S-, and 35Cl/37Cl-substitution has been calculated. From these results general conclusions concerning the dependence of isotope effects from the chemical structure of the corresponding molecules have been drawn. In particular, a relationship between the reduced partition function ratio and the electronic charge of the substituted atom has been found. In addition, examples are given for the application of the calculation algorithm used above in connection with combined isotopic substitutions, radical cations, and transition states of chemical reactions. (author)

  14. 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...

  15. Actinides analysis by accelerator mass spectrometry

    International Nuclear Information System (INIS)

    At the ANTARES accelerator at ANSTO a new beamline has been commissioned, incorporating new magnetic and electrostatic analysers, to optimise the efficiency for Actinides detection by Accelerator Mass Spectrometry (AMS). The detection of Actinides, particularly the isotopic ratios of uranium and plutonium, provide unique signatures for nuclear safeguards purposes. We are currently engaged in a project to evaluate the application of AMS to the measurement of Actinides in environmental samples for nuclear safeguards. Levels of certain fission products, Actinides and other radioactive species can be used as indicators of undeclared nuclear facilities or activities, either on-going or in the past Other applications of ultra-sensitive detection of Actinides are also under consideration. neutron-attenuation images of a porous reservoir rock

  16. Note on isotopic effects in range calculations of high-energy ion beams

    International Nuclear Information System (INIS)

    A simple analytical model that allows the calculation of the percent-level differences of the average ranges of isotopic ion beams slowing down in solid targets is extended to energies in the MeV region and to investigate isotopic effects due to small variations in the mass of the target species. The various contributions to the range in terms of ion stopping, both nuclear and electronic, and angular scattering, can be investigated separately. The model agrees with available experimental data, and predictions are made for a range of cases of interest. (orig.)

  17. Calculation of neutron cross sections on isotopes of yttrium and zirconium

    International Nuclear Information System (INIS)

    Multistep Hauser-Feshbach calculations with preequilibrium corrections were made for neutron-induced reactions on yttrium and zirconium isotopes between 0.001 and 20 MeV. Recently new neutron cross-section data have been measured for unstable isotopes of these elements. These data, along with results from charged-particle simulation of neutron reactions, provide unique opportunities under which to test nuclear-model techniques and parameters in this mass region. A complete and consistent analysis of varied neutron reaction types using input parameters determined independently from additional neutron and charged-particle data. The overall agreement between calculations and a wide variety of experimental results available for these nuclei leads to increased confidence in calculated cross sections made where data are incomplete or lacking. 75 references

  18. 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].

  19. Consistent activation cross section calculations for all stable isotopes of V, Cr, Mn, Fe, Co, Ni

    International Nuclear Information System (INIS)

    Comparison of the available experimental fast neutron reaction excitation functions on all stable isotopes of the elements V, Cr, Mn, Fe, Co, and Ni with nuclear model calculations is presented. Neutron and charged-particle emission spectra have also been analyzed in order to validate the pre-equilibrium emission model calculations (with no free internal parameters). The trial procedure involved provides confidence in the nuclear-model parameter basis used and makes possible calculations of increased accuracy for activation cross sections in this mass range, required for applications. (author). 13 refs, 27 figs

  20. 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

  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. Vapor pressure isotope effects of water studied by molecular orbital calculations

    International Nuclear Information System (INIS)

    H/D and 16O/18O fractionation factors between liquid water and water vapor in the temperature range of 0 to 100degC were calculated using the reduced partition function ratios of small water clusters, (H2O)n with n=1 to 10, obtained at the HF/6-31G(d) and B3LYP/6-311G(d) levels of theory. The calculated fractionation factor values were heavily dependent on the choice of the MO theory and the basis set. Both the calculation levels showed that the formation of hydrogen bonds in liquid water caused the heavier isotopes of hydrogen and oxygen to be preferentially fractionated into the liquid water phase. While the HF/6-31G(d) level calculations yielded better results of the absolute values of the H/D and 16O/18O fractionation factors, the B3LYP/6-311G(d) level calculations reproduced the slopes of their temperature dependence better than the HF/6-31G(d) level calculations. As a whole, the quantitative agreements between the experiment and the present calculations were not satisfactory. It was indicated that a proper choice of MO theory, the basis set and the number of hydrogen bonds per molecule in liquid water may reproduce well the experimental vapor pressure isotope effect data of water. (author)

  3. 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

  4. 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

  5. Calculation of partial isotope incorporation into peptides measured by mass spectrometry

    Directory of Open Access Journals (Sweden)

    Harms Hauke

    2010-06-01

    Full Text Available Abstract Background Stable isotope probing (SIP technique was developed to link function, structure and activity of microbial cultures metabolizing carbon and nitrogen containing substrates to synthesize their biomass. Currently, available methods are restricted solely to the estimation of fully saturated heavy stable isotope incorporation and convenient methods with sufficient accuracy are still missing. However in order to track carbon fluxes in microbial communities new methods are required that allow the calculation of partial incorporation into biomolecules. Results In this study, we use the characteristics of the so-called 'half decimal place rule' (HDPR in order to accurately calculate the partial13C incorporation in peptides from enzymatic digested proteins. Due to the clade-crossing universality of proteins within bacteria, any available high-resolution mass spectrometry generated dataset consisting of tryptically-digested peptides can be used as reference. We used a freely available peptide mass dataset from Mycobacterium tuberculosis consisting of 315,579 entries. From this the error of estimated versus known heavy stable isotope incorporation from an increasing number of randomly drawn peptide sub-samples (100 times each; no repetition was calculated. To acquire an estimated incorporation error of less than 5 atom %, about 100 peptide masses were needed. Finally, for testing the general applicability of our method, peptide masses of tryptically digested proteins from Pseudomonas putida ML2 grown on labeled substrate of various known concentrations were used and13C isotopic incorporation was successfully predicted. An easy-to-use script 1 was further developed to guide users through the calculation procedure for their own data series. Conclusion Our method is valuable for estimating13C incorporation into peptides/proteins accurately and with high sensitivity. Generally, our method holds promise for wider applications in qualitative

  6. 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

  7. Calculation of critical experiment parameters for the High Flux Isotope Reactor

    International Nuclear Information System (INIS)

    Six critical experiments were performed shortly before the initial ascension to power of the High Flux Isotope Reactor (HFIR). Critical configurations were determined at various control rod positions by varying the soluble boron content in the light water coolant. Calculated k-effective was 2% high at beginning-of-life (BOL) typical conditions, but was 1.0 at end-of-life (EOL) typical conditions. Axially averaged power distributions for a given radial location were frequently within experimental error. At specific r,z locations with the core, the calculated power densities were significantly different from the experimentally derived values. A reassessment of the foil activation data seems desirable

  8. 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.

  9. 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

  10. 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

  11. 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)

  12. 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.

  13. Calculations of energy levels and electromagnetic properties for tellurium pair isotopes, by unified method

    International Nuclear Information System (INIS)

    Calculations with the Unified Model (vibrator coupled to two particles), of the energy levels and the eletromagnetic properties have been performed and compared with the twelve pair isotopes from tellurium with A between 112 and 134. The results were analysed using as particles interaction: pairing and SDI (Surface Delta Interaction). The SDI and 3 fonons collective states were used in the fittings, and a syntematic comparison between the theoretical and experimental results was made. The dependence of the results with the model parameters was determined, through large variation sof them. Calculations using 4 fonons have been made, and the importance of the introduced variations in the results was discussed. Calculations have been made in the VAX Computer of the Pelletron at IFUSP. (author)

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

    International Nuclear Information System (INIS)

    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 (Ye) of the corematerial. It is suggested that the temporal variation of Ye 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 54–56Fe, are considered to be key players in controlling Ye 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 Ye 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 54–56Fe. 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. ALMR potential for actinide consumption

    International Nuclear Information System (INIS)

    The Advanced Liquid Metal Reactor (ALMR) is a US Department of Energy (DOE) sponsored fast reactor design based on the Power Reactor, Innovative Small Module (PRISM) concept originated by General Electric. This reactor combines a high degree of passive safety characteristics with a high level of modularity and factory fabrication to achieve attractive economics. The current reference design is a 471 MWt modular reactor fueled with ternary metal fuel. This paper discusses actinide transmutation core designs that fit the design envelope of the ALMR and utilize spent LWR fuel as startup material and for makeup. Actinide transmutation may be accomplished in the ALMR core by using either a breeding or burning configuration. Lifetime actinide mass consumption is calculated as well as changes in consumption behavior throughout the lifetime of the reactor. Impacts on system operational and safety performance are evaluated in a preliminary fashion. Waste disposal impacts are discussed. (author)

  16. 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 ...

  17. 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.

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

    International Nuclear Information System (INIS)

    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

  19. 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)

  20. Ventilation system of actinides handling facility in Oarai-branch of Tohoku University

    International Nuclear Information System (INIS)

    We have reported the development of the facility for handling actinides in Tohoku University at the second KAERI-JAERI joint seminar on PIE technology. Actinide isotopes have most hazardous α-radioactivity. Therefore, a specially designed facility is necessary to carry out experimental study for actinide physics and chemistry. In this paper, we will describe the ventilation system and monitoring system for actinide handling facility. (author)

  1. Derivation of correction factor to be applied for calculated results of PWR fuel isotopic composition by ORIGEN2 code

    Energy Technology Data Exchange (ETDEWEB)

    Suyama, Kenya; Nomura, Yasushi [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment; Murazaki, Minoru [Tokyo Nuclear Service Inc., Tokyo (Japan); Mochizuki, Hiroki [The Japan Research Institute Ltd., Tokyo (Japan)

    2001-11-01

    For providing conservative PWR spent fuel compositions from the view point of nuclear criticality safety, correction factors applicable for result of burnup calculation by ORIGEN2 were evaluated. Its conservativeness was verified by criticality calculations using MVP. To calculate these correction factors, analyses of spent fuel isotopic composition data were performed by ORIGEN2. Maximum or minimum value of the ratio of calculation result to experimental data was chosen as correction factor. These factors are given to each set of fuel assembly and ORIGEN2 library. They could be considered as the re-definition of recommended isotopic composition given in Nuclear Criticality Safety Handbook. (author)

  2. 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

  3. 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.

  4. 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.

  5. ORIGEN-S: SCALE system module to calculate fuel depletion, actinide transmutation, fission product buildup and decay, and associated radiation source terms

    International Nuclear Information System (INIS)

    ORIGEN-S computes time-dependent concentrations and source terms of a large number of isotopes, which are simultaneously generated or depleted through neutronic transmutation, fission, radioactive decay, input feed rates and physical or chemical removal rates. The calculations may pertain to fuel irradiation within nuclear reactors, or the storage, management, transportation or subsequent chemical processing of removed fuel elements. The matrix exponential expansion model of the ORIGEN code is unaltered in ORIGEN-S. Essentially all features of ORIGEN were retained, expanded or supplemented within new computations. The primary objective of ORIGEN-S, as requested by the Nuclear Regulatory Commission, is that the calculations may utilize the multi-energy-group cross sections from any currently processed standardized ENDF/B data base. This purpose has been implemented through the prior execution of codes within either the SCALE System or the AMPX System, developed at the Oak Ridge National Laboratory. These codes compute flux-weighted cross sections, simulating conditions within any given reactor fuel assembly, and convert the data into a library that can be input to ORIGEN-S. Time-dependent libraries may be produced, reflecting fuel composition variations during irradiation. Presented in the document are: detailed and condensed input instructions, model theory, features available, range of applicability, brief subroutine descriptions, sample input, and I/O requirements

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

    International Nuclear Information System (INIS)

    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

  7. TMI-2 decay power: LASL fission-product and actinide decay power calculations for the President's commission on the accident at Three Mile Island

    International Nuclear Information System (INIS)

    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

  8. 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.

  9. Monte Carlo calculations on transmutation of transuranic nuclear waste isotopes using spallation neutrons. Difference of lead and graphite moderators

    International Nuclear Information System (INIS)

    Transmutation rates of 239Pu and some minor actinides (237Np, 241Am, 245Cm and 246Cm), 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 (∼ 30 m3) and contained no fissile material, except for a small amount of fissionable waste nuclei that existed in some cases. Calculations were performed at incident proton energy of 1.5 GeV and spallation target was lead. Also breeding rates of 239Pu and 233U as well as the transmutation rates of two long-lived fission products 99Tc and 129I 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

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

    Science.gov (United States)

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

    1976-01-01

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

  11. Study on remain actinides recovery in pyro reprocessing

    International Nuclear Information System (INIS)

    The spent fuel reprocessing by dry process called pyro reprocessing have been studied. Most of U, Pu and MA (minor actinides) from the spent fuel will be recovered and be fed back to the reactor as new fuel. Accumulation of remain actinides will be separated by extraction process with liquid cadmium solvent. The research was conducted by computer simulation to calculate the stage number required. The calculation's results showed on the 20 stages extractor more than 99% actinides can be separated. (author)

  12. Four years of experience with the use of calculated isotopic correlations in establishing input balances at the La Hague plant

    International Nuclear Information System (INIS)

    For more than four years the La Hague reprocessing plant has been using calculated isotopic correlations to establish and check its input balances. The masses of uranium and plutonium entering the plant are determined by the gravimetric balance method, which utilizes the burnup obtained by calculated isotopic correlation as well as the Pu/U ratio measured at the dissolver after cross-checking with the values obtained by correlation. Further, a verification of all the parameters needed to establish these balances - whether physical or chemical in origin - is carried out systematically by means of internal coherence constants which make it possible to detect any anomalies in the dissolution data. The calculated isotopic correlations were evaluated when the analyses of numerous representative samples of irradiated fuel and experimental results of separated isotopic irradiation in water reactor spectra had been interpreted. The accuracy achieved was improved by allowing in the neutron calculations for effects inherent in the first reactor core and by selecting a set of calculation functions which attenuates (by compensation effects) the various perturbations in the irradiation history. The results obtained at La Hague with calculated isotopic correlations on nearly 600 t of reprocessed UO2, because of their large number and above all their high quality, suggest that it be proposed extending the method to other reprocessing plants. This could be done by the operator himself or by national or international control bodies within the framework of a safeguards arrangement. (author)

  13. 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

  14. Spin and orbital moments in actinide compounds

    DEFF Research Database (Denmark)

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

    1991-01-01

    -electron band-structure calculations, is that the orbital moments of the actinide 5f electrons are considerably reduced from the values anticipated by a simple application of Hund's rules. To test these ideas, and thus to obtain a measure of the hybridization, we have performed a series of neutron scattering...... 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 as...

  15. 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

  16. Chemical analyses and calculation of isotopic compositions of high-burnup UO2 fuels and MOX fuels

    International Nuclear Information System (INIS)

    Chemical analysis activities of isotopic compositions of high-burnup UO2 fuels and MOX fuels in CRIEPI and calculation evaluation are reviewed briefly. C/E values of ORIGEN2, in which original libraries and JENDL-3.2 libraries are used, and other codes with chemical analysis data are reviewed and evaluated. Isotopic compositions of main U and Pu in fuels can be evaluated within 10% relative errors by suitable libraries and codes. Void ratio is effective parameter for C/E values in BWR fuels. JENDL-3.2 library shows remarkable improvement compared with original libraries in isotopic composition evaluations of FP nuclides. (author)

  17. BRAIN 2.0: Time and Memory Complexity Improvements in the Algorithm for Calculating the Isotope Distribution

    Science.gov (United States)

    Dittwald, Piotr; Valkenborg, Dirk

    2014-04-01

    Recently, an elegant iterative algorithm called BRAIN ( Baffling Recursive Algorithm for Isotopic distributio N calculations) was presented. The algorithm is based on the classic polynomial method for calculating aggregated isotope distributions, and it introduces algebraic identities using Newton-Girard and Viète's formulae to solve the problem of polynomial expansion. Due to the iterative nature of the BRAIN method, it is a requirement that the calculations start from the lightest isotope variant. As such, the complexity of BRAIN scales quadratically with the mass of the putative molecule, since it depends on the number of aggregated peaks that need to be calculated. In this manuscript, we suggest two improvements of the algorithm to decrease both time and memory complexity in obtaining the aggregated isotope distribution. We also illustrate a concept to represent the element isotope distribution in a generic manner. This representation allows for omitting the root calculation of the element polynomial required in the original BRAIN method. A generic formulation for the roots is of special interest for higher order element polynomials such that root finding algorithms and its inaccuracies can be avoided.

  18. Results of the isotopic concentrations of WWER calculation Burnup Credit Benchmark NO.2 (CB2)

    International Nuclear Information System (INIS)

    The purpose of this document is to present the results of the nuclide concentrations of the WWER 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 WWER burnup credit benchmark is summarized in [1]. The CB2 benchmark focused on WWER burnup credit study proposed on the 97' Atomic Energy Research symposium [2]. 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. This work also comprises the results obtained by other codes [4]. (Author)

  19. 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 .

  20. 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.

  1. Calculations of kinetic isotope effects in the syn-eliminations of (2-phenylethyl)dimethylamine oxides

    International Nuclear Information System (INIS)

    Transition state theory (TST) calculations of kinetic isotope effects (KIE) for the syn-elimination of (2-phenylethyl)dimethylamine oxides have been carried out for a series of transition state (TS) models encompassing both E1-like and E1cB-like regions of the E2 mechanistic spectrum. A large number of different reaction coordinates were explored for both unsolvated and for coordination of solvent dimethylsulfoxide in the cyclic transition state models. The models of reaction for both solvated and unsolvated models of proton transfer are presented. A simplified method for easier initial screening of reaction coordinate contributions is developed, discussed, and found to produce accurate approximations to the full model KIE values. Both unsolvated and solvated models show E1-like E2 mechanism and the calculated values from both models are in extremely good agreement with experimentally measured KIE. Both models were used to investigate para-substituted derivatives (Z = CL, OCH3) of the parent compound (Z = H). The transition states are related by a shift in structure parallel to the central E2 diagonal of an O'Ferrall-Jencks-Fry reaction diagram, as predicted by Thornton, indicating that in the absence of other factors, the extent to which negative charge is accumulated at C/sub β/ in the transition state is a function primarily of the leaving group. All of the structural parameters such as bond distances and bond angles were related to independent bond orders. Beta-deuterium isotope effects produced by both solvated and nonsolvated models are temperature dependent

  2. Study of multiplication factor sensitivity to the spread of WWER spent fuel isotopics calculated by different codes

    International Nuclear Information System (INIS)

    As a sensitivity study the impact on the system reactivity was studied in the case that different calculational methodologies of spent fuel isotopic concentrations were used for WWER spent fuel inventory computations. The sets of isotopic concentrations obtained by calculations with different codes and libraries as a result of the CB2 international benchmark focused on WWER-440 burnup credit were used to show the spread of the calculated spent fuel system reactivity. Using the MCNP 4B code and changing the isotopics input data, the multiplication factor of an infinite array of the WWER-440 fuel pin cells was calculated. The evaluation of the results shows the sensitivity of the calculated reactivity to different calculational methodologies used for the spent fuel inventory computation. In the studied cases of the CB2 benchmark, the spread of the reference k-results relative to the mean was found less or about ±1% in spite of the fact that the data of isotopic concentrations were spread much more. (author)

  3. 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)

  4. 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.

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

    International Nuclear Information System (INIS)

    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)

  6. Actinide environmental chemistry

    International Nuclear Information System (INIS)

    In order to predict release and transport rates, as well as design cleanup and containment methods, it is essential to understand the chemical reactions and forms of the actinides under aqueous environmental conditions. Four important processes that can occur with the actinide cations are: precipitation, complexation, sorption and colloid formation. Precipitation of a solid phase will limit the amount of actinide in solution near the solid phase and have a retarding effect on release and transport rates. Complexation increases the amount of actinide in solution and tends to increase release and migration rates. Actinides can sorb on to mineral or rock surfaces which tends to retard migration. Actinide ions can form or become associated with colloidal sized particles which can, depending on the nature of the colloid and the solution conditions, enhance or retard migration of the actinide. The degree to which these four processes progress is strongly dependent on the oxidation state of the actinide and tends to be similar for actinides in the same oxidation state. In order to obtain information on the speciation of actinides in solution, i.e., oxidation state, complexation form, dissolved or colloidal forms, the use of absorption spectroscopy has become a method of choice. The advent of the ultrasensitive, laser induced photothermal and fluorescence spectroscopies has made possible the detection and study of actinide ions at the parts per billion level. With the availability of third generation synchrotrons and the development of new fluorescence detectors, X-ray absorption spectroscopy (XAS) is becoming a powerful technique to study the speciation of actinides in the environment, particularly for reactions at the solid/solution interfaces. (orig.)

  7. Ground-state electronic structure of actinide monocarbides and mononitrides

    DEFF Research Database (Denmark)

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

    2009-01-01

    The self-interaction corrected local spin-density approximation is used to investigate the ground-state valency configuration of the actinide ions in the actinide monocarbides, AC (A=U,Np,Pu,Am,Cm), and the actinide mononitrides, AN. The electronic structure is characterized by a gradually...... the localization transition. The calculated valence electron densities of states are in good agreement with photoemission data....

  8. PIE analysis for minor actinide

    International Nuclear Information System (INIS)

    Minor actinide (MA) is generated in nuclear fuel during the operation of power reactor. For fuel design, reactivity decrease due to it should be considered. Out of reactors, MA plays key role to define the property of spent fuel (SF) such as α-radioactivity, neutron emission rate, and criticality of SF. In order to evaluate the calculation codes and libraries for predicting the amount of MA, comparison between calculation results and experimentally obtained data has been conducted. In this report, we will present the status of PIE data of MA taken by post irradiation examinations (PIE) and several calculation results. (author)

  9. 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.

  10. Inventory of programs. Calculation of the isotope inventory after a hypothetical accident at the Cofrentes Nuclear power

    International Nuclear Information System (INIS)

    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)

  11. Use of fast reactors for actinide transmutation

    International Nuclear Information System (INIS)

    The management of radioactive waste is one of the key issues in today's discussions on nuclear energy, especially the long term disposal of high level radioactive wastes. The recycling of plutonium in liquid metal fast breeder reactors (LMFBRs) would allow 'burning' of the associated extremely long life transuranic waste, particularly actinides, thus reducing the required isolation time for high level waste from tens of thousands of years to hundreds of years for fission products only. The International Working Group on Fast Reactors (IWGFR) decided to include the topic of actinide transmutation in liquid metal fast breeder reactors in its programme. The IAEA organized the Specialists Meeting on Use of Fast Breeder Reactors for Actinide Transmutation in Obninsk, Russian Federation, from 22 to 24 September 1992. The specialists agree that future progress in solving transmutation problems could be achieved by improvements in: Radiochemical partitioning and extraction of the actinides from the spent fuel (at least 98% for Np and Cm and 99.9% for Pu and Am isotopes); technological research and development on the design, fabrication and irradiation of the minor actinides (MAs) containing fuels; nuclear constants measurement and evaluation (selective cross-sections, fission fragments yields, delayed neutron parameters) especially for MA burners; demonstration of the feasibility of the safe and economic MA burner cores; knowledge of the impact of maximum tolerable amount of rare earths in americium containing fuels. Refs, figs and tabs

  12. 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

  13. 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)

  14. 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+

  15. Actinides reduction by recycling in a thermal reactor

    International Nuclear Information System (INIS)

    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)

  16. Research in actinide chemistry

    International Nuclear Information System (INIS)

    This research studies the behavior of the actinide elements in aqueous solution. The high radioactivity of the transuranium actinides limits the concentrations which can be studied and, consequently, limits the experimental techniques. However, oxidation state analogs (trivalent lanthanides, tetravalent thorium, and hexavalent uranium) do not suffer from these limitations. Behavior of actinides in the environment are a major USDOE concern, whether in connection with long-term releases from a repository, releases from stored defense wastes or accidental releases in reprocessing, etc. Principal goal of our research was expand the thermodynamic data base on complexation of actinides by natural ligands (e.g., OH-, CO32-, PO43-, humates). The research undertakes fundamental studies of actinide complexes which can increase understanding of the environmental behavior of these elements

  17. 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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Yanase, Satoshi; Oi, Takao [Sophia Univ., Tokyo (Japan). Faculty of Science and Technology

    2015-10-01

    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{sup +} 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.

  19. 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.

  20. 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

  1. Measurements of minor actinides cross sections for transmutation

    International Nuclear Information System (INIS)

    The existing reactors produce two kinds of nuclear waste: the fission products and heavy nuclei beyond uranium called minor actinides (Americium and Curium isotopes). Two options are considered: storage in deep geological site and/or transmutation by fast neutron induced fission. These studies involve many neutron data. Unfortunately, these data bases have still many shortcomings to achieve reliable results. The aim of these measurements is to update nuclear data and complement them. We have measured the fission cross section of 243Am (7370 y) in reference to the (n,p) elastic scattering to provide new data in a range of fast neutrons (1-8 MeV). A statistical model has been developed to describe the reaction 243Am (n,f). Moreover, the cross sections from the following reactions have been be extracted from these calculations: inelastic scattering 243Am (n,n') and radiative capture 243Am (n,γ) cross sections. The direct measurements of neutron cross sections are often a challenge considering the short half-lives of minor actinides. To overcome this problem, a surrogate method using transfer reactions has been used to study few isotopes of curium. The reactions 243Am (3He, d)244Cm, 243Am (3He, t)243Cm and 243Am (3He, α)242Am allowed to measure the fission probabilities of 243,244Cm and 242Am. The fission cross sections of 242,243Cm (162,9 d, 28,5 y) and 241Am (431 y) have been obtained by multiplying these fission probabilities by the calculated compound nuclear neutron cross section relative to each channel. For each measurement, an accurate assessment of the errors was realized through variance-covariance studies. For measurements of the reaction 243Am(n,f), the analysis of error correlations allowed to interpret the scope of these measures within the existing measurements. (author)

  2. The Lawrence Livermore National Laboratory Intelligent Actinide Analysis System

    International Nuclear Information System (INIS)

    The authors have developed an Intelligent Actinide Analysis System (IAAS) for Materials Management to use in the Plutonium Facility at the Lawrence Livermore National Laboratory. The IAAS will measure isotopic ratios for plutonium and other actinides non-destructively by high-resolution gamma-ray spectrometry. This system will measure samples in a variety of matrices and containers. It will provide automated control of many aspects of the instrument that previously required manual intervention and/or control. The IAAS is a second-generation instrument, based on the authors' experience in fielding gamma isotopic systems, that is intended to advance non-destructive actinide analysis for nuclear safeguards in performance, automation, ease of use, adaptability, systems integration and extensibility to robotics. It uses a client-server distributed monitoring and control architecture. The IAAS uses MGA3 as the isotopic analysis code. The design of the IAAS reduces the need for operator intervention, operator training, and operator exposure

  3. The Lawrence Livermore National Laboratory Intelligent Actinide Analysis System

    International Nuclear Information System (INIS)

    The authors have developed an Intelligent Actinide Analysis System (IAAS) for Materials Management to use in the Plutonium Facility at the Lawrence Livermore National Laboratory. The IAAS will measure isotopic ratios for plutonium and other actinides non-destructively by high-resolution gamma-ray spectrometry. This system will measure samples in a variety of matrices and containers. It will provide automated control of many aspects of the instrument that previously required manual intervention and/or control. The IAAS is a second-generation instrument, based on experience in fielding gamma isotopic systems, that is intended to advance non-destructive actinide analysis for nuclear safeguards in performance, automation, ease of use, adaptability, systems integration and extensibility to robotics. It uses a client-server distributed monitoring and control architecture. The IAAS uses MGA as the isotopic analysis code. The design of the IAAS reduces the need for operator intervention, operator training, and operator exposure

  4. ZZ AMZ, 70-Group 40 Isotope Multigroup Library for Fast Reactor Calculation

    International Nuclear Information System (INIS)

    1 - Description of program or function: format: EXPANDA; number of groups: 70-group library of multigroup constants; nuclides: H-1, Be-9, B-10, B-11, C-12, O-16, N-23, Mg, Al-27, Si, Ti, V, Cr, Mn-55, Fe, Ni, Cu, Ga, Zr, Nb-93, Mo, In-115, Sn, Pb, Th-232, Pa-233, U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242, Am-241, and lumped fission products of U-233, U-235, Pu-239. origin: ENDF/B-IV and ENDF/B-V; weighting spectrum: Fission products inventories for BBR reactor at 360 and 600 days of irradiation were calculated and used as weighting function. AMZ is a 70-group library of multigroup constants for the fast reactor nuclear design code EXPANDA. Data is stored for three temperatures (300 K, 900 K, 2100 K) and for seven background cross sections. The following isotopes are available: H1, Be9, B10, B11, C12, O16, N23, Mg, Al27, Si, Ti, V, Cr, Mn55, Fe, Ni, Cu, Ga, Zr, Nb93, Mo, In115, Sn, Pb, Th232, Pa233, U233, U234, U235, U236, U238, Pu238, Pu239, Pu240, Pu241, Pu242, Am241, and lumped fission products of U233, U235, Pu239. 2 - Method of solution: Nuclear cross sections, transfer matrices, and self-shielding factors were generated from ENDF/B-IV data using the codes NJOY (PSR-0171) and RGENDF

  5. 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

  6. 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

  7. 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

  8. Coupled-Channel Calculation of the Phase Variation in the Scattering of α- Particles by Ni Isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Tamura, Taro

    1965-11-01

    It is shown that coupled-channel calculations can fit very well the recent data by Meriwether et al. of the scattering of α-particles of 25 to 100 MeV by Ni isotopes. It is shown in particular that the energy variation of the phase of the inelastic scattering cross section relative to that of the elastic cross section is reasonably explained in this way.

  9. 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)

  10. Calculation of boron-isotope fractionation between B(OH)(3)(aq) and B(OH)(4)(-)(aq)

    Energy Technology Data Exchange (ETDEWEB)

    Rustad, James R.; Bylaska, Eric J.; Jackson, Virgil E.; Dixon, David A.

    2010-05-15

    Density functional and correlated molecular orbital calculations (MP2) are carried out on B(OH)3-nH2O clusters (n = 0, 6,32), and B(OH)-4.nH20 (n = 0, 8, 11, 32) to estimate the equilibrium distribution of 10B and 11B isotopes between boric acid and borate in aqueous solution. For the large 32-water clusters, multiple conformations are generated from ab initio molecular dynamics simulations to account for the effect of solvent fluctuations on the isotopic fractionation. We provide an extrapolated value of the equilibrium constant x34 for the isotope exchange reaction 10B(OH)3(aq) + 11B(OH)-4 (aq) = 11B(OH)3(aq) + 11B(OH)-4 (aq) of 1.026-1.028 near the MP2 complete basis set limit with 32 explicit waters of solvation. With some exchange-correlation functionals we find potentially important contributions from a tetrahedral neutral B(OH)3.H2O Lewis acid-base complex. The extrapolations presented here suggest that DFT calculations give a value for 103lnx34 about 15% higher than the MP2 calculations.

  11. Research in actinide chemistry

    Energy Technology Data Exchange (ETDEWEB)

    1991-01-01

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

  12. PF-4 actinide disposition strategy

    International Nuclear Information System (INIS)

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

  13. 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).

  14. 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

  15. 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)

  16. 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.

  17. 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...

  18. 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.)

  19. 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)

  20. 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

  1. Biological pathways and chemical behavior of plutonium and other actinides in the environment

    International Nuclear Information System (INIS)

    The principal long-lived actinide elements that may enter the environment from either U or Pu fuel cycles are Pu, Am, Cm, and Np. Approximately 25% of the alpha activity estimated to be released to the atmosphere from the LMFBR fuel cycle will be contributed by 241Am, 242Cm, and 244Cm. The balance of the alpha activity will come from Pu isotopes. Activities of 242Cm, 244Cm, 241Am, 243Am, and 237Np in waste may exceed concentrations of Pu isotopes in waste after various periods of decay. Thorium and uranium isotopes may also be released by operations of the thorium fuel cycle. Environmental actinides are discussed under the following headings: sources of man-made actinide elements; pathways of exposure; environmental chemistry of actinides; uptake of actinides by plants; distribution of actinides in components of White Oak Lake; entry of actinides into terrestrial food chains; relationship between chemical behavior and uptake of actinides by organisms; and behavior of Pu in freshwater and marine food chains

  2. 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

  3. 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.

  4. 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

  5. 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)

  6. Actinides at the crossroads: ICP-MS or alpha spectrometry?

    International Nuclear Information System (INIS)

    The report contains viewgraphs only that summarize the following: Why turn to mass spectrometry for radiochemical measurements; What might be some advantages of using ICP mass spectrometry; Sensitivity of ETV-ICP-MS relative to decay counting (versus half-life); ICP-MS instrument detection limits for dissolved actinide isotopes; Effect of dissolved solids on USN-ICP-MS analysis; Polyatomic ion interferences in ICP-MS actinide measurements; Effect of operating conditions on uranium and protonated uranium signal; ICP mass spectrometry performance in actinide determinations; Determination of actinide elements in soil; Leachable Th-230 and Pu-239 in soil as determined by ICP-MS and alpha spectrometry; Leachable U-234 and U-238 in soil by ICP-MS and alpha spectrometry; Determination of uranium isotopic composition on smears; Activity ratios (U-234/U-238) as determined by mass spectrometry and alpha spectrometry; Uranium isotopic abundances as determined by TIMS and ICP-MS; and Comparison of uranium atom percentages determined by TIMS and ICP-MS. It is concluded that isotope dilution and radiochemical preparative techniques work well in radioanalytical applications of ICP-MS; radioanalytical ICP-MS data are equivalent to data from standard methods (TIMS, alpha spectrometry); and applications in radiation protection and earth sciences are certain to expand further

  7. 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.)

  8. Radiochemistry and actinide chemistry

    International Nuclear Information System (INIS)

    The analysis of trace amounts of actinide elements by means of radiochemistry, is discussed. The similarities between radiochemistry and actinide chemistry, in the case of species amount by cubic cm below 1012, are explained. The parameters which allow to define what are the observable chemical reactions, are given. The classification of radionuclides in micro or macrocomponents is considered. The validity of the mass action law and the partition function in the definition of the average number of species for trace amounts, is investigated. Examples illustrating the results are given

  9. 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

    2011-10-01

    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.

    This comment has no merit for the following reasons: (a the isotopic composition of photosynthetic oxygen cannot be "defined", it can only be measured, modelled or calculated based on other data; (b the isotopic composition of photosynthetic oxygen was not "defined" in Kaiser (2011a, but derived from published measurements; (c the published measurements themselves were inconsistent and no single result could be identified as best; (d since no best value could be identified, a hypothetical base case was constructed in a way that was consistent with previous publications; (e the values of 17δP=−11.646‰ and 18δP=−22.835‰ assumed for the base case are compatible with the experimental evidence published before the paper of Kaiser (2011a; (f even if the "biological end-member" was based on a definition, there could be no argument about the "consistency" of this definition – as per its nature, a definition is arbitrary.

    The qualification of base case gross production values as being "30 % too high" must therefore also be rejected. Even though recently revised measurements of the relative 17O/16O isotope ratio difference between VSMOW and Air-O2, 17δVSMOW (Barkan and Luz, 2011, do support lower estimates of gross production, our own measurements disagree with these revised 17δVSMOW values. If scaled for differences in 18

  10. 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

  11. 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.

  12. The speciation of actinide ions in concentrated salt solutions

    International Nuclear Information System (INIS)

    Many separations of actinide ions involve concentrated solutions. There is additional interest in actinide behavior in brine solutions in the WIPP salt repository. Unfortunately, little understanding exists on the speciation of actinides in concentrated solutions. The author has studied the extraction distribution of Am(III) as a function of concentration of NX salts (N-, Li+, Na+, K+, NH4+ and X = ClO4-, Cl-, NO3-). Analyses of the distribution curves are discussed in terms of hydration, complexation, etc. effects on the Am(III). The variation of the calculated stability constants with ionic strength is compared with the expected variation using Specific-Ion Interaction Theory (SIT)

  13. 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...... 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...

  14. A modified Gaussian integration method for thermal reaction rate calculation in U- and Pu-isotopes

    International Nuclear Information System (INIS)

    An advanced multi-group cell calculations a lot of data information is very often necessary, and hence the data administration will be elaborate, and the spectrum calculation will be time consuming. We think it is possible to reduce the necessary data information by using an effective reaction rate integration method well suited for U- and Pu-absorptions (author)

  15. Fission level density and barrier parameters for actinide neutron-induced cross section calculations. Final report of research contract 8832/RB. Time period covered: 15 December 1995 - 14 June 1998

    International Nuclear Information System (INIS)

    Fission and total level densities modelling approach was developed. Neutron-induced fission cross section data for incident energies from 10 keV up to emissive fission threshold were employed to extract level density and fission barrier parameters. In particular, fission barrier parameters (inner barrier height, outer barrier height, curvatures) were extracted for altogether 49 isotopes of Th, Pa, U, Np, Pu, Am, Cm, Bk, and Cf. The adopted level density modelling approach and fission barrier parametrization was supported by calculations of fission cross section data above the emissive fission threshold, up to 20 MeV neutron incident energy. (author)

  16. 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

  17. 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.)

  18. Actinide separative chemistry

    International Nuclear Information System (INIS)

    Actinide separative chemistry has focused very heavy work during the last decades. The main was nuclear spent fuel reprocessing: solvent extraction processes appeared quickly a suitable, an efficient way to recover major actinides (uranium and plutonium), and an extensive research, concerning both process chemistry and chemical engineering technologies, allowed the industrial development in this field. We can observe for about half a century a succession of Purex plants which, if based on the same initial discovery (i.e. the outstanding properties of a molecule, the famous TBP), present huge improvements at each step, for a large part due to an increased mastery of the mechanisms involved. And actinide separation should still focus R and D in the near future: there is a real, an important need for this, even if reprocessing may appear as a mature industry. We can present three main reasons for this. First, actinide recycling appear as a key-issue for future nuclear fuel cycles, both for waste management optimization and for conservation of natural resource; and the need concerns not only major actinide but also so-called minor ones, thus enlarging the scope of the investigation. Second, extraction processes are not well mastered at microscopic scale: there is a real, great lack in fundamental knowledge, useful or even necessary for process optimization (for instance, how to design the best extracting molecule, taken into account the several notifications and constraints, from selectivity to radiolytic resistivity?); and such a need for a real optimization is to be more accurate with the search of always cheaper, cleaner processes. And then, there is room too for exploratory research, on new concepts-perhaps for processing quite new fuels- which could appear attractive and justify further developments to be properly assessed: pyro-processes first, but also others, like chemistry in 'extreme' or 'unusual' conditions (supercritical solvents, sono-chemistry, could be

  19. 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

  20. Ten years of experience in extraction chromatographic processes for the recovery, separation and purification of actinides elements

    International Nuclear Information System (INIS)

    Ten years ago the extraction chromatographic technique was developed for preparative purposes and is now applied for all chemicals separations needed for the production of actinides isotopes. That technique appears to be simple and flexible. It can be used for the production of microgram to kilogram amounts of actinide isotopes. This paper focuses on the experience gained and describes some peculiar production of actinide isotopes solved by using extraction chromatographic technique. After a review of extracting molecules and equipment, treatment of irradiated targets (preparation of Pu 238 and removal of neptunium, production of Am 243 and Cm 244), recovery of actinides from alpha aqueous wastes (preparation of Am 241) and recovery of decay products from aged actinide stocks (recovery of Am 241 from Pu stocks, of U 234 from Pu 238 stocks) are described

  1. 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.

  2. 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.)

  3. 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

  4. Direct calculation of equilibrium constants for isotopic exchange reactions by ab initio molecular orbital theory

    International Nuclear Information System (INIS)

    The ability of simple levels of ab initio molecular orbital theory to describe with reasonable accuracy the energetics of isotopic exchange processes is demonstrated. Three levels of ab initio molecular orbital theory have been surveyed. The first two levels are single-determinant Hartree-Foch methods utilizing the 3-21G split-valence and 6-31G* polarization basis sets. The third level, which is computationally the most complex, uses the 6-31G* basis set but allows for partial account of electron correlation by way of Moller-Plesset perturbation theory terminated at second order. Theoretical and spectroscopic equilibrium constants for reactions XH + XD reversible XD + H2 where XD is a hydride of the first row of the periodic table are tabulated

  5. First-principles calculation of H/D isotopic fractionation between hydrous minerals and water

    OpenAIRE

    Meheut, M.; Lazzeri, M.; Balan, Etienne; Mauri, F.

    2010-01-01

    Hydrogen fractionation laws between selected hydrous minerals (brucite, kaolinite, lizardite, and gibbsite) and perfect water gas have been computed from first-principles quantum-mechanical calculations. The beta-factor of each phase was calculated using the harmonic phonon dispersion curves obtained within density functional theory. All the fractionation laws show the same shape, with a minimum between 200 degrees C (brucite) and 500 degrees C (gibbsite). At low temperatures, the mineral/liq...

  6. Structure effects in the calculation of beta strength functions and half lives of Rb and Br isotopes

    International Nuclear Information System (INIS)

    The properties of beda delayed neutron emission of the precursors around mass 95 are investigated using spherical Shell Model plus pairing. The objective of this work is to find out the important parameters that effect these properties. The strength functions and half lives of both even and odd Rb and Br precursors are calculated in BCS quasi-particle theory as well as in Seniority Truncated Exact Diagonalization (STED) scheme. The calculated half lives from the two schemes are in close agreement with each other. STED gave much smoother overall trend which is in better agreement with experimental values. The calculations reveal that the so called 'odd decays' which depend in an essential way on the parent ground state configuration are of crucial importance in determining both half life, t/sub 1/2/ and delayed neutron emission probability, P/sub n/. Furthermore, it is shown that it is not possible to choose apriori global set for the single particle Shell model basis to predict the correct ground state configurations for both the odd and even nuclei. Instead, it is necessary to examine available experimental evidence in order to construct a more valid global set for single particle basis. The significant variations of the predicted half lives according to the different parent ground-state configuration choices, reveal the importance of nuclear structure effects in these isotopes. The calculated t/sub 1/2/ and P/sub n/ of Rb and Br precursors are presented, discussed and compared with experimental values

  7. 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.

  8. 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.

  9. 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.

  10. 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

  11. 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)

  12. 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...

  13. 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

  14. Isotopic Generation and Confirmation of the PWR Application Model 

    Energy Technology Data Exchange (ETDEWEB)

    L.B. Wimmer

    2003-11-10

    The objective of this calculation is to establish an isotopic database to represent commercial spent nuclear fuel (CSNF) from pressurized water reactors (PWRs) in criticality analyses performed for the proposed Monitored Geologic Repository at Yucca Mountain, Nevada. Confirmation of the conservatism with respect to criticality in the isotopic concentration values represented by this isotopic database is performed as described in Section 3.5.3.1.2 of the ''Disposal Criticality Analysis Methodology Topical Report'' (YMP 2000). The isotopic database consists of the set of 14 actinides and 15 fission products presented in Section 3.5.2.1.1 of YMP 2000 for use in CSNF burnup credit. This set of 29 isotopes is referred to as the principal isotopes. The oxygen isotope from the UO{sub 2} fuel is also included in the database. The isotopic database covers enrichments of {sup 235}U ranging from 1.5 to 5.5 weight percent (wt%) and burnups ranging from approximately zero to 75 GWd per metric ton of uranium (mtU). The choice of fuel assembly and operating history values used in generating the isotopic database are provided is Section 5. Tables of isotopic concentrations for the 29 principal isotopes (plus oxygen) as a function of enrichment and burnup are provided in Section 6.1. Results of the confirmation of the conservatism with respect to criticality in the isotopic concentration values are provided in Section 6.2.

  15. 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

  16. 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.

  17. Actinide nuclear data evaluation for BROND and beyond

    International Nuclear Information System (INIS)

    The neutron cross sections of minor actinides U, Pu, Am, Cm have been calculated in the energy range of 0.01 to 20 MeV. The optical cross sections were calculated with coupled channel model. Since in case of minors the fission data fit is virtually the only constraint for (n,xn), x=1,2,3 and (n,γ) calculations, the theoretical tools employed were tested in case of consistent analysis of total, (n,f), (n,γ), (n,n'), (n,2n) and (n,3n) data for major actinides. The role of statistical model parameters testing is exemplified. (author)

  18. 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.

  19. 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

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

    International Nuclear Information System (INIS)

    The need for improved nuclear data for minor actinides has been stressed by various organizations throughout the world - especially for studies relating to plutonium management, waste incineration, transmutation of waste, and Pu burning in future nuclear concepts. Several international programs have indicated a strong desire to obtain accurate integral reaction rate data for improving the major and minor actinides cross sections. Data on major actinides (i.e. 235U, 236U, 238U, 239Pu, 240Pu, 241Pu, 242Pu and 241Am) are reasonably well-known and available in the Evaluated Nuclear Data Files (JEFF, JENDL, ENDF-BX However information on the minor actinides (i.e. 232Th, 233U, 237Np, 238Pu, 242Am, 243Am, 243Cm, 235Cm, 244Cm, 245Cm, 246Cm and 247Cm) is less well-known and considered to be relatively poor in some cases, having to rely on model and extrapolation of few data points. In this framework, the ambitious OSMOSE program between the Commissariat a l'Energie Atomique (CEA), Electricite de France (EDF) and the U.S. Dept. of Energy (DOE) has been undertaken with the aim of measuring the integral absorption rate parameters of actinides in the MINERVE experimental facility located at the CEA Cadarache Research Center. The OSMOSE Program (Oscillation in Minerve of isotopes in 'Eupraxic' Spectra) includes a complete analytical program associated with the experimental measurement program and aims at understanding and resolving potential discrepancies between calculated and measured values. In the OSMOSE program, the reactivity worth of samples containing separated actinides are measured in different neutron spectra using an oscillation technique with an overall expected accuracy better than 3%. Reactivity effects of less than 10 pcm (0.0001 or approximately 1.5 cents) are measured and compared with calibrations to determine the differential reactivity-worth of the individual samples. The first experimental results were obtained with a very good reproducibility in 2005 and

  1. 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...

  2. Analysis of optical properties of actinide dioxides

    International Nuclear Information System (INIS)

    Ionic calculations, symmetry considerations, and detailed analysis of reflectivity experiments have been used to identify general features of the band structure of actinide dioxides with a fluorite lattice. The ionic calculations adjust atomic energy levels by the electrostatic energies arising from long range electric fields of the ionic lattice; the labelling of high lying energy bands is determined by symmetry; experimental analysis includes the use of appropriate sum rules. A combination of these considerations enable a tentative band scheme to be constructed. It is suggested that there are filled valence bands (GAMMA15,GAMMA'25) originating in oxygen 2p-states and empty conduction bands (GAMMA1,GAMMA12,GAMMA'25) originating in actinide 7s and 6d states. The mean band gap (Penn gap) is of the order of 14 eV. The actinide f-electron states, which lie approximately 5 eV below the conduction bands, are taken to be localized - at least in UO2. (author)

  3. Carbon Isotope Composition of Ecosystem Respired Carbon Dioxide in Three Boreal Forest Ecosystems: Measurements and Model Calculations

    Science.gov (United States)

    Cai, T.; Flanagan, L. B.

    2007-12-01

    We conducted measurements of seasonal and inter-annual variation in the carbon isotope composition of ecosystem respired CO2 (δR) in aspen, black spruce and jack pine dominated ecosystems in northern Saskatchewan during 2004-2006 as part of the Fluxnet-Canada Research Network. All three sites showed relatively small variation (approximately -26 to -29 per mil) in δR values during the entire study. The measurements were strongly correlated with modeled δ13C values of ecosystem respired CO2. The model calculated leaf CO2 assimilation, stomatal conductance and chloroplast CO2 concentration separately for sunlit and shaded leaves within multiple canopy layers, and, therefore, allowed us to estimate canopy photosynthetic 13C discrimination. All three sites showed variation in canopy 13C discrimination in response to environmental conditions in a manner consistent with well-known leaf-level studies. Specifically, 13C discrimination was positively correlated with soil moisture and negatively correlated with photon flux density, air temperature and vapor pressure deficit. As a consequence a strong diurnal pattern was observed for 13C discrimination. The measured δR values also varied in response to environmental conditions in a manner consistent with well-known leaf-level studies of photosynthetic 13C discrimination, but with a dampened response caused by the contribution of heterotrophic respiration, which had a constant δ13C value. These results indicate that the stable isotope composition of respired CO2 is a useful ecosystem-scale tool to study constraints to photosynthesis and acclimation of ecosystems to environmental stress.

  4. Calculation of excitation functions for the production of Cu and Co medical isotopes

    International Nuclear Information System (INIS)

    Copper and cobalt radioisotopes have been used for both diagnostic and therapeutic purposes in the field of nuclear medicine. There is considerable interest in 60,61,64,67Cu and 55,57Co radioisotopes for some applications like PET, SPECT imaging and targeted radiotherapy of tumors. In present study, the production of 60,61,64,67Cu and 55,57Co via 64Zn(p,a)61Cu, 67Zn(p,a)64Cu, 70Zn(p,a)67Cu, 58Ni(p,a)55Co, 60Ni(p,a)57Co, 64Zn(p,na)60Cu and 68Zn(p,na)64Cu reactions have been investigated in the range of 5-40 MeV proton incident energy. The new version of the code ALICE-2011 is used to determine the excitation functions of these nuclear reactions. The calculated excitation functions were compared with experimental results and semi-empirical cross section values of a previously developed model. (orig.)

  5. 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)

  6. 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

  7. 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

  8. RIPL starter file parameter validation for actinide nuclei

    International Nuclear Information System (INIS)

    Nuclear reaction theory calculations are of particular importance for actinide nuclei data evaluation. Measured data base for 238-U provides a unique possibility to compare calculated data with measured total, elastic, inelastic, fission, capture, (n,2n), (n,3n) and (n,4n) cross section data up to 40 MeV

  9. 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

  10. Shielding calculations by using the analytic methods : Application to the radio-isotopes production in the CENM reactor

    International Nuclear Information System (INIS)

    Full text: this work is part of developing an analytical method for solving the neutrons transport equation in improving the treatment of the anisotropy of neutron scattering through heterogeneous shielding. We also develop the tools necessary for the formation of multigroup libraries (cross section) with the best choice of the weighting function. Among the radioprotection problems of radioisotopes production experiments in the research reactor core is mainly the photons gamma generation produced by radiative capture: activation of samples and their capsules. So, in order to review the safety of operating personnel and the public is essential to quantify the neutrons flux and gamma photons produced. In this study a numerical methods is used in two different Fortran program to solve the neutron transport problem and to determine the neutron and photon flux. This program based on the Monte Carlo method: the neutron is born with a unit statistical weight, this corrected after each imposed scattering event during its whole history within the shield. The final neutron statistical weight is used in an appropriate estimator to determine the searched response. The generated gamma rays by neutron capture are calculated of different isotopes, and then the equivalent dose rate is evaluated in biological tissue for different neutron source energies. We have identified and studied the choice of the best weighting function to calculate a library of multigroup cross sections self protected by using the energy weighting function. A Fortran program is used as a mathematical tool to solve the neutron slowing down equation in infinite homogeneous medium for different dilutions. We determined the energetic flux distribution and the effective integrals. The results of both calculations are in a good agreement; the relative error is less than 0.5%.

  11. 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

  12. Systematic analysis of fission cross sections of uranium and plutonium isotopes

    International Nuclear Information System (INIS)

    Neutron induced fission cross section of 10 actinide nuclei is analyzed in terms of the double humped fission barrier model to deduce the barrier heights. Good fits were obtained by assuming the inner barrier axially-asymmetric and the outer one mass asymmetric. The obtained values of barrier heights are compared to other results. Systematic trends were observed in the barrier heights of the isotopes studied, their isotopical dependence presents the odd-even fluctuations. The difference EA-EB with increasing of neutron number is also analyzed. The level density is calculated in the frame of Semimicroscopical Combined Method (SCM) for all extreme points of fission path

  13. Comparative analysis of spent fuel isotope composition for VVER-440 compare to VVER-1000 reactors

    International Nuclear Information System (INIS)

    Calculations were made for reactor cell of fuel assemblies for VVER-440 and VVER-1000 depending on their manufactory and operation conditions. These cells were composed of the fuel assemblies with the maximum multiplying purpose (enrichment of 4.4% for both reactor types). Concentration as function of burnup of ten most usable isotopes, such as main fuel isotopes U235, U236, U238, Pu239, Pu240, Pu241, as well as some actinides, and fission products, such as Pu242, Am241, Sm149, Sm151 was analyzed

  14. The fission fragment yields at the photofission of actinide nuclei

    International Nuclear Information System (INIS)

    The fission fragment yields of isotopes 101Mo, 135I, 135mCs were measured at the photo-fission of actinide nuclei 232Th, 238U, 237Np. These fission fragments have some peculiarities in nuclear structure or in practical using. The measurements were performed on the microtron bremsstrahlung at the Flerov Laboratory of Nuclear Reactions, JINR, at the electron energy 22 MeV. The activation method with an HPGe detector was used in these measurements of the yields

  15. Measurement of fast neutron induced fission cross section of minor-actinide

    International Nuclear Information System (INIS)

    In fuel cycles with recycled actinide, core characteristics are largely influenced by minor actinide (MA: Np, Am, Cm). Accurate nuclear data of MA such as fission cross section are required to estimate the effect of MA with high accuracy. In this study, fast neutron induced fission cross section of MA is measured using Dynamitron Accelerator in Tohoku University. The experimental method and the samples, which were developed or introduced during the last year, were improved in this fiscal year: (1) Development of a sealed fission chamber, (2) Intensification of Li neutron target, (3) Improvement of time-resolution of Time-of-Flight (TOF) electronic circuit, (4) Introduction of Np237 samples with large sample mass and (5) Introduction of a U235 sample with high purity. Using these improved tools and samples, the fission cross section ratio of Np237 relative to U235 was measured between 5 to 100 keV, and the fission cross section of Np237 was deduced. On the other hand, samples of Am241 and Am243 were obtained from Japan Atomic Energy Research Institute (JAERI) after investigating fission cross section of two americium isotopes (Am241 and Am 243) which are important for core physics calculation of fast reactors. (author)

  16. 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)

  17. Actinides and the environment

    International Nuclear Information System (INIS)

    The book combines in one volume the opinions of experts regarding the interaction of radionuclides with the environment and possible ways to immobilize and dispose of nuclear waste. The relevant areas span the spectrum from pure science, such as the fundamental physics and chemistry of the actinides, geology, environmental transport mechanisms, to engineering issues such as reactor operation and the design of nuclear waste repositories. The cross-fertilization between these various areas means that the material in the book will be accessible to seasoned scientists who may wish to obtain an overview of the current state of the art in the field of environmental remediation of radionuclides, as well as to beginning scientists embarking on a career in this field. refs

  18. 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.

  19. IBM-1 calculations of low-lying excited levels and electric transition probabilities B(E2) on the even-even 174-180Hf isotopes

    International Nuclear Information System (INIS)

    In this paper, the interacting boson model (IBM-1) is discussed and employed for calculating the energy level and the electromagnetic transition probabilities B(E2) of the even - even 174-180Hf isotopes. These isotopes have been investigated based on two different arrangements; i.e., the dynamical symmetry of 176-180Mf isotopes, SU (3) (deformed nuclei) and the dynamical symmetry of 174Hf isotopein transition region SU(30-O(6). The determined values using the IBM-1 Hamiltonian showed significant agreement with the experimentally reported energy level and B(E2) values. The model provides a fast and accurate predication method of energy level B(E2)values. (authors).

  20. Calculations of low laying energy levels of even-even Cd, Sn and Te isotopes in the “Interacting Boson Model” framework

    OpenAIRE

    S. M. Mostajabodda’vati; Parvaresh, A.; E. Hassanzadeh

    2004-01-01

      The dynamical symmetries in even-even nuclei were investigated by Arima and Iachello in 1974, and led to a model called &quotInteracting Boson Model, (IBM)".   In this article we have outlined some basic ideas used in IBM-1 and carried out the calculations for low laying energy levels of even-even isotopes Cd, Sn and Te via PHINT code.   The calculations for energy and quadra pole moment transitions is done and compared to the available experimental data and IBM -.2 calculations...

  1. 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)

  2. 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.

  3. 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 ...

  4. 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.

  5. 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

  6. 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.

  7. Properties of minor actinide nitrides

    International Nuclear Information System (INIS)

    The present status of the research on properties of minor actinide nitrides for the development of an advanced nuclear fuel cycle based on nitride fuel and pyrochemical reprocessing is described. Some thermal stabilities of Am-based nitrides such as AmN and (Am, Zr)N were mainly investigated. Stabilization effect of ZrN was cleary confirmed for the vaporization and hydrolytic behaviors. New experimental equipments for measuring thermal properties of minor actinide nitrides were also introduced. (author)

  8. 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

  9. 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

  10. 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

  11. 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

  12. Electron-phonon coupling of the actinide metals

    DEFF Research Database (Denmark)

    Skriver, H. L.; Mertig, I.

    1985-01-01

    The authors have estimated the strength of the electron-phonon coupling in Fr and Ra plus the light actinides Ac through Pu. The underlying self-consistent band-structure calculations were performed by the scalar relativistic linear-muffin-tin-orbital method including l quantum numbers s through g...

  13. Reducing the impact of used fuel by transmuting actinides in a CANDU reactor

    International Nuclear Information System (INIS)

    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 in CANDU reactors to reduce the decay heat period. Many of the design features of the CANDU reactor make it uniquely adaptable to actinide transmutation. The small, simple fuel bundle facilitates the fabrication and handling of active fuels. Online refueling 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 in CANDU reactors, including both recent and past activities. The transmutation schemes that are presented reflect several different partitioning schemes and include both 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. (author)

  14. Bulk properties of light actinides: modified second variation method

    International Nuclear Information System (INIS)

    The second variation method is a common and efficient way of treating the spin-orbit coupling within electronic structure codes. While it works satisfactorily for most elements, it was demonstrated recently to be inadequate for light actinides. The problem was traced back to insufficient description of the 6p states, resulting in a poor convergence of the total energies with respect to the computational parameters. We present a simple way to overcome this deficiency and demonstrate its effect on the stability of the calculation. The results obtained for bulk properties of light actinides (Th-Pu) are compared to those obtained with methods using full Dirac formalism. (author)

  15. 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.

  16. Actinide transmutation in the advanced liquid metal reactor (ALMR)

    International Nuclear Information System (INIS)

    The Advanced Liquid Metal Reactor (ALMR) is a US Department of Energy (DOE) sponsored fast reactor design based on the Power Reactor, Innovative Small Module (PRISM) concept originated by General Electric. The current reference design is a 471 MWt modular reactor loaded with ternary metal fuel. This paper discusses actinide transmutation core designs that fit the design envelope of the ALMR and utilize spent LWR fuel as startup material and makeup. Actinide transmutation may be accomplished in the ALMR by using either a breeding or burning configuration. Lifetime actinide mass consumption is calculated as well as changes in consumption behaviour throughout the lifetime of the reactor. Impacts on system operational and safety performance are evaluated in a preliminary fashion. (author). 3 refs, 6 figs, 3 tabs

  17. 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

  18. 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...

  19. Plutonium build-up credits for a material test research reactor and influence of cross-section differences on actinide production

    International Nuclear Information System (INIS)

    Burnup calculations with SARC system were carried out to analyse the effects of plutonium build-up on criticality of MTR type research reactor PARR-1 using several WIMSD libraries based on evaluated nuclear data files ENDFB-VI.8, JEF-2.2, JEFF-3.1 and JENDL-3.2. For equilibrium core of the reactor, it was found that a net reactivity of more than 3.5 mk is induced due to build-up of plutonium isotopes during depletion. The plutonium credit amounts to 3% of the length of equilibrium cycle. From the analysis of actinide production in the core during burnup, it was observed that in most of the cases, the amounts of actinides obtained using various cross section libraries agree fairly with each other, however, significant differences were observed for 238Pu, 241Pu, 242mAm, 243Am, 242Cm and 244Cm for some libraries. The actinide chain analysis was conducted to investigate the reasons for the observed differences

  20. Plutonium build-up credits for a material test research reactor and influence of cross-section differences on actinide production

    Energy Technology Data Exchange (ETDEWEB)

    Ahmad, Siraj Islam [Pakistan Institute of Engineering and Applied Sciences, Islamabad-45650 (Pakistan)]. E-mail: sirajisl@yahoo.co.uk; Ahmad, Nasir [Pakistan Institute of Engineering and Applied Sciences, Islamabad-45650 (Pakistan)

    2006-12-15

    Burnup calculations with SARC system were carried out to analyse the effects of plutonium build-up on criticality of MTR type research reactor PARR-1 using several WIMSD libraries based on evaluated nuclear data files ENDFB-VI.8, JEF-2.2, JEFF-3.1 and JENDL-3.2. For equilibrium core of the reactor, it was found that a net reactivity of more than 3.5 mk is induced due to build-up of plutonium isotopes during depletion. The plutonium credit amounts to 3% of the length of equilibrium cycle. From the analysis of actinide production in the core during burnup, it was observed that in most of the cases, the amounts of actinides obtained using various cross section libraries agree fairly with each other, however, significant differences were observed for {sup 238}Pu, {sup 241}Pu, {sup 242m}Am, {sup 243}Am, {sup 242}Cm and {sup 244}Cm for some libraries. The actinide chain analysis was conducted to investigate the reasons for the observed differences.

  1. 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.

  2. Actinide burning and waste disposal

    International Nuclear Information System (INIS)

    Here we review technical and economic features of a new proposal for a synergistic waste-management system involving reprocessing the spent fuel otherwise destined for a U.S. high-level waste repository and transmuting the recovered actinides in a fast reactor. The proposal would require a U.S. fuel reprocessing plant, capable of recovering and recycling all actinides, including neptunium americium, and curium, from LWR spent fuel, at recoveries of 99.9% to 99.999%. The recovered transuranics would fuel the annual introduction of 14 GWe of actinide-burning liquid-metal fast reactors (ALMRs), beginning in the period 2005 to 2012. The new ALMRs would be accompanied by pyrochemical reprocessing facilities to recover and recycle all actinides from discharged ALMR fuel. By the year 2045 all of the LWR spent fuel now destined f a geologic repository would be reprocessed. Costs of constructing and operating these new reprocessing and reactor facilities would be borne by U.S. industry, from the sale of electrical energy produced. The ALMR program expects that ALMRs that burn actinides from LWR spent fuel will be more economical power producers than LWRs as early as 2005 to 2012, so that they can be prudently selected by electric utility companies for new construction of nuclear power plants in that era. Some leaders of DOE and its contractors argue that recovering actinides from spent fuel waste and burning them in fast reactors would reduce the life of the remaining waste to about 200-300 years, instead of 00,000 years. The waste could then be stored above ground until it dies out. Some argue that no geologic repositories would be needed. The current view expressed within the ALMR program is that actinide recycle technology would not replace the need for a geologic repository, but that removing actinides from the waste for even the first repository would simplify design and licensing of that repository. A second geologic repository would not be needed. Waste now planned

  3. 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.

  4. Kinetics of actinide complexation reactions

    International Nuclear Information System (INIS)

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

  5. 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.

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

    International Nuclear Information System (INIS)

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

  7. 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.

  8. 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)

  9. Criticality and thermal analyses of separated actinides

    International Nuclear Information System (INIS)

    Curium and americium pose special problems in the chemical preparation of spent fuel for transmutation. Once separated from the other actinides, the isotopes can lead to nuclear fission with the subsequent release of a large amount of radiation. A neutron criticality code was used to determine keff for varying quantities of Cm2O3 and Am2O3 held within spherical or cylindrical containers. These geometries were investigated both in air and in water. Recommendations are made on the maximum amount of Cm2O3 and Am2O3 that can be safely stored or handled before encountering criticality. Several isotopes of curium and americium also generate a significant amount of heat by radioactive decay. If kilogram quantities are stored in a container, for example, the material may heat to an equilibrium temperature that exceeds its melting temperature. The heat generation of curium and americium present even more restriction on the mass of that can safely be contained in one location. (author)

  10. 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

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

    OpenAIRE

    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.; France G. de

    2015-01-01

    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 ...

  12. Actinide cation-cation complexes

    International Nuclear Information System (INIS)

    The +5 oxidation state of U, Np, Pu, and Am is a linear dioxo cation (AnO2+) with a formal charge of +1. These cations form complexes with a variety of other cations, including actinide cations. Other oxidation states of actinides do not form these cation-cation complexes with any cation other than AnO2+; therefore, cation-cation complexes indicate something unique about AnO2+ cations compared to actinide cations in general. The first cation-cation complex, NpO2+·UO22+, was reported by Sullivan, Hindman, and Zielen in 1961. Of the four actinides that form AnO2+ species, the cation-cation complexes of NpO2+ have been studied most extensively while the other actinides have not. The only PuO2+ cation-cation complexes that have been studied are with Fe3+ and Cr3+ and neither one has had its equilibrium constant measured. Actinides have small molar absorptivities and cation-cation complexes have small equilibrium constants; therefore, to overcome these obstacles a sensitive technique is required. Spectroscopic techniques are used most often to study cation-cation complexes. Laser-Induced Photacoustic Spectroscopy equilibrium constants for the complexes NpO2+·UO22+, NpO2+·Th4+, PuO2+·UO22+, and PuO2+·Th4+ at an ionic strength of 6 M using LIPAS are 2.4 ± 0.2, 1.8 ± 0.9, 2.2 ± 1.5, and ∼0.8 M-1

  13. 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

  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. Orbital effects in actinide systems

    International Nuclear Information System (INIS)

    Actinide magnetism presents a number of important challenges; in particular, the proximity of 5f band to the Fermi energy gives rise to strong interaction with both d and s like conduction electrons, and the extended nature of the 5f electrons means that they can interact with electron orbitals from neighboring atoms. Theory has recently addressed these problems. Often neglected, however, is the overwhelming evidence for large orbital contributions to the magnetic properties of actinides. Some experimental evidence for these effects are presented briefly in this paper. They point, clearly incorrectly, to a very localized picture for the 5f electrons. This dichotomy only enhances the nature of the challenge

  16. 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)

  17. Cerium compounds in the fashion of the light actinides

    International Nuclear Information System (INIS)

    Researchers familiar with the light actinides easily recognize in cerium compounds a microcosm of the rich variety of properties seen in the light actinides. The parallelism seen between comparable cerium and actinide compounds strongly suggests that the same physical models are applicable. The most significant is the relative size of the f-orbital. Localization is generally tighter in Ce compounds than uranium compounds, making Ce roughly analogous to Np through Am. A way to see the actinide parallelism is to compare Hill plots. Compounds in the different regions of the plots (representing different physics) are isostructural compounds with the same companion (B) elements. The most common materials exhibiting a direct f-f interaction are the cubic Laves compounds. Accordingly, we have determined the band structures of CeRu2, CeRh2, CeIr2, CeOs2, and CeNi2. Compounds illustrative of the interaction of f-orbitals with ligand orbitals are the Cu3Au structured materials. Materials calculated in this class are CeRh3, CePd3, and CeSn3 - the materials of much interest as mixed valent. Although the focus is on the Ce compounds, calculations performed on uranium isomorphs are used to highlight the interesting physics

  18. 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 which...... combines the kinetic energy calculated within the atomic-sphere approximation with Coulomb- and exchange-correlation-energy terms calculated by means of the complete nonspherically symmetric charge density derived from the atomic-sphere potential within nonoverlapping and space-filling cells. The...... calculated surface energies and work functions are in good agreement with the limited experimental data....

  19. Benchmark analyses for BN-600 MOX core with minor actinides

    International Nuclear Information System (INIS)

    Full text: The IAEA has initiated in 1999 a Coordinated Research Project (CRP) on 'Updated Codes and Methods to Reduce the Calculational Uncertainties of the LMFR Reactivity Effects'. The general objective of the CRP is to validate, verify and improve methodologies and computer codes used for calculation of reactivity coefficients in fast reactors aiming at enhancing the utilization of plutonium and minor actinides (MAs). For this purpose, three benchmark models representing different modifications of the BN-600 reactor UOX core have been sequentially established and analyzed,the benchmark specifications being provided by IPPE. The first benchmark model is a hybrid UOX/MOX core, with UOX fuel in the inner core part and MOX fuel in the outer one, the fresh MOX fuel containing depleted uranium and weapons grade plutonium. The second model is a full MOX core, similar MOX fuel composition being assumed; a sodium plenum being introduced above the core to improve the core safety. The third model is analyzed in the paper. The model represents a similar full MOX core, but with plutonium and MAs from 60 GWd/t LWR spent fuel after 50 years cooling (thus assuming a so-called homogeneous recycling of MAs in a fast system). This option is the most challenging one (compared to those analyzed earlier in the CRP) as concerns the reactor safety since an increased content of MAs, in particular americium, and higher (than Pu239) isotopes of Pu leads to less favourable safety parameters. On the other hand, existing uncertainties in nuclear data for MAs and higher Pu isotopes may lead to relatively high uncertainties in the computation results for the considered model. The benchmark results include core criticality at the beginning and end of the equilibrium fuel cycle, kinetics parameters, spatial distributions of power and reactivity coefficients provided by CRP participants and obtained by employing different computation models and nuclear data. Sensitivity studies were performed at

  20. 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.

  1. 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.)

  2. Developing isotopic functions

    International Nuclear Information System (INIS)

    Isotopic functions, or ratios of two isotopic variables, are used to verify Pu and U measurements of spent fuels in reprocessing plants. Systematic methods have been developed for forming and evaluating isotopic functions. This paper describes the method used at Battelle to form and evaluate isotopic functions. The data base at Battelle contains measurements and calculations for the fuel from 35 reactors

  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. ENDF/B-V actinides

    International Nuclear Information System (INIS)

    This document summarizes the contents of the actinides part of the ENDF/B-V nuclear data library released by the US National Nuclear Data Center. This library or selective retrievals of it, are available from the IAEA Nuclear Data Section. (author)

  5. Detection of the actinides and cesium from environmental samples

    Science.gov (United States)

    Snow, Mathew Spencer

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

  6. Potential energy surfaces of Polonium isotopes

    Science.gov (United States)

    Nerlo-Pomorska, B.; Pomorski, K.; Schmitt, C.; Bartel, J.

    2015-11-01

    The evolution of the potential energy landscape is analysed in detail for ten even-even polonium isotopes in the mass range 188\\lt A\\lt 220 as obtained within the macroscopic-microscopic approach, relying on the Lublin-Strasbourg drop model and the Yukawa-folded single-particle energies for calculating the microscopic shell and pairing corrections. A variant of the modified Funny-Hills nuclear shape parametrization is used to efficiently map possible fission paths. The approach explains the main features of the fragment partition as measured in low-energy fission along the polonium chain. The latter lies in a transitional region of the nuclear chart, and will be essential to consistently understand the evolution of fission properties from neutron-deficient mercury to heavy actinides. The ability of our method to predict fission observables over such an extended region looks promising.

  7. Octupole collectivity in the Sm isotopes

    International Nuclear Information System (INIS)

    Microscopic models suggest the occurrence of strong octupole correlations in nuclei with N≅88. To examine the signatures of octupole correlations in this region, the spdf interacting boson approximation model is applied to Sm isotopes with N=86-92. The effects of including multiple negative-parity bosons in this basis are compared with more standard one negative-parity boson calculations and are analyzed in terms of signatures for strong octupole correlations. It is found that multiple negative-parity bosons are needed to describe properties at medium spin. Bands with strong octupole correlations (multiple negative-parity bosons) become yrast at medium spin in 148,150Sm. This region shares some similarities with the light actinides, where strong octupole correlations were also found at medium spin

  8. Systematic study of neutron induced reactions of the actinide nuclei

    Energy Technology Data Exchange (ETDEWEB)

    Maslov, V.M. [Akadehmiya Navuk Belarusi, Minsk (Belarus). Inst. Radyyatsyjnykh Fizika-Khimichnykh Prablem; Kikuchi, Yasuyuki

    1996-06-01

    A statistical theory is used for the calculation of the neutron-induced reaction cross sections of actinide nuclides from 10 keV up to 20 MeV. Available experimental data bases for major actinides were extensively used to develop theoretical tools for consistent evaluation of neutron data of minor actinides. The approach employed up to the second chance fission threshold is based on the full-scale Hauser-Feshbach theory, a phenomenological modelling of level densities, the giant dipole resonance model for gamma-ray emission, the double-humped fission barrier model and the coupled channel optical model calculations. The pairing, collective and shell effects are introduced into the level density model for equilibrium and saddle point deformations. Step-like structures observed in fission cross section of {sup 235}U around 1 MeV incident neutron energies are interpreted as due to pairing effects. Pairing correlation parameters are adjusted to fit the fission cross section slope in the first plateau region. The level density collective effect inclusion influences drastically the extracted experimental fission barrier parameters due to the inner saddle point asymmetry. The shell effects dumping is manifested as a consistent fit of fission data above the second chance fission threshold. In case of minor actinides, fission data fits are used as a constraint for capture and inelastic scattering cross section predictions. The capture cross sections were analyzed with the allowance for (n,{gamma}n`) and (n,{gamma}f) reactions. To fit the high-energy tails in the (n,2n) reaction, the pre-equilibrium processes in the neutron channel were included. All these effects were modelled, and the model parameters were obtained using major actinides neutron data. The resulted parameter systematics were applied for analysis of available data and prediction of capture, inelastic scattering, (n,2n), (n,3n) reaction and fission cross sections. (J.P.N.). 87 refs.

  9. 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.

  10. The OSMOSE Experimental Program for the qualification of integral cross sections of actinides

    International Nuclear Information System (INIS)

    The need of better nuclear data on minor actinides has been stressed by various organizations throughout the world. It especially deals with the studies on plutonium management and waste incineration in existing systems and transmutation of waste or Pu burning in future nuclear concepts. To address this issue, a Working Party of the OECD has been concerned with identifying these needs and has produced a detailed High Priority Request List for Nuclear Data. The first step in obtaining better nuclear data consists in measuring accurate integral data and comparing them to integrated energy dependent data: this comparison provides a direct assessment of the effect of deficiencies in the differential data. Several international programs have indicated a strong desire to obtain accurate integral reaction rate data for improving the major and minor actinides cross sections. Data on major actinides (i.e. 235U, 236U, 238U, 239Pu, 240Pu, 241Pu, 242Pu and 241Am) are reasonably well-known and available in the Evaluated Nuclear Data Files (JEFF, JENDL, ENDF-B). However information on the minor actinides (i.e. 232Th, 233U, 237Np, 238Pu, 242Am, 243Am, 242Cm, 243Cm, 244Cm, 245Cm, 246Cm and 247Cm) is less well-known and considered to be relatively poor in some cases, having to rely on model and extrapolation of few data points. In this framework, the ambitious OSMOSE program between the Commissariat a l'Energie Atomique (CEA), Electricite de France (EDF) and the U.S. Department of Energy (DOE) has been undertaken with the aim of measuring the integral absorption rate parameters of actinides in the MINERVE experimental facility located at the CEA Cadarache Research Center. The OSMOSE Program (Oscillation in Minerve of isOtopes in 'Eupraxic' Spectra) includes a complete analytical program associated with the experimental measurement program and aims at understanding and resolving potential discrepancies between calculated and measured values. The OSMOSE program began in 2005 and will

  11. Molecular solids of actinide hexacyanoferrate: Structure and bonding

    International Nuclear Information System (INIS)

    The hexacyanometallate family is well known in transition metal chemistry because the remarkable electronic delocalization along the metal-cyano-metal bond can be tuned in order to design systems that undergo a reversible and controlled change of their physical properties. We have been working for few years on the description of the molecular and electronic structure of materials formed with [Fe(CN)6]n- building blocks and actinide ions (An = Th, U, Np, Pu, Am) and have compared these new materials to those obtained with lanthanide cations at oxidation state +III. In order to evaluate the influence of the actinide coordination polyhedron on the three-dimensional molecular structure, both atomic number and formal oxidation state have been varied : oxidation states +III, +IV. EXAFS at both iron K edge and actinide LIII edge is the dedicated structural probe to obtain structural information on these systems. Data at both edges have been combined to obtain a three-dimensional model. In addition, qualitative electronic information has been gathered with two spectroscopic tools : UV-Near IR spectrophotometry and low energy XANES data that can probe each atom of the structural unit : Fe, C, N and An. Coupling these spectroscopic tools to theoretical calculations will lead in the future to a better description of bonding in these molecular solids. Of primary interest is the actinide cation ability to form ionic - covalent bonding as 5f orbitals are being filled by modification of oxidation state and/or atomic number.

  12. Promising pyrochemical actinide/lanthanide separation processes using aluminum

    International Nuclear Information System (INIS)

    Thermodynamic calculations have shown that aluminum is the most promising metallic solvent or support for the separation of actinides (An)from lanthanides (Ln). In molten fluoride salt, the technique of reductive extraction is under development in which the separation is based on different distributions of An and Ln between the salt and metallic Al phases. In this process molten aluminum alloy acts as both a reductant and a solvent into which the actinides are selectively extracted. It was demonstrated that a one-stage reductive extraction process, using a concentrated solution, allows a recovery of more than 99.3% of Pu and Am. In addition excellent separation factors between Pu and Ln well above 103 were obtained. In molten chloride media similar separations are developed by constant current electrorefining between a metallic alloy fuel (U60Pu20-Zr10Am2Nd3.5Y0.5Ce0.5Gd0.5) and an Al solid cathode. In a series of demonstration experiments, almost 25 g of metallic fuel was reprocessed and actinides collected as An-Al alloys on the cathode. Analysis of the An-Al deposits confirmed that an excellent An/Ln separation (An/Ln mass ratio = 2400) had been obtained. These results show that Al is a very promising material to be used in pyrochemical reprocessing of actinides. (authors)

  13. 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.

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

    International Nuclear Information System (INIS)

    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 (237Np, 240Pu, 241Am, and 243Am) 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

  15. 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

  16. Actinide behavior in the Integral Fast Reactor. Final project report

    International Nuclear Information System (INIS)

    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 (237Np, 240Pu, 241Am, and 243Am) 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 weapons grade plutonium. Eighteen sets of seven actinide and five light metal targets have been selected for seven day exposure in the Experimental Breeder Reactor-II 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

  17. Toward laser ablation Accelerator Mass Spectrometry of actinides

    International Nuclear Information System (INIS)

    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.

  18. 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.

  19. Sensitivity of ICP-MS, PERALS and alpha spectrometry for the determination of actinides

    International Nuclear Information System (INIS)

    The purpose of this study was to compare the sensitivity of the three most popular techniques for the determination of minor actinides at environmental levels: ICP-MS, PERALS and solid state alpha spectrometry. For each method the limit of detection and the resolution were estimated in order to study the content and isotopic composition of the actinides. The sensitivities of the three determination techniques were compared. Two international reference materials, IAEA-135 (Irish Sea sediment) and IAEA-300 (Baltic Sea sediment) were analyzed for activity concentrations of 238Pu, 239Pu, 240Pu, 241Pu and 241Am. (authors)

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

    International Nuclear Information System (INIS)

    The irradiation of Th232 breeds fewer of the problematic minor actinides (Np, Am, Cm) than the irradiation of U238. This characteristic makes thorium an attractive potential matrix for the transmutation of these minor actinides, as these species can be transmuted without the creation of new actinides as is the case with a uranium fuel matrix. Minor actinides are the main contributors to long term decay heat and radiotoxicity of spent fuel, so reducing their concentration can greatly increase the capacity of a long term deep geological repository. Mixing minor actinides with thorium, three times more common in the Earth's crust than natural uranium, has the additional advantage of improving the sustainability of the fuel cycle. In this work, lattice cell calculations have been performed to determine the results of transmuting minor actinides from light water reactor spent fuel in a thorium matrix. 15-year-cooled group-extracted transuranic elements (Np, Pu, Am, Cm) from light water reactor (LWR) spent fuel were used as the fissile component in a thorium-based fuel in a heavy water moderated reactor (HWR). The minor actinide (MA) transmutation rates, spent fuel activity, decay heat and radiotoxicity, are compared with those obtained when the MA were mixed instead with natural uranium and taken to the same burnup. Each bundle contained a central pin containing a burnable neutron absorber whose initial concentration was adjusted to have the same reactivity response (in units of the delayed neutron fraction β) for coolant voiding as standard NU fuel. (authors)

  1. Trajectory Calculations for Bergman Cyclization Predict H/D Kinetic Isotope Effects Due to Nonstatistical Dynamics in the Product.

    Science.gov (United States)

    Doubleday, Charles; Boguslav, Mayla; Howell, Caronae; Korotkin, Scott D; Shaked, David

    2016-06-22

    An unusual H/D kinetic isotope effect (KIE) is described, in which isotopic selectivity arises primarily from nonstatistical dynamics in the product. In DFT-based quasiclassical trajectories of Bergman cyclization of (Z)-3-hexen-1,5-diyne (1) at 470 K, the new CC bond retains its energy, and 28% of nascent p-benzyne recrosses back to the enediyne on a vibrational time scale. The competing process of intramolecular vibrational redistribution (IVR) in p-benzyne is too slow to prevent this. Deuteration increases the rate of IVR, which decreases the fraction of recrossing and increases the yield of statistical (trapable) p-benzyne, 2. Trapable yields for three isotopomers of 2 range from 72% to 86%. The resulting KIEs for Bergman cyclization differ substantially from KIEs predicted by transition state theory, which suggests that IVR in this reaction can be studied by conventional KIEs. Leakage of vibrational zero point energy (ZPE) into the reaction coordinate was probed by trajectories in which initial ZPE in the CH/CD stretching modes was reduced by 25%. This did not change the predicted KIEs. PMID:27281683

  2. 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

    International Nuclear Information System (INIS)

    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

  3. PAPIN: A FORTRAN-4 program to calculate cross section probability tables, Bondarenko and transmission self-shielding factors for fertile isotopes in the unresolved resonance region

    Science.gov (United States)

    Munoz-Cobos, J. G.

    1981-08-01

    A FORTRAN 4 code was 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 prescriptions for the unresolved resonance region. Monte-Carlo methods are utilized to generate ladders of resonance parameters in he unresolved resonance region, from average resonance parameters and their appropriate distribution functions. The neutron cross sections are calculated by the single level Breit-Wigner 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 was validated through extensive comparisons with several deterministic codes.

  4. 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

  5. Synergistic extraction of actinides : Part II. Tetra-and trivalent actinides

    International Nuclear Information System (INIS)

    A detailed discussion on the synergistic solvent extraction behaviour of tetra- and trivalent actinide ions is presented. Structural aspects of the natural donor adducts of the tetravalent actinide ion chelates involved in synergism are also discussed. (author)

  6. 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

  7. 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.

  8. Spin Hamiltonians for actinide ions

    International Nuclear Information System (INIS)

    The breakdown of Russel Saunders coupling for correlated f-levels of actinide ions is due to both spin orbit coupling and the crystalline electric field (CEF). Experiments on curium, an S-state ion in the metal for which the CEF is weak indicate a g-factor close to the Russel-Saunders value. Spin-orbit coupling is therefore too weak to produce jj coupling. This suggests a model for magnetic actinide ions in which the CEF ground multiplet is well separated from higher levels, completely determining thermodynamic magnetic properties. On this basis simplified spin Hamiltonians are derived for GAMMA1-GAMMA5 ground states in order to interpret thermodynamic measurements and ordering phenomena. (author)

  9. 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

  10. 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

  11. 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

  12. 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

  13. Actinides in earth materials: the importance of natural analogues

    International Nuclear Information System (INIS)

    Predictions of the stability of waste forms designed for long-term storage of actinides require an accurate knowledge of the long-term properties of these actinides in their host matrix. One useful approach to address this issue involves comparison of structural and thermodynamic information derived from short time-scale experiments on synthetic samples with similar information from natural samples, including natural glasses and metamict minerals. These natural analogues of synthetic waste forms, although significantly different in structure, properties and composition from the synthetic samples, offer a number of examples of earth materials that have received large doses of radioactivity (mainly α events) over very long time periods (106-109 years). In this paper, we present a review of the co-ordination chemistry of actinides in natural deep-seated earth systems and their analogues (mostly glasses, melts and radiation-damaged minerals). Special emphasis is given to data analysis methods that are important in determining accurate XAFS-derived interatomic distances and co-ordination numbers for actinides in these complex materials, including anharmonicity, multi-electronic transitions, deconvolution procedures, and ab initio calculations of near-edge structure. The effects of anharmonicity and multi-electronic transitions are best studied using high-energy resolution spectrometers on third-generation synchrotron sources. Application of these methods to selected natural minerals (crystalline and radiation-damaged) is presented, together with a comprehensive list of unusual mineral structures that are known to incorporate relatively large amounts of actinides over long periods of geologic time in a stable manner. (authors)

  14. 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)

  15. 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)

  16. 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)

  17. 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...

  18. 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)

  19. 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...

  20. 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)

  1. 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

  2. PWRs potentialities for minor actinides burning

    International Nuclear Information System (INIS)

    In the frame of the SPIN program at CEA, the impacts of the minor actinides (MA) incineration in PWRs are analysed. The aim is to reduce the mass, the potential radiotoxicity level. The recycling of all actinide elements is evaluated in a PWR nuclear yard. A sensitivity study is done to evaluate the incineration for each minor actinide element. This gives the most efficient way of incineration for each MA elements in a PWR and helps to design a PWR burner. This burner is disposed in a PWR nuclear system in which the actinides are recycled until equilibrium. (author)

  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. 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

  5. A measurement of actinide neutron transmutations with accelerator mass spectrometry in order to infer neutron capture cross sections

    Science.gov (United States)

    Bauder, William K.

    Improved neutron capture cross section data for transuranic and minor actinides are essential for assessing possibilities for next generation reactors and advanced fuel cycles. The Measurement of Actinide Neutron TRAnsmutation (MANTRA) project aims to make a comprehensive set of energy integrated neutron capture cross section measurements for all relevant isotopes from Th to Cf. The ability to extract these cross sections relies on the use of Accelerator Mass Spectrometry (AMS) to analyze isotopic concentrations in samples irradiated in the Advanced Test Reactor (ATR). The AMS measurements were performed at the Argonne Tandem Linear Accelerator System (ATLAS) and required a number of key technical developments to the ion source, accelerator, and detector setup. In particular, a laser ablation material injection system was developed at the electron cyclotron resonance ion source. This system provides a more effective method to produce ion beams from samples containing only 1% actinide material and offers some benefits for reducing cross talk in the source. A series of four actinide measurements are described in this dissertation. These measurements represent the most substantial AMS work attempted at ATLAS and the first results of the MANTRA project. Isotopic ratios for one and two neutron captures were measured in each sample with total uncertainties around 10%. These results can be combined with a MCNP model for the neutron fluence to infer actinide neutron capture cross sections.

  6. 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

  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. 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)

  9. Studies of actinides in a superanoxic fjord

    International Nuclear Information System (INIS)

    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 H2S 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 (232Th and 230Th) continues to increase. The flux of 232Th 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/m2/y. 208 refs

  10. 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.

  11. 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.

  12. 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...

  13. 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.

  14. Calculation of the Absorption Cross Sections of Some Molecules from GEISA Database at the Wavelengths of Isotopically Different CO2 Lasers

    OpenAIRE

    Asylkhan Rakhymzhan; Alexey Chichinin

    2013-01-01

    A calculation of the absorption cross section of some molecules (NH3, C2H4, CO2, O3, NO2, PH3, HNO3, SF6, CH3OH, HCOOH, OCS, CH3CN, C2H6, SO2, and H2O) at the wavelengths transmitted by a CO2 laser filled with different isotopes (12C16O2, 13C16O2, 12C18O2, 14C16O2, 14C18O2, 13C18O2, and 12C16O18O) is presented. The spectroscopical parameters for the molecules from GEISA database have been used. Hence the selection of the molecules was substantially based on the availability of the parameters ...

  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. Dynamics of H2 elimination from the methaniminium cation, [CH2NH2]+. Isotope effects, translational energy release, and molecular orbital calculations

    International Nuclear Information System (INIS)

    Various molecular orbital methods have been used to examine possible reaction mechanisms for the unimolecular decomposition [CH2NH2]+ → [HCNH]+ + H2. Measurements of deuterium isotope effects on the translational energy release indicate the nonequivalence of the two departing hydrogen atoms, as does the reported absence of hydrogen scrambling in the products of this decomposition. The semiempirical calculations and the ab initio calculations up to and including the 6-31G** level predict that the departing hydrogen atoms do become equivalent and indistinguishable and that there will be significant hydrogen scrambling. This paradox is resolved on the grounds that geometries corresponding to stationary points in these calculations would not be stationary were a degree of configuration interaction to be included. The overall conclusion reached is that the transition state for elimination for H2 from [CH2NH2]+ is an asymmetric nonplanar structure with a geometry not far distant from [CH3NH]+, which is not a stable minimum on the potential surface

  19. Sensitivity analysis for actinide production and depletion in fast reactors

    International Nuclear Information System (INIS)

    In sensitivity analysis of the actinide production and depletion in fast reactors, a mathematical method of calculating sensitivity coefficients is improved and simplified by combining the time-dependent generalized perturbation technique with the eigenvalue method. Numerical calculations show that the eigenvalue method is well applicable in solving the nuclide chain equation and its adjoint equation and the cylic chains in the decay scheme of the actinides can be interpreted by means of complex eigenvalues. The sensitivity coefficients of actinide production and depletion in a 1000 MWe fast reactor are strongly dependent on the type of Pu fuel used, i.e. Pu fuel from BWR or Pu fuel from the blanket of FBR. The sensitivity coefficients due to variations of capture cross sections, σsub(n,2n) of 238U, lambda sub(β) of 241Pu and lambda sub(α) of 242Cm are especially large. Sensitivity analyses for the 1000 MWe fast reactors show that higher priorily should be given to decay constants of 241Pu and 242Cm, capture cross sections of 237Np, 241Am, 243Am and 242Pu, and fission cross sections of 237Np, 242Pu, 241Am and sup(242m)Am. (author)

  20. 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

  1. MANTRA: Measuring Neutron Capture Cross Sections in Actinides with Accelerator Mass Spectrometry

    Science.gov (United States)

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

    2013-10-01

    With rising global energy needs, there is substantial interest in nuclear energy research. To explore possibilities for advanced fuel cycles, better neutron cross section data are needed for the minor actinides. The MANTRA (Measurement of Actinide Neutron TRAsmutation) project will improve these data by measuring integral (n, γ) cross sections. The cross sections will be extracted by measuring isotopic ratios in pure actinide samples, irradiated in the Advanced Test Reactor at Idaho National Lab, using Accelerator Mass Spectrometry(AMS) at the Argonne Tandem Linac Accelerator System (ATLAS). MANTRA presents a unique AMS challenge because of the goal to measure multiple isotopic ratios on a large number of samples. To meet these challenges, we have modified the AMS setup at ATLAS to include a laser ablation system for solid material injection into our ECR ion source. I will present work on the laser ablation system and modified source geometry, as well as preliminary measurements of unirradiated actinide samples at ATLAS. This work was supported by the U.S. Department of Energy, Office of Nuclear Physics, under Contract No. DE-AC02-06CH11357.

  2. Environmental chemistry of the actinide elements

    International Nuclear Information System (INIS)

    The environmental chemistry of the actinide elements is a new branch of science developing with the application of nuclear energy on a larger and larger scale. Various aspects of the environmental chemistry of the actinide elements are briefly reviewed in this paper, such as its significance in the nuclear waste disposal, its coverage of research fields and possible directions for future study

  3. 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.

  4. 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

  5. Experimental level-structure determination in odd-odd actinide nuclei

    International Nuclear Information System (INIS)

    The status of experimental determination of level structure in odd-odd actinide nuclei is reviewed. A technique for modeling quasiparticle excitation energies and rotational parameters in odd-odd deformed nuclei is applied to actinide species where new experimental data have been obtained by use of neutron-capture gamma-ray spectroscopy. The input parameters required for the calculation are derived from empirical data on single-particle excitations in neighboring odd-mass nuclei. Calculated configuration-specific values for the Gallagher-Moszkowski splittings are used. Calculated and experimental level structures for 238Np, 244Am, and 250Bk are compared, as well as those for several nuclei in the rare-earth region. The agreement for the actinide species is excellent, with bandhead energies deviating 22 keV and rotational parameters 5%, on the average. Applications of this modeling technique are discussed

  6. 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

  7. 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)

  8. 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.

  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. Factors influencing the transport of actinides in the groundwater environment. Final report

    International Nuclear Information System (INIS)

    This report summarizes investigations of factors that significantly influence the transport of actinide cations in the groundwater environment. Briefly, measurements of diffusion coefficients for Am(III), Cm(III), and Np(V) in moist US soils indicated that diffusion is negligible compared to mass transport in flowing groundwater. Diffusion coefficients do, however, indicate that, in the absence of flowing water, actinide elements will migrate only a few centimeters in a thousand years. The remaining investigations were devoted to the determination of distribution ratios (K/sub d/s) for representative US soils, factors influencing them, and chemical and physical processes related to transport of actinides in groundwaters. The computer code GARD was modified to include complex formation to test the importance of humic acid complexing on the rate of transport of actinides in groundwaters. Use of the formation constant and a range of humic acid, even at rather low concentrations of 10-5 to 10-6 molar, significantly increases the actinide transport rate in a flowing aquifer. These computer calculations show that any strong complexing agent will have a similar effect on actinide transport in the groundwater environment. 32 references, 9 figures

  13. 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

  14. MGA, Pu Isotope Abundance from Multichannel Analyzer Gamma Spectra

    International Nuclear Information System (INIS)

    1 - Description of program or function: The MGA (Multiple Group Analysis) program determines the relative abundances of plutonium and other actinide isotopes in different materials. The program analyzes spectra taken of such samples using a 4096-channel germanium (Ge) gamma-ray spectrometer. The code can be run in a one or two detector mode. The first spectrum which is required and must be taken at a gain of .075 keV/channel with a high resolution planar detector, contains the 0-300 keV energy region. The second spectrum, which is optional, must be taken at a gain of 0.25 keV/channel; it becomes important when analyzing high burnup samples (concentration of Pu(241) greater than one percent). Isotopic analysis precision of one percent or better can be obtained, and no calibrations are required. The system also measures the abundances of U(235,238), Np-237, and Am-241. A special calibration option is available to perform a one-time peak-shape characterization when first using a new detector system. 2 - Method of solution: The basic method for determining the relative abundance of the isotopes of plutonium is to measure the intensity of two or more peaks from gamma rays of similar energy, but arising from different isotopes. Since the gamma-ray emission probabilities and half-lives are known, the atom ratios can be calculated provided relative detection efficiencies for the peaks can be estimated

  15. 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

  16. Fast neutron scattering on actinide nuclei

    International Nuclear Information System (INIS)

    More and more sophisticated neutron experiments have been carried out with better samples in several laboratories and it was necessary to intercompare them. In this respect, let us quote for example (n,n'e) and (n,n'#betta#) measurements. Moreover, high precision (p,p), (p,p') and (p,n) measurements have been made, thus supplementing neutron experiments in the determination of the parameters of the optical model, still widely used to describe the neutron-nucleus interaction. The optical model plays a major role and it is therefore essential to know it well. The spherical optical model is still very useful, especially because of its simplicity and of the relatively short calculation times, but is obviously insufficient to treat deformed nuclei such as actinides. For accurate calculations about these nuclei, it is necessary to use a deformed potential well and solve a set of coupled equations, hence long computational times. The importance of compound nucleus formation at low energy requires also a good knowledge of the statistical model together with that of all the reaction mechanisms which are involved, including fission for which an accurate barrier is necessary and, of course, well-adjusted level densities. The considerations form the background of the Scientific Programme set up by a Programme Committee whose composition is given further on in this book

  17. 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.

  18. 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.

  19. 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...

  20. 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

  1. 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

  2. LSDS Development for Isotopic Fissile Content Assay

    International Nuclear Information System (INIS)

    Concerning the sustainable energy supply and green house effect, nuclear energy became the most feasible option to meet the energy demand in Korea. However, the production of the spent nuclear fuel is the inevitable situation. Since the first nuclear power plant started to produce the electricity in Korea, the accumulated amount of spent fuels exceeded 10k tomes recently. The accumulation of the spent fuels is the big issue in the society. Therefore, as an option which strengthens the nuclear proliferation resistance and reduces the amount of spent fuels, sodium fast reactor (SFR) program linked with pyro-processing is under development to re-use the PWR spent fuel and produce the energy. In the process, the produced metallic material involves uranium and TRU (transuranic; neptunium, plutonium, and americium). The uranium-TRU is used to fabricate SFR fuel. The burning the recycled fuel in the reactor is to solve the current spent fuel storage problem and to minimize the actinides accumulation having long half-life. Generally, the spent fuel from PWR has unburned ∼1 % U235, produced ∼0.5 % plutonium from decay chain, ∼3 % fission products, ∼ 0.1 % minor actinides (MA) and uranium remainder. About 1.5 % fissile materials still exist in the spent fuel. Therefore, spent fuel is not only waste but energy resource. The direct and isotopic fissile content assay is the crucial technology for the spent fuel reuse. Additionally, the fissile content analysis will contribute to the optimum storage design and safe spent fuel management. Several nondestructive technologies have been developed for the spent fuel assay; gamma ray measurement, passive and active neutron measurements. Spent fuel emits intense gamma rays and neutrons by (a, n) and spontaneous fission. This intense background has the limitation on the direct analysis of fissile materials. Recently, to analyze the individual fissile content, leadslowing down spectrometer (LSDS) has been being developed in Korea

  3. 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

  4. 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.

  5. 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

  6. 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

  7. Physical mechanism analysis of burnup actinide composition in light water reactor MOX fuel and its application to uncertainty evaluation

    International Nuclear Information System (INIS)

    Highlights: • We discuss physical mechanisms for burnup actinide compositions in LWR’s MOX fuel. • Mechanisms of 244Cm and 238Pu productions are analyzed in detail with sensitivity. • We can evaluate the indirect effect on actinide productions by nuclear reactions. • Burnup sensitivity is applied to uncertainty evaluation of nuclide production. • Actinides can be categorized into patterns according to a burnup sensitivity trend. - Abstract: In designing radioactive waste management and decommissioning facilities, understanding the physical mechanisms for burnup actinide composition is indispensable to satisfy requirements for its validity and reliability. Therefore, the uncertainty associated with physical quantities, such as nuclear data, needs to be quantitatively analyzed. The present paper illustrates an analysis methodology to investigate the physical mechanisms of burnup actinide composition with nuclear-data sensitivity based on the generalized depletion perturbation theory. The target in this paper is the MOX fuel of the light water reactor. We start with the discussion of the basic physical mechanisms for burnup actinide compositions using the reaction-rate flow chart on the burnup chain. After that, the physical mechanisms of the productions of Cm-244 and Pu-238 are analyzed in detail with burnup sensitivity calculation. Conclusively, we can identify the source of actinide productions and evaluate the indirect influence of the nuclear reactions if the physical mechanisms of burnup actinide composition are analyzed using the reaction-rate flow chart on the burnup chain and burnup sensitivity calculation. Finally, we demonstrate the usefulness of the burnup sensitivity coefficients in an application to determine the priority of accuracy improvement in nuclear data in combination with the covariance of the nuclear data. In addition, the target actinides and reactions are categorized into patterns according to a sensitivity trend

  8. 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

  9. 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.

  10. 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

  11. Actinide chemistry in the far field

    International Nuclear Information System (INIS)

    The environmental chemistry of the actinides is complicated due both to the extensive redox and coordination chemistry of the elements and also to the complexity of the reactive phases encountered in natural environments. In the far field, interactions with reactive surfaces, coatings and colloidal particles will play a crucial role in controlling actinide mobility. By virtue of both their abundance and reactivity; clays and other layer aluminosilicate minerals, hydrous oxides and organic matter (humic substances) are all identified as having the potential to react with actinide ions and some possible modes of interaction are described, together with experimental evidence for their occurrence. (author)

  12. 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

  13. Determination of artifactual formation of monomethylmercury (CH{sub 3}Hg{sup +}) in environmental samples using stable Hg{sup 2+} isotopes with ICP-MS detection: Calculation of contents applying species specific isotope addition

    Energy Technology Data Exchange (ETDEWEB)

    Hintelmann, H. [Trent University, Environmental Science Centre, Peterborough ON K9J 7B8 (Canada); Falter, R. [Bayreuth Institute for Terrestrial Ecosystem Research (BITOEK), Central Analytics, POB 101251, University of Bayreuth, D-95440 Bayreuth (Germany); Ilgen, G. [Bayreuth Institute for Terrestrial Ecosystem Research (BITOEK), Central Analytics, POB 101251, University of Bayreuth, D-95440 Bayreuth (Germany); Evans, R.D. [Trent University, Environmental Science Centre, Peterborough ON K9J 7B8 (Canada)

    1997-06-01

    Various extraction techniques, as distillation, acid and alkaline extraction, have been tested with regard to their potential to form a monomethylmercury (CH{sub 3}Hg{sup +}) artifact from inorganic Hg during sample preparation. Hg{sup 2+} has been added to different reference materials in the form of enriched stable tracers and the formation of new methylmercury from that tracer has been analyzed by HPLC/ICP-MS and GC/ICP-MS. Both techniques gave comparable results. In particular, the distillation technique was prone to artifact formation. The resulting overestimation of methylmercury in sediments was as high as 80%. Artifact formation in hair, liver and algae samples was less significant, though still observable. Fish muscle tissue showed no artifact formation upon distillation, but some of the inorganic tracer was converted to methylmercury during alkaline extraction. Acid extraction of sediments resulted in low artifact formation rates. Fractionated measurements of sediment distillates revealed high methylmercury formation rates towards the end of the distillation process when acid concentrations in the solution are highest. A technique for correction of the measured apparent methylmercury content applying species specific isotope addition (SSIA) is proposed and the calculation scheme is presented. (orig.). With 6 figs., 3 tabs.

  14. Endohedral Fullerenes with Actinide-Actinide Bonds: Unwilling Bonding in U2@C80

    Czech Academy of Sciences Publication Activity Database

    Foroutan-Nejad, C.; Patzschke, M.; Straka, Michal

    Opole: -, 2014. [MMNB 2014. Polish-Taiwanese Conference. From Molecular Modeling to Nano- and Biotechnology . 04.09.2014-06.09.2014, Opole] R&D Projects: GA ČR(CZ) GA14-03564S Grant ostatní: European Social Fund(XE) CZ.1.07/2.3.00/30.009 Institutional support: RVO:61388963 Keywords : endohedral actinide fullerene * U-U bonding * actinide-actinide bonding Subject RIV: CF - Physical ; Theoretical Chemistry

  15. 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)

  16. 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....

  17. 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

  18. Multi-nucleon transfer experiments in the actinide region

    Energy Technology Data Exchange (ETDEWEB)

    Geibel, Kerstin; Reiter, Peter; Birkenbach, Benedikt [Institut fuer Kernphysik, Universitaet zu Koeln (Germany); Valiente-Dobon, Jose Javier; Recchia, Francesco [Istituto Nazionale di Fisica Nucleare, Laboratori Nazionali di Legnaro (Italy); Gadea, Andres [IFIC, CSIC-Universidad de Valencia (Spain); Lenzi, Silvia [Dipartimento di Fisica, University of Padova (Italy)

    2012-07-01

    Two experiments at the PRISMA-CLARA-Setup at the LNL in Legnaro were analysed focussing on the target-like reaction products in the actinide region after multi-nucleon transfer reactions. Both experiments use {sup 238}U as target; a {sup 70}Zn-beam with 460 MeV and a {sup 136}Xe-beam with 926 MeV were employed. Kinematic correlations between the reaction partners are used to obtain information about the unobserved target-like reaction products by the analysis of the beam-like particles identified with the PRISMA-spectrometer. Clean {gamma}-spectra from neutron-rich actinide nuclei are obtained with the CLARA-array. An extension of the ground state rotational band in {sup 240}U and insights in neutron-rich Th-isotopes were achieved. Based on relative cross section distributions for various reaction channels the perspectives and limitations for in-beam {gamma}-spectroscopy with this experimental method in this mass region are discussed.

  19. 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, the way how bioremediation controls the fate of actinides is assessed. 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. The way 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 is described. Why inhibition caused by chemical or radiolytic toxicities uniquely affects microbial reactions is explained. 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. Development of mathematical models that link microbiological and geochemical reactions is described. Throughout, the key research needs are identified. (author)

  20. 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.

  1. 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

  2. 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

  3. 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

  4. Magnetic form factor studies of actinide compounds

    International Nuclear Information System (INIS)

    Some results obtained at ILL on Actinide compound form factors are reviewed. In the paramagnetic NpO2 single crystal (5mg), an induced magnetic moment of 0.07μsub(B) was obtained at 4.2K (4.6T). In the ferromagnetic phase of NpAs2 single crystal (0.2mm3), the magnetic moment (1.46μsub(B)/Np atom) has been found fixed along the [001] direction. In both cases, the Np form factors fit satisfactorily the Np4+ form factor calculated with relativistic atomic wave functions. The Fermi length for Np was deduced (b(Np) = 1.015(15)10-12cm). In the paramagnetic Laves phase UNi2 compound, equally small moments are observed on U atom (0.013(1)μsub(B)) and on Ni atom (0.016(1)μsub(B)) confirming important changes in 3d band structure of Ni by hybridization with U electrons

  5. 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)

  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. 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

  9. PWRs potentialities for minor actinides burning

    International Nuclear Information System (INIS)

    In the frame of the SPIN program at CEA, the impacts of the Minor Actinides (MA) incineration in PWRs are analysed. The aim is to reduce the mass and the potential radiotoxicity level. This study is done separately one on the Plutonium recycling. But the plutonium is essential. Thus, the recycling of all Actinide elements is evaluated in a PWR nuclear yard. A sensitivity study is done to evaluate the incineration for each Minor Actinide element. This gives us the most efficient way of incineration for each MA element in a PWR and help us to design a PWR burner. This burner is disposed in a PWR nuclear system in which the Actinides are recycled until equilibrium. (authors). 2 refs

  10. 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.

  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. 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).

  13. 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.

  14. 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.)

  15. 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...

  16. New molecules to separate actinides: the picolinamides

    International Nuclear Information System (INIS)

    The reprocessing of spent fuel is made with the Purex process, funded on liquid-liquid extraction of uranium nitrates(VI) and plutonium nitrates(IV) by the BTP (tributyl phosphate). To improve this proceeding, we look for extractants which allow, beyond U and Pu extractions, these of actinides (II) and allow separation of the whole actinides from the fission products, which have an important fraction of lanthanides. A new family seems to give good results: the picolinamides

  17. 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.)

  18. Lattice effects in the light actinides

    International Nuclear Information System (INIS)

    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

  19. 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...

  20. 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)

  1. 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

  2. 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

  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. 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

  5. Study of crystalline actinide waste forms produced by self-propagating high-temperature synthesis

    International Nuclear Information System (INIS)

    Prospective matrices for a safe immobilisation of long-lived actinide-bearing wastes were produced by self-propagating high-temperature synthesis. The samples were examined using XRD, SEM/EDS, and TEM. The data show that the ceramics consist of oxide phases with a fluorite- or pyrochlore-type structure and also metallic Mo. The structural properties of the target actinide-loaded host phase depend primarily on the composition of the immobilised waste. It is suggested that for streams enriched with tetravalent actinides having relatively small dimension of the cations: U4+ (0.10 nm), Np4+ (0.098 nm), and Pu4+ (0.096 nm), a cubic fluorite-structured ZrO2-based solid solution can be used to fix the waste, whereas titanates or zirconates with a pyrochlore-type lattice are well suited for wastes containing large amounts of the bulkier ions of trivalent actinides (Pu3+, Am3+) and lanthanides (Nd, Ce, La, Pr). Among other elements which can be located into the octahedral sites of the pyrochlore lattice, Tc4+ with a radius of 0.065 nm is worth mentioning. Long-lived 99Tc is produced during 235U fission events. Due to a high hazard associated with this isotope, it should also be fixed in highly durable matrices such as pyrochlore

  6. 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

  7. Calculations of different transmutation concepts. An international benchmark exercise

    International Nuclear Information System (INIS)

    In April 1996, the NEA Nuclear Science Committee (NSC) Expert Group on Physics Aspects of Different Transmutation Concepts launched a benchmark exercise to compare different transmutation concepts based on pressurised water reactors (PWRs), fast reactors, and an accelerator-driven system. The aim was to investigate the physics of complex fuel cycles involving reprocessing of spent PWR reactor fuel and its subsequent reuse in different reactor types. The objective was also to compare the calculated activities for individual isotopes as a function of time for different plutonium and minor actinide transmutation scenarios in different reactor systems. This report gives the analysis of results of the 15 solutions provided by the participants: six for the PWRs, six for the fast reactor and three for the accelerator case. Various computer codes and nuclear data libraries were applied. (author)

  8. 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

  9. 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...

  10. FY2011 Annual Report for the Actinide Isomer Detection Project

    Energy Technology Data Exchange (ETDEWEB)

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

    2011-10-01

    This project seeks to identify a new signature for actinide element detection in active interrogation. This technique works by exciting and identifying long-lived nuclear excited states (isomers) in the actinide isotopes and/or primary fission products. Observation of isomers in the fission products will provide a signature for fissile material. For the actinide isomers, the decay time and energy of the isomeric state is unique to a particular isotope, providing an unambiguous signature for SNM. This project entails isomer identification and characterization and neutron population studies. This document summarizes activities from its third year - completion of the isomer identification characterization experiments and initialization of the neutron population experiments. The population and decay of the isomeric state in 235U remain elusive, although a number of candidate gamma rays have been identified. In the course of the experiments, a number of fission fragment isomers were populated and measured [Ressler 2010]. The decays from these isomers may also provide a suitable signature for the presence of fissile material. Several measurements were conducted throughout this project. This report focuses on the results of an experiment conducted collaboratively by PNNL, LLNL and LBNL in December 2010 at LBNL. The measurement involved measuring the gamma-rays emitted from an HEU target when bombarded with 11 MeV neutrons. This report discussed the analysis and resulting conclusions from those measurements. There was one strong candidate, at 1204 keV, of an isomeric signature of 235U. The half-life of the state is estimated to be 9.3 {mu}s. The measured time dependence fits the decay time structure very well. Other possible explanations for the 1204-keV state were investigated, but they could not explain the gamma ray. Unfortunately, the relatively limited statistics of the measurement limit, and the lack of understanding of some of the systematic of the experiment, limit

  11. A method of the sensitivity analysis of build-up and decay of actinides

    International Nuclear Information System (INIS)

    To make sensitivity analysis of build-up and decay of actinides, mathematical methods related to this problem have been investigated in detail. Application of time-dependent perturbation technique and Bateman method to sensitivity analysis is mainly studied. For the purpose, a basic equation and its adjoint equation for build-up and decay of actinides are systematically solved by introducing Laplace and modified Laplace transforms and their convolution theorems. Then, the mathematical method of sensitivity analyses is formulated by the above technique; its physical significance is also discussed. Finally, application of eigenvalue-method is investigated. Sensitivity coefficients can be directly calculated by this method. (auth.)

  12. 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

  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. Consideration of uncertain nuclear data in the computation of the reduction of waste actinides by irradiation

    International Nuclear Information System (INIS)

    The most promising physical measure for quantity reduction of long-lived radiation sources and thus for the reduction of long-term risks at the ultimate store is further irradiation of the waste actinide nuclides in the neutron field of the reactor. In order to determine whether the nuclear data base now available on waste actinides (neptunium 237, plutonium 238, americium 241, americium 242, and americium 243) allows even now the actual design of reactors for further irradiation of such actinides, burn-up calculations must be made taking into consideration the uncertain character of nuclear data. For this purpose, an improved method for the computation of error propagation had to be elaborated. (orig./DG)

  15. Studies on fluoride complexing of hexavalent actinides using a fluoride ion selective electrode

    International Nuclear Information System (INIS)

    Complex formation between actinide(VI) and fluoride ions in aqueous solutions was investigated using a fluoride ion selective electrode (F-ISE). As fairly high acidity used to suppress hydrolysis of the actinide(VI) ions, significant liquid junction potentials (Esub(j)) existed in the system. An iterative procedure was developed for computing free hydrogen ion concentration [Hsup(+)] as it colud not be measured directly, using data obtained with F-ISE. Esub(j) values were estimated from known [Hsup(+)] and the stability constants of fluoride complexes of actinide(VI) ions were calculated following King and Gallagher's method using a computer program. The stability constants were found to follow the order U(VI)>Np(VI)>Pu(VI). (author)

  16. Build-Up Of Actinides In Irradiated Fuel Rods Of The ETRR-1 Reactor

    International Nuclear Information System (INIS)

    The content concentrations of actinides are calculated as a function of operating reactor regime and cooling time at different percentage of fuel burn-up. The build-up transmutation equations of actinides content in an irradiated fuel are solved numerically .A computer code BAC was written to operate on PC computer to provide the required calculations. The fuel element of 10% 235U enrichment of ETRR-1 reactor was taken as an example for calculations using BAC code. The results are compared with other calculations for the ETRR-1 fuel rod. An estimation of fissile build-up content of a proposed new fuel of 20% '235U enrichment for ETRR-1 reactor is given. The sensitivity coefficients of build-up plutonium concentrations as a function of cross-section data uncertainties are also calculated

  17. Build up of actinides in burnt fuel rods of the ET-RR-1 reactor

    International Nuclear Information System (INIS)

    The content concentrations of actinides are calculated as a function of operating reactor regime and cooling time at different percentage of fuel burn-up. The build-up transmutation equations of actinides content in an irradiated fuel are solved numerically .A computer code BAC was written to operate on a PC computer to provide the required calculations. The fuel element of 10% 235U enrichment of ET-RR-1 reactor was taken as an example for calculations using the BAC code. The results are compared with other calculations for the ET-RR-1 fuel rod. An estimation of fissile build-up content of a proposed new fuel of 20% 235U enrichment for ET-RR-1 reactor is given. The sensitivity coefficients of build-up plutonium concentrations as a function of cross-section data uncertainties are also calculated. (author)

  18. Investigation on the application of the isotopic correlation technique in post-irradiation analysis and safeguards

    International Nuclear Information System (INIS)

    An extensive analysis of irradiated fuel shows that the theoretical prediction of isotopic ratios for actinides in PWRs is very satisfactory. Comparisons of theoretical results with those from post-irradiation measurements demonstrate the capability of the used data and methods: all calculated values are within the range of the interlaboratory deviations. Sensitivities for a variety of isotopic ratios on reactor parameters as burn-up, enrichment, boron concentration, fuel-to-moderator-ratio, etc. have been calculated. On the basis of these sensitivity studies, a recipe has been worked out how to apply the isotopic correlation techniques to safeguarding fissile material. The capability of this recipe is demonstrated for realistic situations. The essential characteristic of the proposed method lies in the application of several (e.g. six) selectively sensitive (with respect to the reactor parameters) isotopic correlations. Theory is used as a verified tool in deciding on erroneous measurements, accidental or intentional fuel substitution or diversion. The proposed recipe is verified with simulated as well as with realistic, actually observed examples. (orig.)

  19. 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.

  20. Radioecology of the actinide elements

    International Nuclear Information System (INIS)

    Research progress is reported in sections entitled: scope of studies supported by the Department of Energy; oxidation state diagrams are a potential tool for studying the redox chemistry of Pu in natural waters; studies are initiated to investigate the effect of pH and organic matter on the distribution coefficients of Cm with natural sediments; the relative distributions of resuspended and direct deposited Pu in a corn canopy are quantified; the retention of Pu surface contamination by corn plants is being studied; Pu concentrations in tobacco are being determined; concentrations of Pu per unit mass and per unit surface area are compared for subterranean crops; models of Pu behavior in agricultural crops are being validated; distribution of aerially released Pu in loblolly pine plantations is independent of deposition rate; investigation of the effects of chelate and redox potential of the uptake of Pu and Cm by rice is underway; studies of Cm cycling in a floodplain forest have been initiated; the effects of unusually large Pu deposition onto a wheat ecosystem are being studied using computer simulations; long-term kinetic models of Pu behavior in plant-soil systems are being developed; scope of studies supported by the Nuclear Regulatory Commission; growth form of broadleaf crop may affect Pu contents; root uptake of Pu and Cm measured for rice root uptake of Pu and Cm measured for rice; long-term actinide uptake study is continuing at SREL; and uranium cycling in major southeastern agricultural crops being studied

  1. Actinide transmutation in nuclear reactors

    International Nuclear Information System (INIS)

    An optimization method is developed to maximize the burning capability of the ALMR while complying with all constraints imposed on the design for reliability and safety. This method leads to a maximal transuranics enrichment, which is being limited by constraints on reactivity. The enrichment can be raised by using the neutrons less efficiently by increasing leakage from the fuel. With the developed optimization method, a metallic and an oxide fueled ALMR were optimized. Both reactors perform equally well considering the burning of transuranics. However, metallic fuel has a much higher heat conductivity coefficient, which in general leads to better safety characteristics. In search of a more effective waste transmuter, a modified Molten Salt Reactor was designed. A MSR operates on a liquid fuel salt which makes continuous refueling possible, eliminating the issue of the burnup reactivity loss. Also, a prompt negative reactivity feedback is possible for an overmoderated reactor design, even when the Doppler coefficient is positive, due to the fuel expansion with fuel temperature increase. Furthermore, the molten salt fuel can be reprocessed based on a reduction process which is not sensitive to the short-lived spontaneously fissioning actinides. (orig./HP)

  2. Burnup credit calculations on long-term disposal

    International Nuclear Information System (INIS)

    One of the considered options for handling of irradiated nuclear fuel is the final disposal in some kind of repository. This necessitates the long-term investigation of subcriticality, heat production, public dose etc. NEA WPNCS Burnup Credit Expert Group defined a new benchmark to test the codes and data used for such problems. The effect of cooling time should be investigated. This implies that the decay data and not the cross sections influence the results. Composition of 4.5 % UO2 fuel with 50 MWd/kgU is given at the assembly removal from the core. Change of composition should be evaluated for 30 values of cooling time up to 1 million years. Keff should be evaluated with these compositions for a container housing 21 fuel assemblies. Initial concentration of 115 isotopes is given. For criticality calculations the usual 'burnup credit set' is used (14 actinides and 15 fission products). Results for additional isotopes is not presented now. The investigated fuel is 17 x 17 PWR UO2 type, with 25 guide tubes. The selected cooling times covers the time intervals of the usual handling procedures around the reactors (few years storing in storage pool, transport), interim storage (hundred years), and the long time scale of disposal up to 1 million years. Results: 1) For major actinides, ORIGEN and MULTICELL based keff results are practically identical up to 1000 years, far beyond the cooling times it was intended. 2) For actinides and fission products, the agreement is excellent up to 100 years, which covers the interim storage. 3) The difference of keff results about 0.02 at 1000 years. The reason is mainly the presence of Np-237, not considered in the previous case. It is produced from Am-241 by α-decay (432 years). Compositions calculated by ORIGEN and TIBSO results the same keff values for cooling times up to 1 million years. Changes in keff with cooling time have clear physical explanation. Compositions calculated by ORIGEN and MULTICELL results the same keff

  3. 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)

  4. Online oxygen kinetic isotope effects using membrane inlet mass spectrometry can differentiate between oxidases for mechanistic studies and calculation of their contributions to oxygen consumption in whole tissues.

    Science.gov (United States)

    Cheah, Mun Hon; Millar, A Harvey; Myers, Ruth C; Day, David A; Roth, Justine; Hillier, Warwick; Badger, Murray R

    2014-05-20

    The reduction chemistry of molecular oxygen underpins the energy metabolism of multicellular organisms, liberating free energy needed to catalyze a plethora of enzymatic reactions. Measuring the isotope signatures of (16)O and (18)O during O2 reduction can provide insights into both kinetic and equilibrium isotope effects. However, current methods to measure O2 isotope signatures are time-consuming and disruptive. This paper describes the application of membrane inlet mass spectrometry to determine the oxygen isotope discrimination of a range of O2-consuming reactions, providing a rapid and convenient method for determining these values. A survey of oxygenase and oxidase reactions provides new insights into previously uncharacterized amino acid oxidase enzymes. Liquid and gas phase measurements show the ease of assays using this approach for purified enzymes, biological extracts and intact tissues. PMID:24786640

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

    International Nuclear Information System (INIS)

    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 235U, 238U, 239Pu and 241Pu, to be used in quick LWR reactor accident decay heat calculation tools. (authors)

  6. 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

  7. 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.

  8. 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

  9. 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.

  10. Taking into account absorbed doses in tooth enamel due to internal irradiation of human body by radioactive cesium isotopes at analysis EPR dosimetry data: Calculation by Monte-Carlo method

    Energy Technology Data Exchange (ETDEWEB)

    Borysheva, N. [Medical Radiological Research Center, Korolyov str., 4, Obninsk 249020 (Russian Federation); Ivannikov, A. [Medical Radiological Research Center, Korolyov str., 4, Obninsk 249020 (Russian Federation)], E-mail: Ivannikov-Alexander@yandex.ru; Tikunov, D.; Orlenko, S.; Skvortsov, V.; Stepanenko, V. [Medical Radiological Research Center, Korolyov str., 4, Obninsk 249020 (Russian Federation); Hoshi, M. [Research Institute for Radiation Biology and Medicine, Hiroshima University, 1-2-3 Kasumi, Minami-ku, Hiroshima 734-8553 (Japan)

    2007-07-15

    By Monte-Carlo simulation of ionizing particles transport, for a realistic mathematical phantom of a man supplemented by a dental region, absorbed doses in teeth enamel and whole body doses are calculated for cases of internal irradiation by {sup 137}Cs and {sup 134}Cs isotopes incorporated in the human body resulted from staying in radioactive contaminated territory. It is shown that dose in enamel constitutes (40{+-}4)% and (59{+-}6)% of whole body dose resulted from the decay of {sup 137}Cs and {sup 134}Cs isotopes, respectively. The results of calculations may be used for conversion of absorbed dose in enamel obtained by the tooth enamel EPR spectroscopy method to whole body dose for dosimetric investigation of population of territories contaminated by the radioactive cesium, which is specific for the Chernobyl accident.

  11. New reagents for actinide-lanthanide group separations

    International Nuclear Information System (INIS)

    Organic extractants which possess nitrogen or sulfur donor atoms preferentially complex the trivalent actinide. They are potential reagents for actinide lanthanide group separations, which can be performed at low pH without the addition of inorganic salts

  12. 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

  13. 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

  14. 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.

  15. Spent nuclear fuel corrosion: The application of ICP-MS to direct actinide analysis

    International Nuclear Information System (INIS)

    The ICP-MS technique has been applied to the analysis of the actinide contents of corrodant solutions from experiments performed to study the corrosion of spent nuclear fuel in simulated groundwaters. Analysis was performed directly on the solutions, without employing separation or isotope dilution techniques. The results from two analytical campaigns using natural indium and thorium internal standards are compared. Under both oxic and anoxic conditions, the U contents can be determined with good accuracy and precision. The same applies to Np and Pu under oxic conditions, where the solution concentrations range down to about 0.1 ppb. Under anoxic conditions, where solution concentrations are lower by one or two orders of magnitude, reasonable results for these two actinides can be obtained, but with much lower precision. Direct analysis of Am and Cm, however, gave unsatisfactory results, since the technique is limited by poor measurement statistics and background uncertainty

  16. Strontium and Actinides Removal from Savannah River Site Actual Waste Samples by Freshly Precipitated Manganese Oxide

    International Nuclear Information System (INIS)

    The authors investigated the performance of freshly precipitated manganese oxide and monosodium titanate (MST) for the removal of strontium (Sr) and actinides from actual high-level waste. Manganese oxide precipitation occurs upon addition of a reductant such as formate (HCO2-) or peroxide (H2O2) to a waste solution containing permanganate (MnO4-). An addition of non-radioactive strontium typically precedes the MnO4- and reductant addition, which serves primarily to isotopically dilute the strontium-90 (90Sr) present in the waste. Tests utilized a Tank 37H/44F composite waste solution. Personnel significantly increased the concentration of actinides in the waste by the addition of acidic americium/curium solution (F-Canyon Tank 17.1 solution), which contained a significant quantity of plutonium (Pu), and neptunium-237 (237Np) stock solution. Initial tests examined three manganese oxide treatment options

  17. Denaturing of plutonium by transmutation of minor-actinides for enhancement of proliferation resistance

    International Nuclear Information System (INIS)

    Feasibility study for the plutonium denaturing by utilizing minor-actinide transmutation in light water reactors has been performed. And the intrinsic feature of proliferation resistance of plutonium has been discussed based on IAEA's publication and Kessler's proposal. The analytical results show that not only 238Pu but also other plutonium isotopes with even-mass-number have very important role for denaturing of plutonium due to their relatively large critical mass and noticeably high spontaneous fission neutron generation. With the change of the minor-actinide doping ratio in U-Pu mix oxide fuel and moderator to fuel ratio, it is found that the reactor-grade plutonium from conventional light water reactors can be denatured to satisfy the proliferation resistance criterion based on the Kessler's proposal but not to be sufficient for the criterion based on IAEA's publication. It has been also confirmed that all the safety coefficients take negative value throughout the irradiation. (author)

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

    International Nuclear Information System (INIS)

    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.

  19. 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.

  20. 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)

  1. Separation of actinides with alkylpyridinium salts

    International Nuclear Information System (INIS)

    Various f-elements are separated as anionic complexes from both acidic and alkaline solutions by precipitation with alkylpyridinium salts. The precipitates are also cationic surfactants where the simple counter-ion (e.g. nitrate or chloride) is replaced by the negatively charged complex anion of an actinide or lanthanide. The low solubility of these precipitates is explained by a strong affinity of divalent complex counter-ions of f-elements to the quaternary nitrogen. Precipitations in solutions of nitric acid allow to separate tetravalent f-elements from other metals, in alkaline carbonate solutions tetravalent and hexavalent actinides are precipitated simultaneously. The last procedure yields precipitates, which are very intimate mixtures of hexavalent and tetravalent actinides. This allows to prepare mixed oxides in a simple way. (author) 6 refs.; 3 figs.; 3 tabs

  2. Neutron scattering studies of the actinides

    International Nuclear Information System (INIS)

    The electronic structure of actinide materials presents a unique example of the interplay between localized and band electrons. Together with a variety of other techniques, especially magnetization and the Mossbauer effect, neutron studies have helped us to understand the systematics of many actinide compounds that order magnetically. A direct consequence of the localization of 5f electrons is the spin-orbit coupling and subsequent spin-lattice interaction that often leads to strongly anisotropic behavior. The unusual phase transition in UO2, for example, arises from interactions between quadrupole moments. On the other hand, in the monopnictides and monochalcogenides, the anisotropy is more difficult to understand, but probably involves an interaction between actinide and anion wave functions. A variety of neutron experiments, including form-factor studies, critical scattering and measurements of the elementary excitations have now been performed, and the conceptual picture emerging from these studies will be discussed

  3. 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

  4. 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)

  5. 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)

  6. On a fast reactor cycle scheme that incorporates a thoria-based minor actinide-containing cermet fuel

    International Nuclear Information System (INIS)

    A fast reactor cycle scheme that incorporates a thoria-based minor actinide-containing cermet fuel is given. The present cermet fuel consists of an oxide solid solution of Th and minor actinides and Mo-inert matrix. It has been proposed as a high-performance device that can enhance minor actinide incineration in a fast reactor cycle. It is used in an independent small sub-cycle, whereby dedicated cycle technologies are adopted. Two-step reprocessing process was proposed for the present cermet fuel; it consists of a pre-removal of Mo-inert matrix and an actinide recovery. A preliminary test for the pre-removal of Mo-inert matrix was carried out using a surrogate cermet fuel. Burnup characteristics of a fast reactor core loaded with the cermet fuel were investigated by using neutronic calculation codes. It was revealed that a heterogeneous composition of Mo-inert in inner and outer cores may lead to an effective transmutation of minor actinides and a flattered power density. It was concluded that the present cermet fuel was potentially promising as a high-performance incineration device of minor actinides for fast reactors. (author)

  7. 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.

  8. 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

  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

    Energy Technology Data Exchange (ETDEWEB)

    Bagus, Paul S.; Ilton, Eugene S.; Martin, Richard L.; Jensen, Hans Jorgen A.; Knecht, Stefan

    2012-09-01

    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 reduced 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. Spin-orbit coupling in actinide cations

    Science.gov (United States)

    Bagus, Paul S.; Ilton, Eugene S.; Martin, Richard L.; Jensen, Hans Jørgen Aa.; Knecht, Stefan

    2012-09-01

    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 reduced 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.

  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 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

  14. 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.)

  15. 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.

  16. Oxidation state and structure of actinides in environmental samples using synchrotron-based techniques

    International Nuclear Information System (INIS)

    Our experimental investigations are focused on the use of XANES/EXAFS to identify actinide phases and oxidation state in environmentally-relevant samples. Oxidation state trends with XANES edge position were first established for plutonium and neptunium reference solids. The results for a series of plutonium solids that differ in oxidation state are shown. We have also examined a series of Pu(III) solids where we have shown that even though significant differences in the geometry exist, the edge positions do not change (to an uncertainty of ± 0.3 eV). Similar experiments were done with neptunium standards but the oxidation state trends are less clear. On the basis of the results with plutonium standards, XANES was used to establish oxidation state in actinide precipitates in WIPP brine, actinide waste forms, and biologically-induced actinide precipitation reactions. These experimental efforts are integrated with theoretical efforts to calculate XANES/EXAFS spectra to help interpret the experimental results. Calculations of the Pu LIII XANES of small cluster models of the local Pu environment in PuO2 have been carried out to compare with the experimental results obtained at the APS. The resulting spectra give relative peak energies and intensities in good agreement with experiment. (authors)

  17. 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

  18. 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

  19. Comparison among MCNP-based depletion codes applied to burnup calculations of pebble-bed HTR lattices

    International Nuclear Information System (INIS)

    The double-heterogeneity characterising pebble-bed high temperature reactors (HTRs) makes Monte Carlo based calculation tools the most suitable for detailed core analyses. These codes can be successfully used to predict the isotopic evolution during irradiation of the fuel of this kind of cores. At the moment, there are many computational systems based on MCNP that are available for performing depletion calculation. All these systems use MCNP to supply problem dependent fluxes and/or microscopic cross sections to the depletion module. This latter then calculates the isotopic evolution of the fuel resolving Bateman's equations. In this paper, a comparative analysis of three different MCNP-based depletion codes is performed: Montburns2.0, MCNPX2.6.0 and BGCore. Monteburns code can be considered as the reference code for HTR calculations, since it has been already verified during HTR-N and HTR-N1 EU project. All calculations have been performed on a reference model representing an infinite lattice of thorium-plutonium fuelled pebbles. The evolution of k-inf as a function of burnup has been compared, as well as the inventory of the important actinides. The k-inf comparison among the codes shows a good agreement during the entire burnup history with the maximum difference lower than 1%. The actinide inventory prediction agrees well. However significant discrepancy in Am and Cm concentrations calculated by MCNPX as compared to those of Monteburns and BGCore has been observed. This is mainly due to different Am-241 (n,γ) branching ratio utilized by the codes. The important advantage of BGCore is its significantly lower execution time required to perform considered depletion calculations. While providing reasonably accurate results BGCore runs depletion problem about two times faster than Monteburns and two to five times faster than MCNPX.

  20. 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.

    2016-03-01

    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 (CRM-126a, and compared with traditional total evaporation methods.