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Sample records for actinide isotopes

  1. Actinide isotopic analysis systems

    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

  2. Radiochemical studies of neutron deficient actinide isotopes

    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

  3. Radiochemical studies of neutron deficient actinide isotopes

    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.

  4. Preparation of isotopes and sources of actinide elements

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

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

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

    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

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

    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)

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

    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

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

    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.

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

    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

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

    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)

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

    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 ...

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

    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)

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

    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

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

    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.

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

    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

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

    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)

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

    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 ...

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

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

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

    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)

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

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

    2016-06-01

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

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

    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.

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

    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.

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

    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.

  5. Managing Inventories of Heavy Actinides

    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.

  6. Actinides-1981

    1981-09-01

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

  7. Actinides-1981

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

  8. Calorimetric assay of minor actinides

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

    1996-12-31

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

  9. Calorimetric assay of minor actinides

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

  10. Research needs in metabolism and dosimetry of the actinides

    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;

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

    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.)

  12. Research on the chemical speciation of actinides

    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

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

    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

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

    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.)

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

    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

    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. Anthropogenic Actinides in the Environment

    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)

  18. Actinide recycle

    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

  19. Research on the chemical speciation of actinides

    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

  20. Actinides analysis by accelerator mass spectrometry

    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

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

    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)

  2. Coordination chemistry for new actinide separation processes

    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. The lanthanides and actinides

    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

  4. Actinide environmental chemistry

    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.)

  5. Use of fast reactors for actinide transmutation

    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

  6. 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

    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

  7. Rapid determination of actinides in asphalt samples

    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)

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

    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

  9. Research in actinide chemistry

    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

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

    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

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

    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.

  12. The Lawrence Livermore National Laboratory Intelligent Actinide Analysis System

    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

  13. The Lawrence Livermore National Laboratory Intelligent Actinide Analysis System

    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

  14. Research in actinide chemistry

    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.

  15. PF-4 actinide disposition strategy

    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.

  16. Subsurface Biogeochemistry of Actinides

    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).

  17. Actinide measurements by AMS using fluoride matrices

    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.

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

    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

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

    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

  20. Radiochemistry and actinide chemistry

    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

  1. Actinide separative chemistry

    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

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

    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

  3. Status of nuclear data for actinides

    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.

  4. Compilation of actinide neutron nuclear data

    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.)

  5. Nuclear data for plutonium and minor actinides

    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

  6. Physics studies of higher actinide consumption in an LMR

    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.

  7. Evaluation of prompt neutron spectra for minor actinide nuclei

    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.)

  8. Recovering actinide values

    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)

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

    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.

  10. Actinides: why are they important biologically

    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

  11. Photoelectron spectra of actinide compounds

    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

  12. Actinides in irradiated graphite of RBMK-1500 reactor

    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 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

    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)

  14. Optical techniques for actinide research

    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

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

    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

  16. Concentration of actinides in the food chain

    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

    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

    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. Environmental research on actinide elements

    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

  20. Actinides, accelerators and erosion

    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.

  1. Properties of minor actinide nitrides

    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)

  2. The advanced liquid metal reactor actinide recycle system

    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

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

    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)

  4. THERMODYNAMICS OF THE ACTINIDES

    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)

  5. Actinide burning and waste disposal

    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

  6. Kinetics of actinide complexation reactions

    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

  7. 33rd Actinide Separations Conference

    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.

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

    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

  9. Actinide-specific sequestering agents and decontamination applications

    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.

  10. Thermal-hydraulics of actinide burner reactors

    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)

  11. Actinides and Life's Origins.

    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

  12. ALMR potential for actinide consumption

    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)

  13. Criticality and thermal analyses of separated actinides

    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)

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

    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

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

    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 ...

  16. Actinide cation-cation complexes

    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

  17. Orbital effects in actinide systems

    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

  18. Fabrication of actinide mononitride fuel

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

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

    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.)

  20. Environmental research on actinide elements

    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)

  1. ENDF/B-V actinides

    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)

  2. Detection of the actinides and cesium from environmental samples

    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).

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

    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

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

    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.

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

    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

  6. Toward laser ablation Accelerator Mass Spectrometry of actinides

    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.

  7. Toward laser ablation Accelerator Mass Spectrometry of actinides

    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.

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

    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

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

    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)

  10. Actinides recycling assessment in a thermal reactor

    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

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

    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)

  12. Spin Hamiltonians for actinide ions

    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)

  13. Actinide chemistry in ionic liquids.

    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

  14. Actinide recovery techniques utilizing electromechanical processes

    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

  15. Actinide Waste Forms and Radiation Effects

    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

  16. Actinide-only burnup credit for spent fuel transport

    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

    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

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

    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)

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

    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

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

    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...

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

    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%

  3. PWRs potentialities for minor actinides burning

    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)

  4. Long-term plant availability of actinides

    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. Chemistry of actinides and fission products

    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

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

    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.

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

    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.

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

    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.

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

    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)

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

    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)

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

    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

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

    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.

  13. Calculated Atomic Volumes of the Actinide Metals

    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....

  14. Environmental chemistry of the actinide elements

    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

  15. PIE analysis for minor actinide

    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)

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

    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

  17. Actinide co-conversion by internal gelation

    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)

  18. Actinide ion sensor for pyroprocess monitoring

    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.

  19. The ALMR actinide burning system

    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

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

    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...

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

    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. Use of high gradient magnetic separation for actinide application

    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

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

    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

  4. Experimental studies of actinides in molten salts

    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

  5. Experimental studies of actinides in molten salts

    Reavis, J.G.

    1985-06-01

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

  6. Spin and orbital moments in actinide compounds

    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...

  7. Actinide chemistry in the far field

    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)

  8. Electronic structure and magnetic properties of actinides

    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

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

    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

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

    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

  11. Actinide recovery from pyrochemical residues

    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

  12. Minor actinides transmutation strategies in sodium fast reactors

    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

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

    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)

  14. Multi-nucleon transfer experiments in the actinide region

    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.

  15. Subsurface interactions of actinide species and microorganisms. Implications for the bioremediation of actinide-organic mixtures

    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)

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

    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.

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

    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

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

    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

  19. Overview of actinide chemistry in the WIPP

    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

  20. PWRs potentialities for minor actinides burning

    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

  1. Electronic structure and correlation effects in actinides

    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.

  2. Preparation of actinide targets by electrodeposition

    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.

  3. Actinide research to solve some practical problems

    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

  4. Advanced Aqueous Separation Systems for Actinide Partitioning

    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.

  5. BWR Assembly Optimization for Minor Actinide Recycling

    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).

  6. 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

    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.

  7. 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

    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.)

  8. Superconductivity in rare earth and actinide compounds

    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.)

  9. Lanthanides and actinides in ionic liquids

    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...

  10. New molecules to separate actinides: the picolinamides

    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

  11. Lattice effects in the light actinides

    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

  12. Measurements of minor actinides cross sections for transmutation

    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)

  13. Recent progress in actinide borate chemistry.

    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

  14. Evaluation of actinide partitioning and transmutation

    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

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

    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

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

    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)

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

    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)

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

    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.

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

    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.

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

    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

  1. FY2011 Annual Report for the Actinide Isomer Detection Project

    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

  2. Oak Ridge National Laboratory's isotope enrichment program

    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

  3. Radioecology of the actinide elements

    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

  4. Actinide transmutation in nuclear reactors

    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)

  5. 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

    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)

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

    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.

  7. Waste disposal aspects of actinide separation

    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.)

  8. Solubility of actinide surrogates in nuclear glasses

    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

    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. New reagents for actinide-lanthanide group separations

    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

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

    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

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

    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

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

    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.

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

    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

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

    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

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

    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)

  17. Separation of actinides with alkylpyridinium salts

    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

  18. Minior Actinide Doppler Coefficient Measurement Assessment

    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.

  19. Research on Actinides in Nuclear Fuel Cycles

    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

  20. Neutron scattering studies of the actinides

    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

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

    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.

  2. Spin-Orbit Coupling in Actinide Cations

    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.

  3. Spin-orbit coupling in actinide cations

    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.

  4. Actinide and fission product separation and transmutation

    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.)

  5. Actinide phosphonate complexes in aqueous solutions

    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

  6. Actinide elements in aquatic and terrestrial environments

    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

  7. Sequential analysis of selected actinides in urine

    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)

  8. Actinide and fission product separation and transmutation

    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.)

  9. Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples

    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.

  10. Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples

    Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; Spencer, Khalil J.

    2016-06-01

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics "toolbox", especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (CRM-126a, and compared with traditional total evaporation methods.

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

    Maxwell, S.; Jones, V.

    2009-05-27

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

  12. Actinide recycle in LMFBRs as a waste management alternative

    Beaman, S.L.

    1979-08-21

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

  13. Chemical compatibility of HLW borosilicate glasses with actinides

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

  14. Actinide recycle in LMFBRs as a waste management alternative

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

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

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

    2015-07-14

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

  16. Placental transfer of plutonium and other actinides

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

  17. Actinide and fission product partitioning and transmutation

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

  18. Actinide and fission product partitioning and transmutation

    NONE

    1995-07-01

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

  19. Treatment of actinide-containing organic waste

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

  20. Trends in actinide processing at Hanford

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

  1. Report of the panel on inhaled actinides

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

  2. Electronic Structure of the Actinide Metals

    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...

  3. Spin–orbit coupling in actinide cations

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

    2012-01-01

    The limiting case of Russell–Saunders coupling, which leads to a maximum spin alignment for the open shell electrons, usually explains the properties of high spin ionic crystals with transition metals. For actinide compounds, the spin–orbit splitting is large enough to cause a significantly reduced...

  4. ENDF/B-5 Actinides (Rev. 86)

    This document summarizes the contents of the Actinides part of the ENDF/B-5 nuclear data library released by the US National Nuclear Data Center. This library or selective retrievals of it, are available costfree from the IAEA Nuclear Data Section upon request. The present version of the library is the Revision of 1986. (author). Refs, figs and tabs

  5. ACTINET: a European Network for Actinide Sciences

    Full text of publication follows: The research in Actinide sciences appear as a strategic issue for the future of nuclear systems. Sustainability issues are clearly in connection with the way actinide elements are managed (either addressing saving natural resource, or decreasing the radiotoxicity of the waste). The recent developments in the field of minor actinide P and T offer convincing indications of what could be possible options, possible future processes for the selective recovery of minor actinides. But they point out, too, some lacks in the basic understanding of key-issues (such as for instance the control An versus Ln selectivity, or solvation phenomena in organic phases). Such lacks could be real obstacles for an optimization of future processes, with new fuel compounds and facing new recycling strategies. This is why a large and sustainable work appears necessary, here in the field of basic actinide separative chemistry. And similar examples could be taken from other aspects of An science, for various applications (nuclear fuel or transmutation targets design, or migration issues,): future developments need a strong, enlarged, scientific basis. The Network ACTINET, established with the support of the European Commission, has the following objectives: - significantly improve the accessibility of the major actinide facilities to the European scientific community, and form a set of pooled facilities, as the corner-stone of a progressive integration process, - improve mobility between the member organisations, in particular between Academic Institutions and National Laboratories holding the pooled facilities, - merge part of the research programs conducted by the member institutions, and optimise the research programs and infrastructure policy via joint management procedures, - strengthen European excellence through a selection process of joint proposals, and reduce the fragmentation of the community by putting critical mass of resources and expertise on

  6. Library of Recommended Actinide Decay Data, 2011

    A major objective of the nuclear data programme within the IAEA is to devise and promote improvements in the quality of nuclear data used in science and technology. Work of this nature was performed by participants in an IAEA coordinated research project (CRP) formulated in 2005 to produce an updated decay data library of important actinides recommended for adoption in various nuclear applications. The specific objectives of this project were to improve the accuracy of heavy element and actinide decay data in order to: determine more accurately the effects of these recommended data on fission reactor fuel cycles; aid in improved assessments of nuclear waste management procedures; provide more reliable decay data for nuclear safeguards; assess with greater confidence the environmental impact of specific actinides and other heavy element radionuclides generated through their decay chains; and extend the scientific knowledge of actinide decay characteristics for nuclear physics research and non-energy applications. Some CRP participants were able to perform a number of highly precise measurements, based on the availability of suitable source materials, and systematic in depth evaluations of the requested decay data. These requested data consisted primarily of half-lives, and α, β-, EC/β+, Auger electron, conversion electron, X ray and γ ray energies and emission probabilities, all with uncertainties expressed at the 1σ confidence level. The IAEA established a CRP entitled Updated Decay Data Library for Actinides in mid-2005. During the course of discussions at the coordinated research meetings, the participants agreed to undertake work programmes of measurements and evaluations, to be completed by the end of 2010. The results of the evaluation studies undertaken by the CRP are presented in Annex I. Annexes II-V include descriptions of the sources of the evaluated decay data and each individual evaluation process in detail, as well as data files in the Evaluated

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

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

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

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

  9. Enhancing VVER annular proliferation resistance fuel with minor actinides

    Key aspects of the Global Nuclear Energy Partnership (GNEP) are to significantly advance the science and technology of nuclear energy systems and the Advanced Fuel Cycle (AFC) program. It consists of both innovative nuclear reactors and innovative research in separation and transmutation. To accomplish these goals, international cooperation is very important and public acceptance is crucial. The merits of nuclear energy are high-density energy, with low environmental impacts (i.e. almost zero greenhouse gas emission). Planned efforts involve near term and intermediate-term improvements in fuel utilization and recycling in current light water reactors (LWRs) as well as the longer-term development of new nuclear energy systems that offer much improved fuel utilization and proliferation resistance, along with continued advances in operational safety. The challenges are solving the energy needs of the world, protection against nuclear proliferation, the problem of nuclear waste, and the global environmental problem. To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the 238Pu and 240Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides (237Np and 241Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of 238Pu /Pu. For future advanced nuclear systems, the minor actinides (MA) are viewed more as a resource to be recycled, or transmuted to less hazardous and possibly more useful forms, rather than simply as a waste stream to be disposed of in expensive repository facilities. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the

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

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

    1992-01-01

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

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

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

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

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

    2016-01-08

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

  13. R and D for actinide partitioning and recovery of valuables from high level waste using radiotracers

    In the context of growing world population with rapidly increasing energy needs and the threat of global warming due to CO2 emission (caused by fossil fuel burning), the nuclear energy may be an attractive option particularly in the developing countries. Recycling of fuel is a unique feature of nuclear power technology which makes it a favourable choice with respect to conservation of energy resources. Steady growth of global fuel reprocessing activities (6000 tHM/annum) implies a vital role of separation science in developing efficient procedures for the separation and purification of actinides and in devising safe procedures for the management of nuclear waste arising at different stages of the PUREX process. High Level Waste (HLW) comprising of the concentrate of the raffinate of the co-extraction cycle (with over 95% of the total radioactivity produced in the burn up process in reactor) need to be isolated from the biosphere. There is a consensus among the waste management technologists that the safest route to achieve this, is to deposit it in a stable geological formation after it's immobilization in suitable glass/Synroc matrix. It ensures that any risk from exposure due to accidental intervention or natural disturbance is minimized. Risk perception is essentially due to the large radiological toxicity associated with alpha emitters like 237Np, 241Am, 243Am and 245Cm. Isotopes of Pu (left unrecovered) present in HLW also contribute towards radiological toxicity. In view of the high cost involved and the need for continuous surveillance, several countries are considering modifying their reprocessing schemes to partition (isolate) long-lived actinides from HLW. Since the volume of the actinide oxides (which retain major fraction of the radio toxicity of HLW) is significantly lower as compared to the other metal oxides present in HLW, such an approach is expected to reduce the cost of immobilization as well as of disposal (in geological repository) and

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

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

  15. Minor actinide transmutation on PWR burnable poison rods

    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

  16. Method to determine actinide pollution in water

    This patent describes a process for measuring small amounts, of actinide pollution in fluidic samples by use of solid state track recording devices. It comprises: containing a sample to be tested, containing small amounts of less than 3E-12 Curies per cubic centimeter of actinide pollution, in a sample cell defining an internal chamber and having means for ingress and egress and means for establishing a fluidic sample therein, the sample cell being substantially transparent to thermal neutron radiation and the internal chamber defined therein being configured to constitute a fluidic sample therein as an asymptotic fluid fission source; positioning a solid state track recorder within the internal chamber defined by the sample cell, so that the solid state track recorder has a radiation viewing window through an asymptotic thickness of a fluidic sample contained in the sample cell; capturing at least an asymptotic amount of fluidic sample in the sample cell

  17. Microbial Transformations of Actinides and Other Radionuclides

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

    2009-01-07

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

  18. Actinide and fission product separation and transmutation

    NONE

    1991-07-01

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

  19. Interaction of actinide cations with synthetic polyelectrolytes

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

  20. Actinide and fission product separation and transmutation

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

  1. Actinides: from heavy fermions to plutonium metallurgy

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

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

    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.

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

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

  4. Actinide co-ordination and discrimination by human transferrin

    The design and evaluation of synthetic chelating agents which are specific for the actinide(IV) ions are described. The initial approach has been based on the biological and chemical similarities of Pu(IV) and Fe(III). In particular, using a philosophy influenced by naturally occurring ferric ion chelating agents, tetracatechoylamide ligands have been developed for the actinides. The test of the degree to which there was an actinide-specific complexing agent has been based on studies using Pu4+ as a biological contaminant. For a chelating agent to be able to sequester actinides effectively, it must remove actinides from actinide(IV)-protein complexes. The complexation chemistry of Th(IV)-transferrin system is described. The evidence suggests that, based on a size criterion, Th(IV) may be a poor biological model for Pu(IV) in some cases, with U(IV) being a somewhat better model. (author)

  5. Actinide Source Term Program, position paper. Revision 1

    The Actinide Source Term represents the quantity of actinides that could be mobilized within WIPP brines and could migrate with the brines away from the disposal room vicinity. This document presents the various proposed methods for estimating this source term, with a particular focus on defining these methods and evaluating the defensibility of the models for mobile actinide concentrations. The conclusions reached in this document are: the 92 PA open-quotes expert panelclose quotes model for mobile actinide concentrations is not defensible; and, although it is extremely conservative, the open-quotes inventory limitsclose quotes model is the only existing defensible model for the actinide source term. The model effort in progress, open-quotes chemical modeling of mobile actinide concentrationsclose quotes, supported by a laboratory effort that is also in progress, is designed to provide a reasonable description of the system and be scientifically realistic and supplant the open-quotes Inventory limitsclose quotes model

  6. Actinides reduction by recycling in a thermal reactor

    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)

  7. Thermal properties of minor actinide targets

    Staicu, Dragos; Somers, Joseph; FERNANDEZ CARRETERO Asuncion; KONINGS Rudy

    2014-01-01

    The thermal properties of minor actinides targets for the management of high level and long lived radioactive waste are investigated. The microstructure, thermal diffusivity and specific heat of (Pu,Am)O2, (Zr,Pu,Am)O2, (Zr,Y,Am)O2, (Zr,Y,Pu,Am)O2 and CERMETS with Mo matrix are characterised in order to assess the safety limits of these materials.

  8. SPECIFIC SEQUESTERING AGENTS FOR THE ACTINIDES

    Raymond, Kenneth N.; Smith, William L.; Weitl, Frederick L.; Durbin, Patricia W.; Jones, E.Sarah; Abu-Dari, Kamal; Sofen, Stephen R.; Cooper, Stephen R.

    1979-09-01

    This paper summarizes the current status of a continuing project directed toward the synthesis and characterization of chelating agents which are specific for actinide ions - especially Pu(IV) - using a biomimetic approach that relies on the observation that Pu(IV) and Fe(III) has marked similarities that include their biological transport and distribution in mammals. Since the naturally-occurring Fe(III) sequestering agents produced by microbes commonly contain hydroxamate and catecholate functional groups, these groups should complex the actinides very strongly and macrocyclic ligands incorporating these moieties are being prepared. We have reported the isolation and structure analysis of an isostructural series of tetrakis(catecholato) complexes with the general stoichiometry Na{sub 4}[M(C{sub 6}H{sub 4}O{sub 2}){sub 4}] • 21 H{sub 2}O (M = Th, U, Ce, Hf). These complexes are structural archetypes for the cavity that must be formed if an actinide-specific sequestering agent is to conform ideally to the coordination requirements of the central metal ion. The [M(cat){sub 4}]{sup 4-} complexes have the D{sub 2d} symmetry of the trigonal-faced dodecahedron.. The complexes Th [R'C(0)N(O)R]{sub 4} have been prepared where R = isopropyl and R' = t-butyl or neopentyl. The neopentyl derivative is also relatively close to an idealized D{sub 2d} dodecahedron, while the sterically more hindered t-butyl compound is distorted toward a cubic geometry. The synthesis of a series of 2, 3-dihydroxy-benzoyl amide derivatives of linear and cyclic tetraaza- and diazaalkanes is reported. Sulfonation of these compounds improves the metal complexation and in vivo removal of plutonium from test animals. These results substantially exceed the capabilities of compounds presently used for the therapeutic treatment of actinide contamination.

  9. The electrochemical properties of actinide amalgams

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

  10. Actinide and fission product partitioning and transmutation

    NONE

    1997-07-01

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