Investigation of Plutonium and Uranium Precipitation Behavior with Gadolinium as a Neutron Poison

DOE Office of Scientific and Technical Information (OSTI.GOV)

Visser, A.E.

2003-10-17

The caustic precipitation of plutonium (Pu)-containing solutions has been investigated to determine whether the presence of 3:1 uranium (U):Pu in solutions stored in the H-Canyon Facility at the U.S. Department of Energy's (DOE) Savannah River Site (SRS) would adversely impact the use of gadolinium nitrate (Gd(NO3)3) as a neutron poison. In the past, this disposition strategy has been successfully used to discard solutions containing approximately 100 kg of Pu to the SRS high level waste (HLW) system. In the current experiments, gadolinium (as Gd(NO3)3) was added to samples of a 3:1 U:Pu solution, a surrogate 3 g/L U solution, andmore » a surrogate 3 g/L U with 1 g/L Pu solution. A series of experiments was then performed to observe and characterize the precipitate at selected pH values. Solids formed at pH 4.5 and were found to contain at least 50 percent of the U and 94 percent of the Pu, but only 6 percent of the Gd. As the pH of the solution increased (e.g., pH greater than 14 with 1.2 or 3.6 M sodium hydroxide (NaOH) excess), the precipitate contained greater than 99 percent of the Pu, U, and Gd. After the pH greater than 14 systems were undisturbed for one week, no significant changes were found in the composition of the solid or supernate for each sample. The solids were characterized by X-ray diffraction (XRD) which found sodium diuranate (Na2U2O7) and gadolinium hydroxide (Gd(OH)3) at pH 14. Thermal gravimetric analysis (TGA) indicated sufficient water molecules were present in the solids to thermalize the neutrons, a requirement for the use of Gd as a neutron poison. Scanning electron microscopy (SEM) was also performed and the accompanying back-scattering electron analysis (BSE) found Pu, U, and Gd compounds in all pH greater than 14 precipitate samples. The rheological properties of the slurries at pH greater than 14 were also investigated by performing precipitate settling rate studies and measuring the viscosity and density of the materials. Based on the results of these experiments, poisoning the Pu-U solutions with Gd and subsequent neutralization is a viable process for discarding the Pu to the SRS HLW system.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carmack, Jon; Hayes, Steven; Walters, L. C.

This document explores startup fuel options for a proposed test/demonstration fast reactor. The fuel options considered are the metallic fuels U-Zr and U-Pu-Zr and the ceramic fuels UO 2 and UO 2-PuO 2 (MOX). Attributes of the candidate fuel choices considered were feedstock availability, fabrication feasibility, rough order of magnitude cost and schedule, and the existing irradiation performance database. The reactor-grade plutonium bearing fuels (U-Pu-Zr and MOX) were eliminated from consideration as the initial startup fuels because the availability and isotopics of domestic plutonium feedstock is uncertain. There are international sources of reactor grade plutonium feedstock but isotopics and availabilitymore » are also uncertain. Weapons grade plutonium is the only possible source of Pu feedstock in sufficient quantities needed to fuel a startup core. Currently, the available U.S. source of (excess) weapons-grade plutonium is designated for irradiation in commercial light water reactors (LWR) to a level that would preclude diversion. Weapons-grade plutonium also contains a significant concentration of gallium. Gallium presents a potential issue for both the fabrication of MOX fuel as well as possible performance issues for metallic fuel. Also, the construction of a fuel fabrication line for plutonium fuels, with or without a line to remove gallium, is expected to be considerably more expensive than for uranium fuels. In the case of U-Pu-Zr, a relatively small number of fuel pins have been irradiated to high burnup, and in no case has a full assembly been irradiated to high burnup without disassembly and re-constitution. For MOX fuel, the irradiation database from the Fast Flux Test Facility (FFTF) is extensive. If a significant source of either weapons-grade or reactor-grade Pu became available (i.e., from an international source), a startup core based on Pu could be reconsidered.« less

Evidence of extinct 244Pu in ancient terrestrial zircons

NASA Astrophysics Data System (ADS)

Harrison, T. M.; Turner, G.; Holland, G.; Gilmour, J. D.; Mojzsis, S. J.

2003-04-01

The Pu/U ratio of the early Earth is an important parameter in models of mantle evolution based on noble gas isotopes. Current estimates assume the Earth accreted with a chondritic Pu/U and are based on analyses of the chondrite St Severin and the achondrite Angra dos Reis. These estimates are poorly constrained, ranging from 0.004 to 0.008. On account of its short, 82 Ma, half-life, 244Pu was essentially extinct 3,900 Ma ago, and consequently there exists no reliable measurement of Pu/U for the Earth. The discovery of zircons dating from the period when 244Pu was "live" offers the first opportunity to measure the former terrestrial abundance of 244Pu directly. Xenon isotopes are produced by spontaneous fission and, in principle, are readily distinguishable from those produced by 238U-fission (e.g. 131Xe/136Xe = 0.24 and 0.08 respectively). However the expected levels of fission xenon in individual zircons, weighing 1 - 2 μg and containing 100 - 200 ppm U, are below, or at best comparable to, the Xe blank levels (˜10-15 ccSTP) typical of conventional noble gas mass spectrometers. In order to analyse these minute amounts of xenon we have made use of a uniquely sensitive instrument, developed in Manchester, based on the principle of laser resonance ionisation. RELAX (Refrigerator Enhanced Laser Analyser for Xenon) is capable of analysing samples of only a few thousand atoms, some two orders of magnitude smaller than conventional mass spectrometers. We have carried out preliminary analyses of 4 individual 4,150 Ma zircons and one 3,600 Ma zircon from Jack Hills, Western Australia, and obtained five clear fission spectra. All but one were essentially free from significant atmospheric blank (the average 130Xe blank was 3× 10-18 ccSTP, i.e. 80 atoms). The spectra of the older zircons clearly demonstrated the presence of varying amounts of 244Pu fission xenon. The highest 131Xe/136Xe, 0.136 ± 0.003, corresponds to an initial Pu/U ratio of 0.0057. The lower ratios could result from loss of Xe after 4.0 Ga or represent U-Pu fractionation. We are currently repeating the exercise with older zircons and intend to search for correlations with REE patterns, oxygen isotopes, and the degree of U-Pb concordance, and to investigate the thermal release characteristics of the xenon. In addition to constraining the terrestrial Pu/U ratio these investigations may allow us to characterise the geochemical behaviour of Pu as a constraint on the earliest crust forming processes.

Investigating Pu and U isotopic compositions in sediments: a case study in Lake Obuchi, Rokkasho Village, Japan using sector-field ICP-MS and ICP-QMS.

PubMed

Zheng, Jian; Yamada, Masatoshi

2005-08-01

The objectives of the present work were to study isotope ratios and the inventory of plutonium and uranium isotope compositions in sediments from Lake Obuchi, which is in the vicinity of several nuclear fuel facilities in Rokkasho, Japan. Pu and its isotopes were determined using sector-field ICP-MS and U and its isotopes were determined with ICP-QMS after separation and purification with a combination of ion-exchange and extraction chromatography. The observed (240)Pu/(239)Pu atom ratio (0.186 +/- 0.016) was similar to that of global fallout, indicating that the possible early tropospheric fallout Pu did not deliver Pu from the Pacific Proving Ground to areas above 40 degrees N. The previously reported higher Pu inventory in the deep water area of Lake Obuchi could be attributed to the lateral transportation of Pu deposited in the shallow area which resulted from the migration of deposited global fallout Pu from the land into the lake by river runoff and from the Pacific Ocean by tide movement and sea water scavenging, as well as from direct soil input by winds. The (235)U/(238)U atom ratios ranged from 0.00723 to 0.00732, indicating the natural origin of U in the sediments. The average (234)U/(238)U activity ratio of 1.11 in a sediment core indicated a significant sea water U contribution. No evidence was found for the release of U containing wastes from the nearby nuclear facilities. These results will serve as a reference baseline on the levels of Pu and U in the studied site so that any further contamination from the spent nuclear fuel reprocessing plants, the radioactive waste disposal and storage facilities, and the uranium enrichment plant can be identified, and the impact of future release can be rapidly assessed.

Flowsheet Analysis of U-Pu Co-Crystallization Process as a New Reprocessing System

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shunji Homma; Jun-ichi Ishii; Jiro Koga

2006-07-01

A new fuel reprocessing system by U-Pu co-crystallization process is proposed and examined by flowsheet analysis. This reprocessing system is based on the fact that hexavalent plutonium in nitric acid solution is co-crystallized with uranyl nitrate, whereas it is not crystallized when uranyl nitrate does not exist in the solution. The system consists of five steps: dissolution of spent fuel, plutonium oxidation, U-Pu co-crystallization as a co-decontamination, re-dissolution of the crystals, and U re-crystallization as a U-Pu separation. The system requires a recycling of the mother liquor from the U-Pu co-crystallization step and the appropriate recycle ratio is determined bymore » flowsheet analysis such that the satisfactory decontamination is achieved. Further flowsheet study using four different compositions of LWR spent fuels demonstrates that the constant ratio of plutonium to uranium in mother liquor from the re-crystallization step is achieved for every composition by controlling the temperature. It is also demonstrated by comparing to the Purex process that the size of the plant based on the proposed system is significantly reduced. (authors)« less

Pu 236 ( n , f ) , Pu 237 ( n , f ) , and Pu 238 ( n , f ) cross sections deduced from ( p , t ) , ( p , d ) , and ( p , p ' ) surrogate reactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hughes, R. O.; Beausang, C. W.; Ross, T. J.

2014-07-01

The Pu 236(n,f), Pu 237(n,f) and Pu 238(n,f) cross sections have been inferred by utilizing the surrogate ratio method. Targets of Pu 239 and U 235 were bombarded with 28.5-MeV protons, and the light ion recoils, as well as fission fragments, were detected using the STARS detector array at the K150 Cyclotron at the Texas A&M cyclotron facility. The (p, tf) reaction on Pu 239 and U 235 targets was used to deduce the σ (Pu 236(n,f))/σ(U 232(n,f)) ratio, and the Pu 236(n,f) cross section was subsequently determined for En=0.5–7.5 MeV. Similarly, the (p,df) reaction on the same two targetsmore » was used to deduce the σ(Pu 237(n,f))/σ(U 233(n,f)) ratio, and the Pu 237(n,f) cross section was extracted in the energy range En=0.5–7 MeV. The Pu 238(n,f) cross section was also deduced by utilizing the (p,p') reaction channel on the same targets. There is good agreement with the recent ENDF/B-VII.1 evaluated cross section data for Pu 238(n,f) in the range En=0.5–10.5 MeV and for Pu 237(n,f) in the range En=0.5–7 MeV; however, the Pu 236(n,f) cross section deduced in the present work is higher than the evaluation between 2 and 7 MeV.« less

Charge distribution and local structure and speciation in the UO 2+x and PuO 2+x binary oxides for x⩽0.25

NASA Astrophysics Data System (ADS)

Conradson, Steven D.; Begg, Bruce D.; Clark, David L.; den Auwer, Christophe; Ding, Mei; Dorhout, Peter K.; Espinosa-Faller, Francisco J.; Gordon, Pamela L.; Haire, Richard G.; Hess, Nancy J.; Hess, Ryan F.; Webster Keogh, D.; Lander, Gerard H.; Manara, Dario; Morales, Luis A.; Neu, Mary P.; Paviet-Hartmann, Patricia; Rebizant, Jean; Rondinella, Vincenzo V.; Runde, Wolfgang; Drew Tait, C.; Kirk Veirs, D.; Villella, Phillip M.; Wastin, Franck

2005-02-01

The local structure and chemical speciation of the mixed valence, fluorite-based oxides UO 2+x (0.00⩽ x⩽0.20) and PuO 2+x/PuO 2+x-y(OH) 2y· zH 2O have been determined by U/Pu L III XAFS spectroscopy. The U spectra indicate (1) that the O atoms are incorporated as oxo groups at short (1.75 Å) U-O distances consistent with U(VI) concomitant with a large range of U displacements that reduce the apparent number of U neighbors and (2) that the UO 2 fraction remains intact implying that these O defects interact to form clusters and give the heterogeneous structure consistent with the diffraction patterns. The PuO 2+x system, which does not show a separate phase at its x=0.25 endpoint, also displays (1) oxo groups at longer 1.9 Å distances consistent with Pu(V+ δ), (2) a multisite Pu-O distribution even when x is close to zero indicative of the formation of stable species with H 2O and its hydrolysis products with O 2-, and (3) a highly disordered, spectroscopically invisible Pu-Pu component. The structure and bonding in AnO 2+x are therefore more complicated than have previously been assumed and show both similarities but also distinct differences among the different elements.

Development of prototype induced-fission-based Pu accountancy instrument for safeguards applications.

PubMed

Seo, Hee; Lee, Seung Kyu; An, Su Jung; Park, Se-Hwan; Ku, Jeong-Hoe; Menlove, Howard O; Rael, Carlos D; LaFleur, Adrienne M; Browne, Michael C

2016-09-01

Prototype safeguards instrument for nuclear material accountancy (NMA) of uranium/transuranic (U/TRU) products that could be produced in a future advanced PWR fuel processing facility has been developed and characterized. This is a new, hybrid neutron measurement system based on fast neutron energy multiplication (FNEM) and passive neutron albedo reactivity (PNAR) methods. The FNEM method is sensitive to the induced fission rate by fast neutrons, while the PNAR method is sensitive to the induced fission rate by thermal neutrons in the sample to be measured. The induced fission rate is proportional to the total amount of fissile material, especially plutonium (Pu), in the U/TRU product; hence, the Pu amount can be calibrated as a function of the induced fission rate, which can be measured using either the FNEM or PNAR method. In the present study, the prototype system was built using six (3)He tubes, and its performance was evaluated for various detector parameters including high-voltage (HV) plateau, efficiency profiles, dead time, and stability. The system's capability to measure the difference in the average neutron energy for the FNEM signature also was evaluated, using AmLi, PuBe, (252)Cf, as well as four Pu-oxide sources each with a different impurity (Al, F, Mg, and B) and producing (α,n) neutrons with different average energies. Future work will measure the hybrid signature (i.e., FNEM×PNAR) for a Pu source with an external interrogating neutron source after enlarging the cavity size of the prototype system to accommodate a large-size Pu source (~600g Pu). Copyright © 2016 Elsevier Ltd. All rights reserved.

Measurements Conducted on an Unknown Object Labeled Pu-239

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hoteling, Nathan

Measurements were carried out on 12 November 2013 to determine whether Pu-239 was present on an object discovered in a plastic bag with label “Pu-­239 6 uCi.” Following initial survey measurements to verify that the object was not leaking or contaminated, spectra were collected with a High Purity Germanium (HPGe) detector with object positioned in two different configurations. Analysis of the spectra did not yield any direct evidence of Pu-­239. From the measured spectra, minimum detectable activity (MDA) was determined to be approximately 2 uCi for the gamma-­ray measurements. Although there was no direct evidence of Pu-239, a peak atmore » 60 keV characteristic of Am-­241 decay was observed. Since it is very likely that Am-­241 would be present in aged plutonium samples, this was interpreted as indirect evidence for the presence of plutonium on the object. Analysis of this peak led to an estimated Pu-­239 activity of 0.02–0.04 uCi, or <1x10 -6 grams.« less

Beta decay heat following U-235, U-238 and Pu-239 neutron fission

NASA Astrophysics Data System (ADS)

Li, Shengjie

1997-09-01

This is an experimental study of beta-particle decay heat from 235U, 239Pu and 238U aggregate fission products over delay times 0.4-40,000 seconds. The experimental results below 2s for 235U and 239Pu, and below 20s for 238U, are the first such results reported. The experiments were conducted at the UMASS Lowell 5.5-MV Van de Graaff accelerator and 1-MW swimming-pool research reactor. Thermalized neutrons from the 7Li(p,n)7Be reaction induced fission in 238U and 239Pu, and fast neutrons produced in the reactor initiated fission in 238U. A helium-jet/tape-transport system rapidly transferred fission fragments from a fission chamber to a low background counting area. Delay times after fission were selected by varying the tape speed or the position of the spray point relative to the beta spectrometer that employed a thin-scintillator-disk gating technique to separate beta-particles from accompanying gamma-rays. Beta and gamma sources were both used in energy calibration. Based on low-energy(<1 MeV) internal-conversion electron studies, a set of trial responses for the spectrometer was established and spanned electron energies 0-10 MeV. Measured beta spectra were unfolded for their energy distributions by the program FERD, and then compared to other measurements and summation calculations based on ENDF/B-VI fission-product data performed on the LANL Cray computer. Measurements of the beta activity as a function of decay time furnished a relative normalization. Results for the beta decay heat are presented and compared with other experimental data and the summation calculations.

Certified reference materials for radionuclides in Bikini Atoll sediment (IAEA-410) and Pacific Ocean sediment (IAEA-412).

PubMed

Pham, M K; van Beek, P; Carvalho, F P; Chamizo, E; Degering, D; Engeler, C; Gascó, C; Gurriaran, R; Hanley, O; Harms, A V; Herrmann, J; Hult, M; Ikeuchi, Y; Ilchmann, C; Kanisch, G; Kis-Benedek, G; Kloster, M; Laubenstein, M; Llaurado, M; Mas, J L; Nakano, M; Nielsen, S P; Osvath, I; Povinec, P P; Rieth, U; Schikowski, J; Smedley, P A; Suplinska, M; Sýkora, I; Tarjan, S; Varga, B; Vasileva, E; Zalewska, T; Zhou, W

2016-03-01

The preparation and characterization of certified reference materials (CRMs) for radionuclide content in sediments collected offshore of Bikini Atoll (IAEA-410) and in the open northwest Pacific Ocean (IAEA-412) are described and the results of the certification process are presented. The certified radionuclides include: (40)K, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (234)U, (238)U, (239)Pu, (239+240)Pu and (241)Am for IAEA-410 and (40)K, (137)Cs, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (235)U, (238)U, (239)Pu, (240)Pu and (239+240)Pu for IAEA-412. The CRMs can be used for quality assurance and quality control purposes in the analysis of radionuclides in sediments, for development and validation of analytical methods and for staff training. Copyright © 2015 Elsevier Ltd. All rights reserved.

Real-time monitoring of plutonium content in uranium-plutonium alloys

DOEpatents

Li, Shelly Xiaowei; Westphal, Brian Robert; Herrmann, Steven Douglas

2015-09-01

A method and device for the real-time, in-situ monitoring of Plutonium content in U--Pu Alloys comprising providing a crucible. The crucible has an interior non-reactive to a metallic U--Pu alloy within said interior of said crucible. The U--Pu alloy comprises metallic uranium and plutonium. The U--Pu alloy is heated to a liquid in an inert or reducing atmosphere. The heated U--Pu alloy is then cooled to a solid in an inert or reducing atmosphere. As the U--Pu alloy is cooled, the temperature of the U--Pu alloy is monitored. A solidification temperature signature is determined from the monitored temperature of the U--Pu alloy during the step of cooling. The amount of Uranium and the amount of Plutonium in the U--Pu alloy is then determined from the determined solidification temperature signature.

Fission cross sections of some thorium, uranium, neptunium and plutonium isotopes relative to /sup 235/U

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meadows, J W

1983-10-01

Earlier results from the measurements, at this Laboratory, of the fission cross sections of /sup 230/Th, /sup 232/Th, /sup 233/U, /sup 234/U, /sup 236/U, /sup 238/U, /sup 237/Np, /sup 239/Pu, /sup 240/Pu, and /sup 242/Pu relative to /sup 235/U are reviewed with revisions to include changes in data processing procedures, alpha half lives and thermal fission cross sections. Some new data have also been included. The current experimental methods and procedures and the sample assay methods are described in detail and the sources of error are presented in a systematic manner. 38 references.

Traditional and Model Based Assay of Irregular Geometry Items

DOE Office of Scientific and Technical Information (OSTI.GOV)

MOORE, FRANK S.; SALAYMEH, SALEEM

The Analytical Development Section (ADS) of SRNL was requested to perform a waste disposal assay of two heater boxes which had been used in the HB Line dissolvers. They had been sent to SRNL for study to make recommendations on how to prevent future failure of the units when they were replaced. The study having been completed, the units needed to be characterized prior to sending to Solid Waste for disposal. An assay station consisting of a turntable, HPGe detector, CANBERRA Inspector, transmission source and a portable computer was set up to do the required assays. The assays indicate themore » presence of U-235, Pu-239 and Cs-137. No measurable amounts of U-235 or Pu-239 were found. Therefore the Minimum Detectable Activities for U-235 and Pu-239 were calculated. For Heater Box 1, 0.23 grams of U-235 and 0.24 grams of Pu-239. For Heater Box 2, the results were 0.21 grams of U-235 and 0.21 grams of Pu-239. This paper describes and documents the assays employed to determine the amount of U, Pu and Cs contents of the heater boxes. The paper provides results of SNM assays using traditional calibration of the system and on one based on modeling. It also provides the scientific community with data that will assist the user in determining the method of choice for assaying items with irregular geometries.« less

Neutralization of Plutonium and Enriched Uranium Solutions Containing Gadolinium as a Neutron Poison

DOE Office of Scientific and Technical Information (OSTI.GOV)

BRONIKOWSKI, MG.

2004-04-01

Materials currently being dissolved in the HB-Line Facility will result in an accumulated solution containing an estimated uranium:plutonium (U:Pu) ratio of 4.3:1 and an 235U enrichment estimated at 30 per cent The U:Pu ratio and the enrichment are outside the evaluated concentration range for disposition to high level waste (HLW) using gadolinium (Gd) as a neutron poison. To confirm that the solution generated during the current HB-Line dissolving campaign can be poisoned with Gd, neutralized and discarded to the Savannah River Site (SRS) high level waste (HLW) system without undue nuclear safety concerns the caustic precipitation of surrogate solutions wasmore » examined. Experiments were performed with a U/Pu/Gd solution representative of the HB-Line estimated concentration ratio and also a U/Gd solution. Depleted U was used in the experiments as the enrichment of the U will not affect the chemical behavior during neutralization, but will affect the amount of Gd added to the solution. Settling behavior of the neutralized solutions was found to be comparable to previous studies. The neutralized solutions mixed easily and had expected densities of typical neutralized waste. The neutralized solids were found to be homogeneous and less than 20 microns in size. Partially neutralized solids were more amorphous than the fully neutralized solids. Based on the results of these experiments, Gd was found to be a viable poison for neutralizing a U/Pu/Gd solution with a U:Pu mass ratio of 4.3:1 thus extending the U:Pu mass ratio from the previously investigated 0-3:1 to 4.3:1. However, further work is needed to allow higher U concentrations or U:Pu ratios greater than investigated in this work.« less

A Signature Distinguishing Fissile From Non-Fissile Materials Using Linearly Polarized Gamma Rays

NASA Astrophysics Data System (ADS)

Mueller, J. M.; Ahmed, M. W.; Karwowski, H. J.; Myers, L. S.; Sikora, M. H.; Stave, S.; Tompkins, J. R.; Zimmerman, W. R.; Weller, H. R.

2013-04-01

Photofission of ^233,235,238U, ^239,240Pu, and ^232Th was induced by nearly 100% linearly polarized, high intensity (˜10^7 γs per second), and nearly-monoenergetic γ-ray beams of energies between 5.6 and 7.3 MeV at the High Intensity γ-ray Source (HIγS). An array of 18 liquid scintillating detectors was used to measure prompt fission neutron angular distributions. The ratio of prompt fission neutron yields parallel to the plane of beam polarization to the yields perpendicular to this plane was measured as a function of beam and neutron energy, as described in a recent publication showing results from ^235,238U, ^239Pu, and ^232Th [1]. A ratio near unity was found for ^233,235U and ^239Pu while a significant ratio (˜1.5-3) was found for ^238U, ^240Pu, and ^232Th. This large difference could be used to distinguish fissile isotopes (such as ^233,235U and ^239Pu) from non-fissile isotopes (such as ^238U, ^240Pu, and ^232Th). Polarization ratios as a function of the relative abundance of fissile to non-fissile isotopes will be presented. [4pt] [1] J. M. Mueller et al., Phys. Rev. C 85, 014605 (2012).

Impact of the cation distribution homogeneity on the americium oxidation state in the U0.54Pu0.45Am0.01O2-x mixed oxide

NASA Astrophysics Data System (ADS)

Vauchy, Romain; Robisson, Anne-Charlotte; Martin, Philippe M.; Belin, Renaud C.; Aufore, Laurence; Scheinost, Andreas C.; Hodaj, Fiqiri

2015-01-01

The impact of the cation distribution homogeneity of the U0.54Pu0.45Am0.01O2-x mixed oxide on the americium oxidation state was studied by coupling X-ray diffraction (XRD), electron probe micro analysis (EPMA) and X-ray absorption spectroscopy (XAS). Oxygen-hypostoichiometric Am-bearing uranium-plutonium mixed oxide pellets were fabricated by two different co-milling based processes in order to obtain different cation distribution homogeneities. The americium was generated from β- decay of 241Pu. The XRD analysis of the obtained compounds did not reveal any structural difference between the samples. EPMA, however, revealed a high homogeneity in the cation distribution for one sample, and substantial heterogeneity of the U-Pu (so Am) distribution for the other. The difference in cation distribution was linked to a difference in Am chemistry as investigated by XAS, with Am being present at mixed +III/+IV oxidation state in the heterogeneous compound, whereas only Am(IV) was observed in the homogeneous compound. Previously reported discrepancies on Am oxidation states can hence be explained by cation distribution homogeneity effects.

Investigation of the Performance of D 2O-Cooled High-Conversion Reactors for Fuel Cycle Calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hiruta, Hikaru; Youinou, Gilles

2013-09-01

This report presents FY13 activities for the analysis of D 2O cooled tight-pitch High-Conversion PWRs (HCPWRs) with U-Pu and Th-U fueled cores aiming at break-even or near breeder conditions while retaining the negative void reactivity. The analyses are carried out from several aspects which could not be covered in FY12 activities. SCALE 6.1 code system is utilized, and a series of simple 3D fuel pin-cell models are developed in order to perform Monte Carlo based criticality and burnup calculations. The performance of U-Pu fueled cores with axial and internal blankets is analyzed in terms of their impact on the relativemore » fissile Pu mass balance, initial Pu enrichment, and void coefficient. In FY12, Pu conversion performances of D 2O-cooled HCPWRs fueled with MOX were evaluated with small sized axial/internal DU blankets (approximately 4cm of axial length) in order to ensure the negative void reactivity, which evidently limits the conversion performance of HCPWRs. In this fiscal year report, the axial sizes of DU blankets are extended up to 30 cm in order to evaluate the amount of DU necessary to reach break-even and/or breeding conditions. Several attempts are made in order to attain the milestone of the HCPWR designs (i.e., break-even condition and negative void reactivity) by modeling of HCPWRs under different conditions such as boiling of D 2O coolant, MOX with different 235U enrichment, and different target burnups. A similar set of analyses are performed for Th-U fueled cores. Several promising characteristics of 233U over other fissile like 239Pu and 235U, most notably its higher fission neutrons per absorption in thermal and epithermal ranges combined with lower ___ in the fast range than 239Pu allows Th-U cores to be taller than MOX ones. Such an advantage results in 4% higher relative fissile mass balance than that of U-Pu fueled cores while retaining the negative void reactivity until the target burnup of 51 GWd/t. Several other distinctions between U-Pu and Th-U fueled cores are identified by evaluating the sensitivity coefficients of keff, mass balance, and void coefficient. The effect of advanced iron alloy cladding (i.e., FeCrAl) on the performance of Pu conversion in MOX fueled cores is studied instead of using standard stainless-steel cladding. Variations in clad thickness and coolant-to-fuel volume ratio are also exercised. The use of FeCrAl instead of SS as a cladding alloy reduces the required Pu enrichment and improves the Pu conversion rate primarily due to the absence of nickel in the cladding alloy that results in the reduction of the neutron absorption. Also the difference in void coefficients between SS and FeCrAl alloys is nearly 500 pcm over the entire burnup range. The report also shows sensitivity and uncertainty analyses in order to characterize D 2O cooled HCPWRs from different aspects. The uncertainties of integral parameters (keff and void coefficient) for selected reactor cores are evaluated at different burnup points in order to find similarities and trends respect to D 2O-HCPWR.« less

Airborne Plutonium and non-natural Uranium from the Fukushima DNPP found at 120 km distance a few days after reactor hydrogen explosions.

PubMed

Shinonaga, Taeko; Steier, Peter; Lagos, Markus; Ohkura, Takehisa

2014-04-01

Plutonium (Pu) and non-natural uranium (U) originating from the Fukushima Daiichi Nuclear Power Plant (FDNPP) were identified in the atmosphere at 120 km distance from the FDNPP analyzing the ratio of number of atoms, following written as n(isotope)/n(isotope), of Pu and U. The n((240)Pu)/n((239)Pu), n((241)Pu)/n((239)Pu), n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U) in aerosol samples collected before and after the FDNPP incident were analyzed by accelerator mass spectrometry (AMS) and inductively coupled plasma mass spectrometry (ICPMS). The activity concentrations of (137)Cs and (134)Cs in the same samples were also analyzed by gamma spectrometry before the destructive analysis. Comparing the time series of analytical data on Pu and U obtained in this study with previously reported data on Pu, U, and radioactive Cs, we concluded that Pu and non-natural U from the FDNPP were transported in the atmosphere directly over a 120 km distance by aerosol and wind within a few days after the reactor hydrogen explosions. Effective dose of Pu were calculated using the data of Pu: (130 ± 21) nBq/m(3), obtained in this study. We found that the airborne Pu contributes only negligibly to the total dose at the time of the incident. However the analytical results show that the amount of Pu and non-natural U certainly increased in the environment after the incident.

Time-resolved record of 236U and 239,240Pu isotopes from a coral growing during the nuclear testing program at Enewetak Atoll (Marshall Islands).

PubMed

Froehlich, M B; Chan, W Y; Tims, S G; Fallon, S J; Fifield, L K

2016-12-01

A comprehensive series of nuclear tests were carried out by the United States at Enewetak Atoll in the Marshall Islands, especially between 1952 and 1958. A Porites Lutea coral that was growing in the Enewetak lagoon within a few km of all of the high-yield tests contains a continuous record of isotopes, which are of interest (e.g. 14 C, 236 U, 239,240 Pu) through the testing period. Prior to the present work, 14 C measurements at ∼2-month resolution had shown pronounced peaks in the Δ 14 C data that coincided with the times at which tests were conducted. Here we report measurements of 236 U and 239,240 Pu on the same coral using accelerator mass spectrometry, and again find prominent peaks in the concentrations of these isotopes that closely follow those in 14 C. Consistent with the 14 C data, the magnitudes of these peaks do not, however, correlate well with the explosive yields of the corresponding tests, indicating that smaller tests probably contributed disproportionately to the debris that fell in the lagoon. Additional information about the different tests can also be obtained from the 236 U/ 239 Pu and 240 Pu/ 239 Pu ratios, which are found to vary dramatically over the testing period. In particular, the first thermonuclear test, Ivy-Mike, has characteristic 236 U/ 239 Pu and 240 Pu/ 239 Pu signatures which are diagnostic of the first arrival of nuclear test material in various archives. Copyright © 2016 Elsevier Ltd. All rights reserved.

Electronic and Magnetic Properties of Cd-Doped PuRhIn5

NASA Astrophysics Data System (ADS)

Zhu, Jian-Xin

Since their discovery nearly a decade ago, plutonium-based superconductors have attracted considerable interest, which is now heightened by the latest discovery of superconductivity in other Pu-115 compounds. Within the generalized gradient approximation (GGA) of density functional theory and its combination with the dynamical mean-field theory, we present a study of electronic structure in the paramagnetic state of Cd-doped PuRhIn5. A doping-induced delocalization-localization transition is identified. In addition, the spin-polarized GGA-based total energy calculations are performed to determine the magnetic exchange interactions in the pristine PuRhIn5. The implication to the nature of quantum criticality is discussed. This work was carried out under the auspices of the National Nuclear Security Administration of the U.S. Department of Energy at LANL under Contract No. DE-AC52-06NA25396, and was supported by the LANL ASC Program.

Am phases in the matrix of a U–Pu–Zr alloy with Np, Am, and rare-earth elements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Janney, Dawn E.; Kennedy, J. Rory; Madden, James W.

2015-01-01

Phases and microstructures in the matrix of an as-cast U-Pu-Zr alloy with 3 wt% Am, 2% Np, and 8% rare-earth elements were characterized by scanning and transmission electron microscopy. The matrix consists primarily of two phases, both of which contain Am: ζ-(U, Np, Pu, Am) (~70 at% U, 5% Np, 14% Pu, 1% Am, and 10% Zr) and δ-(U, Np, Pu, Am)Zr 2 (~25% U, 2% Np, 10-15% Pu, 1-2% Am, and 55-60 at% Zr). These phases are similar to those in U-Pu-Zr alloys, although the Zr content in ζ-(U, Np, Pu, Am) is higher than that in ζ-(U, Pu)more » and the Zr content in δ-(U, Np, Pu, Am)Zr 2 is lower than that in δ-UZr 2. Nanocrystalline actinide oxides with structures similar to UO2 occurred in some areas, but may have formed by reactions with the atmosphere during sample handling. Planar features consisting of a central zone of ζ-(U, Np, Pu, Am) bracketed by zones of δ-(U, Np, Pu, Am)Zr 2 bound irregular polygons ranging in size from a few micrometers to a few tens of micrometers across. The rest of the matrix consists of elongated domains of ζ-(U, Np, Pu, Am) and δ-(U, Np, Pu, Am)Zr 2. Each of these domains is a few tens of nanometers across and a few hundred nanometers long. The domains display strong preferred orientations involving areas a few hundred nanometers to a few micrometers across.« less

Microbial mobilization of plutonium and other actinides from contaminated soil

DOE PAGES

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

2015-12-01

Here we examined the dissolution of Pu, U, and Am in contaminated soil from the Nevada Test Site (NTS) due to indigenous microbial activity. Scanning transmission x-ray microscopy (STXM) analysis of the soil showed that Pu was present in its polymeric form and associated with Fe- and Mn- oxides and aluminosilicates. Uranium analysis by x-ray diffraction (μ-XRD) revealed discrete U-containing mineral phases, viz., schoepite, sharpite, and liebigite; synchrotron x-ray fluorescence (μ-XRF) mapping showed its association with Fe- and Ca-phases; and μ-x-ray absorption near edge structure (μ-XANES) confirmed U(IV) and U(VI) oxidation states. Addition of citric acid or glucose to themore » soil and incubated under aerobic or anaerobic conditions enhanced indigenous microbial activity and the dissolution of Pu. Detectable amount of Am and no U was observed in solution. In the citric acid-amended sample, Pu concentration increased with time and decreased to below detection levels when the citric acid was completely consumed. In contrast, with glucose amendment, Pu remained in solution. Pu speciation studies suggest that it exists in mixed oxidation states (III/IV) in a polymeric form as colloids. Although Pu(IV) is the most prevalent and generally considered to be more stable chemical form in the environment, our findings suggest that under the appropriate conditions, microbial activity could affect its solubility and long-term stability in contaminated environments.« less

Microbial mobilization of plutonium and other actinides from contaminated soil

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

Here we examined the dissolution of Pu, U, and Am in contaminated soil from the Nevada Test Site (NTS) due to indigenous microbial activity. Scanning transmission x-ray microscopy (STXM) analysis of the soil showed that Pu was present in its polymeric form and associated with Fe- and Mn- oxides and aluminosilicates. Uranium analysis by x-ray diffraction (μ-XRD) revealed discrete U-containing mineral phases, viz., schoepite, sharpite, and liebigite; synchrotron x-ray fluorescence (μ-XRF) mapping showed its association with Fe- and Ca-phases; and μ-x-ray absorption near edge structure (μ-XANES) confirmed U(IV) and U(VI) oxidation states. Addition of citric acid or glucose to themore » soil and incubated under aerobic or anaerobic conditions enhanced indigenous microbial activity and the dissolution of Pu. Detectable amount of Am and no U was observed in solution. In the citric acid-amended sample, Pu concentration increased with time and decreased to below detection levels when the citric acid was completely consumed. In contrast, with glucose amendment, Pu remained in solution. Pu speciation studies suggest that it exists in mixed oxidation states (III/IV) in a polymeric form as colloids. Although Pu(IV) is the most prevalent and generally considered to be more stable chemical form in the environment, our findings suggest that under the appropriate conditions, microbial activity could affect its solubility and long-term stability in contaminated environments.« less

Multiscale Speciation of U and Pu at Chernobyl, Hanford, Los Alamos, McGuire AFB, Mayak, and Rocky Flats.

PubMed

Batuk, Olga N; Conradson, Steven D; Aleksandrova, Olga N; Boukhalfa, Hakim; Burakov, Boris E; Clark, David L; Czerwinski, Ken R; Felmy, Andrew R; Lezama-Pacheco, Juan S; Kalmykov, Stepan N; Moore, Dean A; Myasoedov, Boris F; Reed, Donald T; Reilly, Dallas D; Roback, Robert C; Vlasova, Irina E; Webb, Samuel M; Wilkerson, Marianne P

2015-06-02

The speciation of U and Pu in soil and concrete from Rocky Flats and in particles from soils from Chernobyl, Hanford, Los Alamos, and McGuire Air Force Base and bottom sediments from Mayak was determined by a combination of X-ray absorption fine structure (XAFS) spectroscopy and X-ray fluorescence (XRF) element maps. These experiments identify four types of speciation that sometimes may and other times do not exhibit an association with the source terms and histories of these samples: relatively well ordered PuO2+x and UO2+x that had equilibrated with O2 and H2O under both ambient conditions and in fires or explosions; instances of small, isolated particles of U as UO2+x, U3O8, and U(VI) species coexisting in close proximity after decades in the environment; alteration phases of uranyl with other elements including ones that would not have come from soils; and mononuclear Pu-O species and novel PuO2+x-type compounds incorporating additional elements that may have occurred because the Pu was exposed to extreme chemical conditions such as acidic solutions released directly into soil or concrete. Our results therefore directly demonstrate instances of novel complexity in the Å and μm-scale chemical speciation and reactivity of U and Pu in their initial formation and after environmental exposure as well as occasions of unexpected behavior in the reaction pathways over short geological but significant sociological times. They also show that incorporating the actual disposal and site conditions and resultant novel materials such as those reported here may be necessary to develop the most accurate predictive models for Pu and U in the environment.

Oxygen potential of (U 0.88Pu 0.12)O 2±x and (U 0.7Pu 0.3)O 2±x at high temperatures of 1673-1873 K

NASA Astrophysics Data System (ADS)

Kato, M.; Takeuchi, K.; Uchida, T.; Sunaoshi, T.; Konashi, K.

2011-07-01

The oxygen potential of (U 0.88Pu 0.12)O 2±x (-0.0119 < x < 0.0408) and (U 0.7Pu 0.3)O 2±x (-0.0363 < x < 0.0288) was measured at high temperatures of 1673-1873 K using gas equilibrium method with thermo gravimeter. The measured data were analyzed by a defect chemistry model. Expressions were derived to represent the oxygen potential based on defect chemistry as functions of temperature and oxygen-to-metal ratio. The thermodynamic data, ΔG, ΔH and ΔS, at stoichiometric composition were obtained. The expressions can be used for in situ determination of the oxygen-to-metal ratio by the gas-equilibration method. The calculation results were consistent with measured data. It was estimated that addition of 1 wt.% Pu content increased oxygen potential of uranium and plutonium mixed oxide by 2-5 kJ/mol.

The efficacy of denaturing actinide elements as a means of decreasing materials attractiveness

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hase, K.R.; Bathke, C.G.; Ebbinghaus, B.B.

2013-07-01

This study considers the concept of denaturing as applied to the actinide elements present in spent fuel as a means to reduce materials attractiveness. Highly attractive materials generally have low values of bare critical mass, heat content, and dose. To denature an attractive element, its spent-fuel isotopic composition (isotopic vector) is intentionally modified by introducing sufficient quantities of a significantly less attractive isotope to dilute the concentration of a highly attractive isotope so that the overall attractiveness of the element is reduced. The authors used FOM (Figure of Merit) formula as the material attractiveness metric for their parametric determination ofmore » the attractiveness of the Pu and U. Materials attractiveness needs to be considered in three distinct phases in the process to construct a nuclear explosive device (NED): the acquisition phase, processing phase, and utilization phase. The results show that denaturing uranium with {sup 238}U is actually an effective means of reducing the attractiveness. For uranium with a large minority of {sup 235}U, a mixture of 80% {sup 238}U to 20% {sup 235}U is required to reduce the attractiveness to low. For uranium with a large concentration of {sup 233}U, a mixture of 88% {sup 238}U to 12% {sup 233}U is required to reduce the attractiveness to low. The results also show that denaturing plutonium with {sup 238}Pu is less effective than denaturing uranium with {sup 238}U. Using {sup 238}Pu as the denaturing agent would require 80% or more by mass in order to reduce the attractiveness to low. No amount of {sup 240}Pu is enough to reduce the plutonium attractiveness below medium. The combination of {sup 238}Pu and {sup 240}Pu would require approximately 70% {sup 238}Pu and 25% {sup 240}Pu by mass to reduce the plutonium attractiveness to low.« less

Characterization of DWPF recycle condensate tank materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bannochie, C. J.

2015-01-01

A Defense Waste Processing Facility (DWPF) Recycle Condensate Tank (RCT) sample was delivered to the Savannah River National Laboratory (SRNL) for characterization with particular interest in the concentration of I-129, U-233, U-235, total U, and total Pu. Since a portion of Salt Batch 8 will contain DWPF recycle materials, the concentration of I-129 is important to undertand for salt batch planning purposes. The chemical and physical characterizations are also needed as input to the interpretation of future work aimed at determining the propensity of the RCT material to foam, and methods to remediate any foaming potential. According to DWPF themore » Tank Farm 2H evaporator has experienced foaming while processing DWPF recycle materials. The characterization work on the RCT samples has been completed and is reported here. The composition of the Sludge Batch 8 (SB8) RCT material is largely a low base solution of 0.2M NaNO 2 and 0.1M NaNO 3 with a small amount of formate present. Insoluble solids comprise only 0.05 wt.% of the slurry. The solids appear to be largely sludge-like solids based on elemental composition and SEM-EDS analysis. The sample contains an elevated concentration of I-129 (38x) and substantial 59% fraction of Tc-99, as compared to the incoming SB8 Tank 40 feed material. The Hg concentration is 5x, when compared to Fe, of that expected based on sludge carryover. The total U and Pu concentrations are reduced significantly, 0.536 wt.% TS and 2.42E-03 wt.% TS, respectively, with the fissile components, U-233, U-235, Pu-239, and Pu-241, an order of magnitude lower in concentration than those in the SB8 Tank 40 DWPF feed material. This report will be revised to include the foaming study requested in the TTR and outlined in the TTQAP when that work is concluded.« less

Nondestructive assay of EBR-II blanket elements using resonance transmission analysis

NASA Astrophysics Data System (ADS)

Klann, Raymond Todd

1998-10-01

Resonance transmission analysis utilizing a filtered reactor beam was examined as a means of determining the 239Pu content in Experimental Breeder Reactor - II depleted uranium blanket elements. The technique uses cadmium and gadolinium filters along with a 239Pu fission chamber to isolate the 0.3 eV resonance in 239Pu. In the energy range of this resonance (0.1 eV to 0.5 eV), the total microscopic cross-section of 239Pu is significantly greater than the cross- sections of 238U and 235U. This large difference allows small changes in the 239Pu content of a sample to result in large changes in the mass signal response. Tests with small stacks of depleted uranium and 239Pu foils indicate a significant change in response based on the 239Pu content of the foil stack. In addition, the tests indicate good agreement between the measured and predicted values of 239Pu up to approximately two weight percent.

Precise U and Pu isotope ratio measurements in nuclear samples by hyphenating capillary electrophoresis and MC-ICPMS.

PubMed

Martelat, Benoit; Isnard, Helene; Vio, Laurent; Dupuis, Erwan; Cornet, Terence; Nonell, Anthony; Chartier, Frederic

2018-06-22

Precise isotopic and elemental characterization of spent nuclear fuel is a major concern for the validation of the neutronic calculation codes and waste management strategy in the nuclear industry. Generally, the elements of interest, particularly U and Pu which are the two major elements present in spent fuel, are purified by ion exchange or extractant resins before off-line measurements by thermal ionization mass spectrometry. The aim of the present work was to develop a new analytical approach based on capillary electrophoresis (CE) hyphenated to a multicollector inductively coupled plasma mass spectrometer (MC-ICPMS) for online isotope ratio measurements. An electrophoretic separation protocol of U, Pu and the fraction containing fission products and minor actinides (Am and Cm) was developed using acetic acid as the electrolyte and complexing agent. The instrumentation for CE was designed to be used in a glove box and a laboratory-built interface was developed for hyphenation with MC-ICPMS. The separation was realized with only a few nL of a solution of spent nuclear fuel and the reproducibilities obtained on the U and Pu isotope ratios were on the order of a few ‰ which is comparable to those obtained by thermal ionization mass spectrometer (TIMS). This innovative protocol allowed a tremendous reduction of the analyte masses from μg to ng and also a drastic reduction of the liquid waste production from mL to μL. In addition, the time of analysis was shorted by at least a factor three. All of these improved parameters are of major interest for nuclear applications.

Isolation of 236U and 239,240Pu from seawater samples and its determination by Accelerator Mass Spectrometry.

PubMed

López-Lora, Mercedes; Chamizo, Elena; Villa-Alfageme, María; Hurtado-Bermúdez, Santiago; Casacuberta, Núria; García-León, Manuel

2018-02-01

In this work we present and evaluate a radiochemical procedure optimised for the analysis of 236 U and 239,240 Pu in seawater samples by Accelerator Mass Spectrometry (AMS). The method is based on Fe(OH) 3 co-precipitation of actinides and uses TEVA® and UTEVA® extraction chromatography resins in a simplified way for the final U and Pu purification. In order to improve the performance of the method, the radiochemical yields are analysed in 1 to 10L seawater volumes using alpha spectrometry (AS) and Inductively Coupled Plasma Mass Spectrometry (ICP-MS). Robust 80% plutonium recoveries are obtained; however, it is found that Fe(III) concentration in the precipitation solution and sample volume are the two critical and correlated parameters influencing the initial uranium extraction through Fe(OH) 3 co-precipitation. Therefore, we propose an expression that optimises the sample volume and Fe(III) amounts according to both the 236 U and 239,240 Pu concentrations in the samples and the performance parameters of the AMS facility. The method is validated for the current setup of the 1MV AMS system (CNA, Sevilla, Spain), where He gas is used as a stripper, by analysing a set of intercomparison seawater samples, together with the Laboratory of Ion Beam Physics (ETH, Zürich, Switzerland). Copyright © 2017 Elsevier B.V. All rights reserved.

Extended optical model for fission

DOE PAGES

Sin, M.; Capote, R.; Herman, M. W.; ...

2016-03-07

A comprehensive formalism to calculate fission cross sections based on the extension of the optical model for fission is presented. It can be used for description of nuclear reactions on actinides featuring multi-humped fission barriers with partial absorption in the wells and direct transmission through discrete and continuum fission channels. The formalism describes the gross fluctuations observed in the fission probability due to vibrational resonances, and can be easily implemented in existing statistical reaction model codes. The extended optical model for fission is applied for neutron induced fission cross-section calculations on 234,235,238U and 239Pu targets. A triple-humped fission barrier ismore » used for 234,235U(n,f), while a double-humped fission barrier is used for 238U(n,f) and 239Pu(n,f) reactions as predicted by theoretical barrier calculations. The impact of partial damping of class-II/III states, and of direct transmission through discrete and continuum fission channels, is shown to be critical for a proper description of the measured fission cross sections for 234,235,238U(n,f) reactions. The 239Pu(n,f) reaction can be calculated in the complete damping approximation. Calculated cross sections for 235,238U(n,f) and 239Pu(n,f) reactions agree within 3% with the corresponding cross sections derived within the Neutron Standards least-squares fit of available experimental data. Lastly, the extended optical model for fission can be used for both theoretical fission studies and nuclear data evaluation.« less

High temperature investigation of the solid/liquid transition in the PuO2-UO2-ZrO2 system

NASA Astrophysics Data System (ADS)

Quaini, A.; Guéneau, C.; Gossé, S.; Sundman, B.; Manara, D.; Smith, A. L.; Bottomley, D.; Lajarge, P.; Ernstberger, M.; Hodaj, F.

2015-12-01

The solid/liquid transitions in the quaternary U-Pu-Zr-O system are of great interest for the analysis of core meltdown accidents in Pressurised Water Reactors (PWR) fuelled with uranium-dioxide and MOX. During a severe accident the Zr-based cladding can become completely oxidised due to the interaction with the oxide fuel and the water coolant. In this framework, the present analysis is focused on the pseudo-ternary system UO2-PuO2-ZrO2. The melting/solidification behaviour of five pseudo-ternary and one pseudo-binary ((PuO2)0.50(ZrO2)0.50) compositions have been investigated experimentally by a laser heating method under pre-set atmospheres. The effects of an oxidising or reducing atmosphere on the observed melting/freezing temperatures, as well as the amount of UO2 in the sample, have been clearly identified for the different compositions. The oxygen-to-metal ratio is a key parameter affecting the melting/freezing temperature because of incongruent vaporisation effects. In parallel, a detailed thermodynamic model for the UO2-PuO2-ZrO2 system has been developed using the CALPHAD method, and thermodynamic calculations have been performed to interpret the present laser heating results, as well as the high temperature behaviour of the cubic (Pu,U,Zr)O2±x-c mixed oxide phase. A good agreement was obtained between the calculated and experimental data points. This work enables an improved understanding of the major factors relevant to severe accident in nuclear reactors.

European roe deer antlers as an environmental archive for fallout (236)U and (239)Pu.

PubMed

Froehlich, M B; Steier, P; Wallner, G; Fifield, L K

2016-01-01

Anthropogenic (236)U and (239)Pu were measured in European roe deer antlers hunted between 1955 and 1977 which covers and extends beyond the period of intensive nuclear weapons testing (1954-1962). The antlers were hunting trophies, and hence the hunting area, the year of shooting and the approximate age of each animal is given. Uranium and plutonium are known to deposit in skeletal tissue. Since antler histology is similar to bone, both elements were expected in antlers. Furthermore, roe deer shed their antlers annually, and hence antlers may provide a time-resolved environmental archive for fallout radionuclides. The radiochemical procedure is based on a Pu separation step by anion exchange (Dowex 1 × 8) and a subsequent U purification by extraction chromatography using UTEVA(®). The samples were measured by Accelerator Mass Spectrometry at the VERA facility (University of Vienna). In addition to the (236)U and (239)Pu concentrations, the (240)Pu/(239)Pu isotopic ratios were determined with a mean value of 0.172 ± 0.023 which is in agreement with the ratio of global fallout (∼0.18). Rather high (236)U/(238)U ratios of the order of 10(-6) were observed. These measured ratios, where the (236)U arises only from global fallout, have implications for the use of the (236)U/(238)U ratio as a fingerprint for nuclear accidents or releases from nuclear facilities. Our investigations have shown the potential to use antlers as a temporally resolved archive for the uptake of actinides from the environment. Copyright © 2015 Elsevier Ltd. All rights reserved.

Recovery of UO{sub 2}/PuO{sub 2} in IFR electrorefining process

DOEpatents

Tomczuk, Z.; Miller, W.E.

1992-01-01

This invention is comprised of a process for converting PuO{sub 2} and U0{sub 2} present in an electrorefiner to the chlorides, by contacting the PuO{sub 2} and U0{sub 2} with Li metal in the presence of an alkali metal chloride salt substantially free of rare earth and actinide chlorides for a time and at a temperature sufficient to convert the U0{sub 2} and PuO{sub 2} to metals while converting Li metal to Li{sub 2}O. Li{sub 2}O is removed either by reducing with rare earth metals or by providing an oxygen electrode for transporting 0{sub 2} out of the electrorefiner and a cathode, and thereafter applying an emf to the electrorefiner electrodes sufficient to cause the Li{sub 2}O to disassociate to 0{sub 2} and Li metal but insufficient to decompose the alkali metal chloride salt. The U and Pu and excess lithium are then converted to chlorides by reaction with CdCl{sub 2}.

Episode 49 of the Pu'u 'Ō'ō-Kūpaianaha eruption of Kilauea volcano-breakdown of a steady-state eruptive era

USGS Publications Warehouse

Mangan, M.T.; Heliker, C.C.; Mattox, T.N.; Kauahikaua, J.P.; Helz, R.T.

1995-01-01

The Pu'u 'O'o-Kupaianaha eruption (1983-present) is the longest lived rift eruption of either Kilauea or neighboring Mauna Loa in recorded history. The initial fissure opening in January 1983 was followed by three years of episodic fire fountaining at the Pu'u 'O'o vent on Kilauea's east rift zone ∼19km from the summit (episodes 4–47). These spectacular events gave way in July 1986 to five and a half years of near-continuous, low-level effusion from the Kupaianaha vent, ∼ 3km to the cast (episode 48). A 49th episode began in November 1991 with the opening of a new fissure between Pu'u 'O'o and Kupaianaha. This three week long outburst heralded an era of more erratic eruptive behavior characterized by the shut down of Kupaianaha in February 1992 and subsequent intermittent eruption from vents on the west flank of Pu'u 'O'o (episodes 50 and 51). The events occurring over this period are due to progressive shrinkage of the rift-zone reservoir beneath the eruption site, and had limited impact on eruption temperatures and lava composition.

Episode 49 of the Pu'u 'O'o-Kupaianaha eruption of Kilauea volcano - breakdown of a steady-state eruptive era

NASA Astrophysics Data System (ADS)

Mangan, M. T.; Heliker, C. C.; Mattox, T. N.; Kauahikaua, J. P.; Helz, R. T.

1995-04-01

The Pu'u 'O'o-Kupaianaha eruption (1983-present) is the longest lived rift eruption of either Kilauea or neighboring Mauna Loa in recorded history. The initial fissure opening in January 1983 was followed by three years of episodic fire fountaining at the Pu'u 'O'o vent on Kilauea's east rift zone ˜19km from the summit (episodes 4 47). These spectacular events gave way in July 1986 to five and a half years of nearcontinuous, low-level effusion from the Kupaianaha vent, ˜ 3km to the cast (episode 48). A 49th episode began in November 1991 with the opening of a new fissure between Pu'u 'O'o and Kupaianaha. this three week long outburst heralded an era of more erratic eruptive behavior characterized by the shut down of Kupaianaha in February 1992 and subsequent intermittent eruption from vents on the west flank of Pu'u 'O'o (episodes 50 and 51). The events occurring over this period are due to progressive shrinkage of the rift-zone reservoir beneath the eruption site, and had limited impact on eruption temperatures and lava composition.

Maps showing the development of the Pu'u 'O'o-Kupaianaha flow field, June 1984-February 1987, Kilauea Volcano, Hawaii

USGS Publications Warehouse

Heliker, Christina; Ulrich, George E.; Margriter, Sandy C.; Hoffmann, John P.

2001-01-01

The Pu'u 'O'o - Kupaianaha eruption on the middle east rift zone of Kilauea began in January 1983 with intermittent activity along several fissures. By June 1983, the eruption had localized at the Pu'u 'O'o vent, and the activity settled into an increasingly regular pattern of brief eruptive episodes characterized by high lava fountains. The first 18 months of this eruption are chronicled in Wolfe and others (1988), which includes maps of the flows erupted in episodes 1-20. The maps presented here extend this series through the beginning of episode 48.

DOE Office of Scientific and Technical Information (OSTI.GOV)

R. Wigeland; T. Taiwo; M. Todosow

The recently completed comprehensive evaluation and screening of nuclear fuel cycle options identified a number of potentially promising fuel cycles for R&D that offer what could be considered by decision-makers as having the potential for significant improvement compared to the current U.S. fuel cycle. The fuel cycles that consistently performed the best were recycle fuel cycles that used self-sustaining fast reactors operating with either U/Pu or U/TRU recycle fuel and also included options where the fast reactors provided fissile materials to support operation of thermal reactors. However, based on the evaluation criteria and metrics used in the study, there wasmore » no difference in benefit between recycle of U/Pu and U/TRU (where TRU is plutonium and the minor actinides) while there were differences in the challenges for developing and deploying such fuel cycles, with U/TRU recycle being more challenging. This observation prompted the question as to the desirability of pursuing R&D on U/TRU recycle given that there may not be an increase in benefit. As a result, activities have been pursued to further investigate the performance differences between U/Pu and U/TRU recycle based on considering issues beyond those used in the evaluation and screening study to identify, if possible, areas where there are significant benefits of U/TRU recycle compared to U/Pu recycle. These new considerations focused on several areas, but especially on the impact on disposal of the HLW, which in the case of U/Pu recycle contains all of the minor actinides along with fission products, while in the case of U/TRU recycle only contains the losses of minor actinides from the reprocessing and recycle fuel fabrication operations. This difference in content has several implications. One impact is on the time dependent decay heat which can affect handling and the use of space in a geologic repository. Another impact concerns the HLW form and volume, since presence of minor actinides may adversely affect the ability to reduce HLW volume. The short-term radioactivity and long-term radiotoxicity of the HLW is also affected, which may be of more or less importance depending on the specific geologic disposal environment. To study these potential effects, a range of waste forms and disposal environments were used in the analysis, documenting to what extent the recycle of minor actinides in addition to plutonium may offer further benefit. Another area of investigation concerned the recycle fuel, for the fast reactor and for the thermal reactors they may support. Information to date indicates that U/Pu fuel may be simpler to fabricate and has a much more extensive database than U/TRU fuel, one of the reasons for the increased challenge for developing and deploying a U/TRU fuel cycle, and also indicates that heterogeneous recycle of the minor actinides may be even more difficult as compared to homogeneous recycle. This information was reviewed and updated to reflect the most recent studies for the purpose of informing on all aspects of the differences between U/Pu and U/TRU recycle. The results of all of these investigations will be presented to provide information on the findings concerning the value of U/TRU recycle.« less

Depth profile of 236U/238U in soil samples in La Palma, Canary Islands

PubMed Central

Srncik, M.; Steier, P.; Wallner, G.

2011-01-01

The vertical distribution of the 236U/238U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the 240Pu/239Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios 236U/238U, 240Pu/239Pu and 236U/239Pu, respectively. The 236U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio 240Pu/239Pu indicated a global fallout signature we assume the same origin as the probable source for 236U. Our measured 236U/239Pu value of around 0.2 is within the expected range for this contamination source. PMID:21481502

Electrowinning of U-Pu onto inert solid cathode in LiCl-KCl eutectic melts containing UCl3 and PuCl3

NASA Astrophysics Data System (ADS)

Sakamura, Yoshiharu; Murakami, Tsuyoshi; Tada, Kohei; Kitawaki, Shinichi

2018-04-01

Electrowinning process was investigated for extracting actinides from molten salts used for the pyrochemical reprocessing of spent nuclear fuels. The separation of actinides from lanthanides is expected to be enhanced by employing inert solid cathodes due to larger potential differences on these cathodes. In this study, the co-deposition behavior of Pu and U metals onto an inert solid cathode made of tungsten was examined in LiCl-KCl eutectic melts containing UCl3 and PuCl3 at 773 K. The standard potential of U3+/U is 0.31 V more positive than that of Pu3+/Pu. The U3+ concentration was varied in the range of 0.11-0.66 wt%, while the Pu3+ concentration was maintained at approximately 2.9 wt%. When the U3+ concentration was not sufficiently low, the deposited U metal readily grew outward from the electrode surface and the electrode surface area rapidly increased, which facilitated only the deposition of U metal. It was estimated that metallic Pu can be efficiently collected along with U at U3+ concentrations lower than ∼0.2 wt%.

Optimization of hybrid-type instrumentation for Pu accountancy of U/TRU ingot in pyroprocessing.

PubMed

Seo, Hee; Won, Byung-Hee; Ahn, Seong-Kyu; Lee, Seung Kyu; Park, Se-Hwan; Park, Geun-Il; Menlove, Spencer H

2016-02-01

One of the final products of pyroprocessing for spent nuclear fuel recycling is a U/TRU ingot consisting of rare earth (RE), uranium (U), and transuranic (TRU) elements. The amounts of nuclear materials in a U/TRU ingot must be measured as precisely as possible in order to secure the safeguardability of a pyroprocessing facility, as it contains the most amount of Pu among spent nuclear fuels. In this paper, we propose a new nuclear material accountancy method for measurement of Pu mass in a U/TRU ingot. This is a hybrid system combining two techniques, based on measurement of neutrons from both (1) fast- and (2) thermal-neutron-induced fission events. In technique #1, the change in the average neutron energy is a signature that is determined using the so-called ring ratio method, according to which two detector rings are positioned close to and far from the sample, respectively, to measure the increase of the average neutron energy due to the increased number of fast-neutron-induced fission events and, in turn, the Pu mass in the ingot. We call this technique, fast-neutron energy multiplication (FNEM). In technique #2, which is well known as Passive Neutron Albedo Reactivity (PNAR), a neutron population's changes resulting from thermal-neutron-induced fission events due to the presence or absence of a cadmium (Cd) liner in the sample's cavity wall, and reflected in the Cd ratio, is the signature that is measured. In the present study, it was considered that the use of a hybrid, FNEM×PNAR technique would significantly enhance the signature of a Pu mass. Therefore, the performance of such a system was investigated for different detector parameters in order to determine the optimal geometry. The performance was additionally evaluated by MCNP6 Monte Carlo simulations for different U/TRU compositions reflecting different burnups (BU), initial enrichments (IE), and cooling times (CT) to estimate its performance in real situations. Copyright © 2015 Elsevier Ltd. All rights reserved.

Corrective Action Decision Document/Closure Report for Corrective Action Unit 482: Area 15 U15a/e Muckpiles and Ponds Nevada Test Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

NSTec Environmental Restoration

This Corrective Action Decision Document /Closure Report (CADD/CR) was prepared by the Defense Threat Reduction Agency (DTRA) for Corrective Action Unit (CAU) 482 U15a/e Muckpiles and Ponds. This CADD/CR is consistent with the requirements of the Federal Facility Agreement and Consent Order agreed to by the State of Nevada, the U.S. Department of Energy, and the U.S. Department of Defense. Corrective Action Unit 482 is comprised of three Corrective Action Sites (CASs) and one adjacent area: CAS 15-06-01, U15e Muckpile; CAS 15-06-02, U15a Muckpile; CAS 15-38-01, Area 15 U15a/e Ponds; and Drainage below the U15a Muckpile. The purpose of thismore » CADD/CR is to provide justification and documentation supporting the recommendation for closure with no further corrective action, by placing use restrictions on the three CASs and the adjacent area of CAU 482. To support this recommendation, a corrective action investigation (CAI) was performed in September 2002. The purpose of the CAI was to fulfill the following data needs as defined during the Data Quality Objective (DQO) process: (1) Determine whether contaminants of concern (COCs) are present. (2) If COCs are present, determine their nature and extent. (3) Provide sufficient information and data to determine appropriate corrective actions. The CAU 482 dataset from the CAI was evaluated based on the data quality indicator parameters. This evaluation demonstrated the quality and acceptability of the dataset for use in fulfilling the DQO data needs. Analytes detected during the CAI were evaluated against final action levels (FALs) established in this document. Tier 2 FALS were determined for the hazardous constituents of total petroleum hydrocarbons (TPH)-diesel-range organics (DRO) and the radionuclides americium (Am)-241, cesium (Cs)-137, plutonium (Pu)-238, and Pu-239. The Tier 2 FALs were calculated for the radionuclides using site-specific information. The hazardous constituents of TPH-DRO were compared to the PALs defined in the CAIP, and because none of the preliminary action levels (PALs) were exceeded, the PALs became the FALs. The radionuclide FALs were calculated using the Residual Radioactive (RESRAD) code (version 6.21). The RESRAD calculation determined the activities of all radionuclides that together would sum to an exposure dose of 25 millirem per year to a site receptor (based on their relative abundances at each CAS). Based on the field investigation, the following contaminants were determined to be present at concentrations exceeding their corresponding FALs: (1) CAS 15-06-01 - None. (2) CAS 15-06-02 - Cs-137 and Pu-239. (3) CAS 15-38-01 - Am-241, Cs-137, Pu-238, and Pu-239. (4) Drainage below CAS 15-06-02 - Cs-137 and Pu-239. Based on the data and risk evaluations, the DQO data needs presented in the Corrective Action Investigation Plan were met, and the data accurately represent the radiological and chemical risk present at CAU 482. Based on the results of the CAI data evaluation, it was determined that closure in place with use restrictions is the appropriate corrective action for CAU 482 and that use restrictions will effectively control exposure to future land users. This is based on the fact that even though the FALs were exceeded in a few samples, this remote, controlled access site poses only limited risk overall to public health and the environment. Given the relatively low levels of contamination present, it would create a greater hazard to worker safety, public health, and the environment to remove the contamination, transport it, and bury it at another location. Therefore, DTRA provides the following recommendations: (1) Close COCs in place at CAS 15-06-02, CAS 15-38-01, and the drainage below CAS 15-06-02 with use restrictions. (2) No further action for CAU 482. (3) A Notice of Completion be issued to DTRA by the Nevada Division of Environmental Protection for closure of CAU 482. (4) Move CAU 482 from Appendix III to Appendix IV of the Federal Facility Agreement and Consent Order.« less

Long-range tropospheric transport of uranium and plutonium weapons fallout from Semipalatinsk nuclear test site to Norway.

PubMed

Wendel, Cato Christian; Fifield, L Keith; Oughton, Deborah H; Lind, Ole Christian; Skipperud, Lindis; Bartnicki, Jerzy; Tims, Stephen G; Høibråten, Steinar; Salbu, Brit

2013-09-01

A combination of state-of-the-art isotopic fingerprinting techniques and atmospheric transport modelling using real-time historical meteorological data has been used to demonstrate direct tropospheric transport of radioactive debris from specific nuclear detonations at the Semipalatinsk test site in Kazakhstan to Norway via large areas of Europe. A selection of archived air filters collected at ground level at 9 stations in Norway during the most intensive atmospheric nuclear weapon testing periods (1957-1958 and 1961-1962) has been screened for radioactive particles and analysed with respect to the concentrations and atom ratios of plutonium (Pu) and uranium (U) using accelerator mass spectrometry (AMS). Digital autoradiography screening demonstrated the presence of radioactive particles in the filters. Concentrations of (236)U (0.17-23nBqm(-3)) and (239+240)Pu (1.3-782μBqm(-3)) as well as the atom ratios (240)Pu/(239)Pu (0.0517-0.237) and (236)U/(239)Pu (0.0188-0.7) varied widely indicating several different sources. Filter samples from autumn and winter tended to have lower atom ratios than those sampled in spring and summer, and this likely reflects a tropospheric influence in months with little stratospheric fallout. Very high (236)U, (239+240)Pu and gross beta activity concentrations as well as low (240)Pu/(239)Pu (0.0517-0.077), (241)Pu/(239)Pu (0.00025-0.00062) and (236)U/(239)Pu (0.0188-0.046) atom ratios, characteristic of close-in and tropospheric fallout, were observed in filters collected at all stations in Nov 1962, 7-12days after three low-yield detonations at Semipalatinsk (Kazakhstan). Atmospheric transport modelling (NOAA HYSPLIT_4) using real-time meteorological data confirmed that long range transport of radionuclides, and possibly radioactive particles, from Semipalatinsk to Norway during this period was plausible. The present work shows that direct tropospheric transport of fallout from atmospheric nuclear detonations periodically may have had much larger influence on radionuclide air concentrations and deposition than previously anticipated. Copyright © 2013 Elsevier Ltd. All rights reserved.

FCRD Advanced Reactor (Transmutation) Fuels Handbook

DOE Office of Scientific and Technical Information (OSTI.GOV)

Janney, Dawn Elizabeth; Papesch, Cynthia Ann

2016-09-01

Transmutation of minor actinides such as Np, Am, and Cm in spent nuclear fuel is of international interest because of its potential for reducing the long-term health and safety hazards caused by the radioactivity of the spent fuel. One important approach to transmutation (currently being pursued by the DOE Fuel Cycle Research & Development Advanced Fuels Campaign) involves incorporating the minor actinides into U-Pu-Zr alloys, which can be used as fuel in fast reactors. U-Pu-Zr alloys are well suited for electrolytic refining, which leads to incorporation rare-earth fission products such as La, Ce, Pr, and Nd. It is, therefore, importantmore » to understand not only the properties of U-Pu-Zr alloys but also those of U-Pu-Zr alloys with concentrations of minor actinides (Np, Am) and rare-earth elements (La, Ce, Pr, and Nd) similar to those in reprocessed fuel. In addition to requiring extensive safety precautions, alloys containing U, Pu, and minor actinides (Np and Am) are difficult to study for numerous reasons, including their complex phase transformations, characteristically sluggish phasetransformation kinetics, tendency to produce experimental results that vary depending on the histories of individual samples, rapid oxidation, and sensitivity to contaminants such as oxygen in concentrations below a hundred parts per million. Although less toxic, rare-earth elements such as La, Ce, Pr, and Nd are also difficult to study for similar reasons. Many of the experimental measurements were made before 1980, and the level of documentation for experimental methods and results varies widely. It is, therefore, not surprising that little is known with certainty about U-Pu-Zr alloys, particularly those that also contain minor actinides and rare-earth elements. General acceptance of results commonly indicates that there is only a single measurement for a particular property. This handbook summarizes currently available information about U, Pu, Zr, Np, Am, La, Ce, Pr, and Nd and alloys of two or three of these elements. It contains information about phase diagrams and related information (including phases and phase transformations); heat capacity, entropy, and enthalpy; thermal expansion; and thermal conductivity and diffusivity. In addition to presenting information about materials properties, the handbook attempts to provide information about how well the property is known and how much variation exists between measurements. Although it includes some results from models, its primary focus is experimental data. The Handbook is organized in two sections: one with information about the U-Pu-Zr ternary and one with information about other elements and binary and vi ternary alloys in the U-Np-Pu-Am-La-Ce-Pr-Nd-Zr system. Within each section, information about elements is presented first, followed by information about binary alloys, then information about ternary alloys. The order in which the elements in each alloy are mentioned follows the order in the first sentence of this paragraph. Much of the information on the U-Pu-Zr system repeats information from the FCRD Transmutation Fuels Handbook 2015. Most of the other data has been published elsewhere (although scattered throughout numerous references, some quite obscure); however, some data from Idaho National Laboratory is presented here for the first time. As the FCRD programmatic mission evolves, future editions of this handbook will begin to include other advanced reactor fuel designs and compositions. Hence, the title of the handbook will transition to the Advanced Reactor Fuels Handbook.« less

Determination of Plutonium Isotope Ratios at Very Low Levels by ICP-MS using On-Line Electrochemically Modulated Separations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liezers, Martin; Lehn, Scott A; Olsen, Khris B

2009-10-01

Electrochemically modulated separations (EMS) are shown to be a rapid and selective means of extracting and concentrating Pu from complex solutions prior to isotopic analysis by inductively coupled plasma mass spectrometry (ICP-MS). This separation is performed in a flow injection mode, on-line with the ICP-MS. A three-electrode, flow-by electrochemical cell is used to accumulate Pu at an anodized glassy carbon electrode by redox conversion of Pu(III) to Pu (IV&VI). The entire process takes place in 2% v/v (0.46M) HNO 3. No redox chemicals or acid concentration changes are required. Plutonium accumulation and release is redox dependent and controlled by themore » applied cell potential. Thus large transient volumetric concentration enhancements can be achieved. Based on more negative U(IV) potentials relative to Pu(IV), separation of Pu from uranium is efficient, thereby eliminating uranium hydride interferences. EMS-ICP-MS isotope ratio measurement performance will be presented for femtogram to attogram level plutonium concentrations.« less

Electronic, structural, and thermodynamic properties of mixed actinide dioxides (U, Pu, Am) O2 from hybrid density functional theory

NASA Astrophysics Data System (ADS)

Ma, Li; Ray, Asok K.

2010-03-01

As a continuation of our studies of pure actinide metals using hybrid density functional theory,footnotetextR. Atta-Fynn and A. K. Ray, Europhysics Letters, 85, 27008-p1- p6 (2009); Chemical Physics Letters, 482, 223-227 (2009). we present here a systematic study of the electronic and geometric structure properties of mixed actinide dioxides, U0.5Pu0.5O2, U0.5Am0.5O2, Pu0.5Am0.5 O2 and U0.8Pu0.2O2. The fraction of exact Hartree-Fock exchange used was 40%. To investigate the effect of spin-orbit coupling on the ground state electronic and geometric structure properties, computations have been carried out at two theoretical levels, one at the scalar-relativistic level with no spin-orbit coupling and one at the fully relativistic level with spin-orbit coupling. Thermodynamic properties have been calculated by a coupling of first-principles calculation and lattice dynamics.

DN/DG Screening of Environmental Swipe Samples: FY2016 Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Glasgow, David C.; Croft, Stephen; Venkataraman, Ramkumar

The Delayed Neutron Delayed Gamma (DNDG) technique provides a new analytical capability to the International Atomic Energy Agency (IAEA) for detecting undeclared nuclear activities. IAEA’s Long Term R&D (LTRD) plan has a stated high urgency need to develop elemental and isotopic signatures of nuclear fuel cycle activities and processes (LTRD 2.2). The new DNDG capability is used to co-detect both uranium and plutonium as an extension of a DN only method that is already being utilized by the IAEA for the analysis of swipes to inform on undeclared nuclear activities. Analytical method involving irradiation of swipe samples potentially containing tracemore » quantities of fissile material in a thermal neutron field, followed by the counting of delayed neutrons, is a well-known technique in the field of safeguards and nonproliferation. It is used for detecting the presence of microscopic amounts of fissile material, (typically a linear combination of 233U, 235U, 239Pu, and 241Pu)and quantifying it in terms of the equivalent mass of 235U. The delayed neutron (DN) technique is very sensitive and is been routinely employed at the High Flux Isotope Reactor (HFIR) facility at Oak Ridge National Laboratory (ORNL). Both uranium and plutonium are of high safeguards value. However, the DN technique is not well suited for distinguishing between U and Pu isotopes since the decay curves overlap closely. The delayed gamma (DG) technique will help detect the presence of 239Pu in a mixture of U and Pu. Thus the DNDG approach combines the best of both worlds; the sensitivity of DN counting and the isotopic specificity of DG counting. The present work seeks to build on the delayed neutron and delayed gamma methods that have been developed at ORNL. It is recognized that the distribution profile of heavy fission products remains fairly invariant for the fissile nuclides whereas the distribution of light fission products varies from one isotope to another. That is, the ratio of the yield of a light fission fragment to a heavy fission fragments is isotope specific. Measurement of the ratio of the net full energy peak (FEP) from low/high mass fission products is an elegant way to characterize the fraction of fissile materials present in a mixture. By empirically calibrating the ratio of the net FEP as a function of known concentration of the binary mixture, one can determine the fraction of fissile isotopes in an unknown sample. In the work done in fiscal year (FY) 2016, samples of single fissile material isotopes as well as binary mixtures were irradiated in a well thermalized irradiation field in the HFIR. Delayed neutron counting was performed using the neutron counter at the HFIR Neutron Activation Analysis (NAA) laboratory. Delayed gamma counting was performed using a shielded high purity germanium (HPGe) detector. Delayed neutron decay curve results highlighted the difficulty of distinguishing between U and Pu isotopes, and the need for including the delayed gamma component. Based on delayed gamma spectrometry, twelve ratios of low mass/high fission product gamma ray FEP have been identified as valid candidates. Linearity of the ratios, as a function of 239Pu fraction in 235U+ 239Pu mixtures, was confirmed for the low mass/high mass candidates that were selected. The DNDG method we are spearheading allows not only the presence of total fissile content to be detected, but whether the material is predominantly U or predominantly Pu, or a mixture. This provides additional SG relevant information.« less

Uranium (III)-Plutonium (III) co-precipitation in molten chloride

NASA Astrophysics Data System (ADS)

Vigier, Jean-François; Laplace, Annabelle; Renard, Catherine; Miguirditchian, Manuel; Abraham, Francis

2018-02-01

Co-management of the actinides in an integrated closed fuel cycle by a pyrochemical process is studied at the laboratory scale in France in the CEA-ATALANTE facility. In this context the co-precipitation of U(III) and Pu(III) by wet argon sparging in LiCl-CaCl2 (30-70 mol%) molten salt at 705 °C is studied. Pu(III) is prepared in situ in the molten salt by carbochlorination of PuO2 and U(III) is then introduced as UCl3 after chlorine purge by argon to avoid any oxidation of uranium up to U(VI) by Cl2. The oxide conversion yield through wet argon sparging is quantitative. However, the preferential oxidation of U(III) in comparison to Pu(III) is responsible for a successive conversion of the two actinides, giving a mixture of UO2 and PuO2 oxides. Surprisingly, the conversion of sole Pu(III) in the same conditions leads to a mixture of PuO2 and PuOCl, characteristic of a partial oxidation of Pu(III) to Pu(IV). This is in contrast with coconversion of U(III)-Pu(III) mixtures but in agreement with the conversion of Ce(III).

Studies of Neutron-Induced Fission of 235U, 238U, and 239Pu

NASA Astrophysics Data System (ADS)

Duke, Dana; TKE Team

2014-09-01

A Frisch-gridded ionization chamber and the double energy (2E) analysis method were used to study mass yield distributions and average total kinetic energy (TKE) release from neutron-induced fission of 235U, 238U, and 239Pu. Despite decades of fission research, little or no TKE data exist for high incident neutron energies. Additional average TKE information at incident neutron energies relevant to defense- and energy-related applications will provide a valuable observable for benchmarking simulations. The data can also be used as inputs in theoretical fission models. The Los Alamos Neutron Science Center-Weapons Neutron Research (LANSCE - WNR) provides a neutron beam from thermal to hundreds of MeV, well-suited for filling in the gaps in existing data and exploring fission behavior in the fast neutron region. The results of the studies on 238U, 235U, and 239Pu will be presented. LA-UR-14-24921.

Analysis of actinides in an ombrotrophic peat core - evidence of post-depositional migration of fallout radionuclides

NASA Astrophysics Data System (ADS)

Quinto, Francesca; Hrnecek, Erich; Krachler, Michael; Shotyk, William; Steier, Peter; Winkler, Stephan R.

2013-04-01

Plutonium (239Pu, 240Pu, 241Pu, 242Pu) and uranium (236U, 238U) isotopes were analyzed in an ombrotrophic peat core from the Black Forest, Germany, representing the last 80 years of atmospheric deposition. The reliable determination of these isotopes at ultra-trace levels was possible using ultra-clean laboratory procedures and accelerator mass spectrometry. The 240Pu/239Pu isotopic ratios are constant along the core with a mean value of 0.19 ±0.02 (N = 32). This result is consistent with the acknowledged average 240Pu/239Pu isotopic ratio from global fallout in the Northern Hemisphere. The global fallout origin of Pu is confirmed by the corresponding 241Pu/239Pu (0.0012 ±0.0005) and 242Pu/239Pu (0.004 ± 0.001) isotopic ratios. The identification of the Pu isotopic composition characteristic for global fallout in peat layers pre-dating the period of atmospheric atom bomb testing (AD 1956 - AD 1980) is a clear evidence of the migration of Pu downwards the peat profile. The maximum of global fallout derived 236U is detected in correspondence to the age/depth layer of maximum stratospheric fallout (AD 1963). This finding demonstrates that the 236U bomb peak can be successfully used as an independent chronological marker complementing the 210Pb dating of peat cores. The profiles of the global fallout derived 236U and 239Pu are compared with those of 137Cs and 241Am. As typical of ombrothrophic peat, the temporal fallout pattern of 137Cs is poorly retained. Similarly like for Pu, post-depositional migration of 241Am in peat layers preceding the era of atmospheric nuclear tests is observed.

Effect of oxidation state and ionic strength on sorption of actinides (Th, U, Np, Am) to geologic media [Abstract and References Only

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dittrich, Timothy M.; Richmann, Michael K.; Reed, Donald T.

2015-10-30

The degree of conservatism in the estimated sorption partition coefficients (K ds) used in a performance assessment model is being evaluated based on a complementary batch and column method. The main focus of this work is to investigate the role of ionic strength, solution chemistry, and oxidation state (III-VI) in actinide sorption to dolomite rock. Based on redox conditions and solution chemistry expected at the WIPP, possible actinide species include Pu(III), Pu(IV), U(IV), U(VI), Np(IV), Np(V), Am(III), and Th(IV).

Minimum pickup velocity ( U pu) of nanoparticles in gas-solid pneumatic conveying

NASA Astrophysics Data System (ADS)

Anantharaman, Aditya; van Ommen, J. Ruud; Chew, Jia Wei

2015-12-01

This paper is the first systematic study of the pneumatic conveying of nanoparticles. The minimum pickup velocity, U pu, of six nanoparticle species of different materials [i.e., silicon dioxide (SiO2), aluminum oxide (Al2O3), and titanium dioxide (TiO2)] and surfaces (i.e., apolar and polar) was determined by the weight loss method. Results show that (1) due to relative lack of hydrogen bonding, apolar nanoparticles had higher mass loss values at the same velocities, mass loss curves with accentuated S-shaped profiles, and lower U pu values, (2) among the three species, SiO2, which has the lowest Hamaker coefficient, exhibited the greatest discrepancy between apolar and polar surfaces with respect to both mass loss curves and U pu values, (3) U mf,polar/ U mf,apolar was between 1 and 3.5 times that of U pu,polar/ U pu,apolar due to greater extents of hydrogen bonding associated with U mf, (4) U pu values were at least an order-of-magnitude lower than that expected from the well-acknowledged U pu correlation (Kalman et al., Powder Technol 160:103-113, 2005) due to agglomeration, (5) although nanoparticles should be categorized as Zone III (Kalman et al. 2005) (or Geldart group C, Powder Technol 7:285-292, 1973), the nanoparticles, and primary and complex agglomerates agreed more with the Zone I (or Geldart group B) correlation.

The application of N,N-dimethyl-3-oxa-glutaramic acid (DOGA) in the PUREX process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jianchen, Wang; Jing, Chen

2007-07-01

The new salt-free complexant, DOGA for separating trace Pu(IV) and Np(IV) from U(VI) nitric acid solution was studied. DOGA has stronger complexing abilities to Pu(IV) and Np(IV), but complexing ability of DOGA to U(VI) was weaker. The DOGA can be used in the PUREX process to separate Pu(IV) and Np(IV) from U(VI) nitric solution. On one hand, U(IV) in the nitric acid solution containing trace Pu(IV) and Np(IV) was extracted by 30%TBP - kerosene(v/v) in the presence of DOGA, but Pu(IV) and Np(IV) were kept in the aqueous phase. On the other hand, Pu(IV) and Np(IV) loading in 30% TBPmore » - kerosene were effectively stripped by DOGA into the aqueous phase, but U(VI) loading in 30% TBP - kerosene was remained in 30% TBP - kerosene. DOGA is a promising complexant to separate Pu(IV) and Np(IV) from U(VI) solution in the U-cycle of the PUREX process. (authors)« less

Rapid dating of recent aquatic sediments using Pu activities and 240Pu/239Pu as determined by quadrupole inductively coupled plasma mass spectrometry.

PubMed

Ketterer, Michael E; Watson, Bridgette R; Matisoff, Gerald; Wilsont, Christopher G

2002-03-15

Quadrupole inductively coupled plasma mass spectrometry has been used to rapidly establish the chronology of recent aquatic sediments via measurements of the activities of 239Pu, 240Pu, and the atom ratio 240Pu/239Pu. Following addition of 0.007 Bq of a 242Pu spike isotope, Pu is leached from 3-20 g aliquots of dry-ashed sediments with HNO3. A selective anion exchanger is used to preconcentrate Pu into approximately 2 mL aliquots, which are directly analyzed using a pneumatic nebulizer and double-pass spraychamber operating at 60 microL/min solution uptake rate. The ICPMS data collection is performed for 10 min per sample. The U concentrations were 0.01-0.05 microg/L in the analyzed solutions, and the interference of 238U1H+ upon 239Pu+ was negligible. The method has been applied to determining Pu activities, inventory, and 240Pu/239Pu in a complete sediment core from Old Woman Creek (Huron, OH). The Pu activity profiles, obtained in approximately 6 h of instrumental measurement time, are in agreement with a y spectrometric 137Cs profile. Peak 239+240Pu and 137Cs activities in the core were 1.60 +/- 0.02 and 47.8 +/- 0.8 Bq/kg, respectively; inventories were 108 +/- 2 Bq/m2 239+240Pu and 2710 +/- 40 Bq/m2 137Cs. Detection limits, based upon the analysis of 20 g samples, were 0.004 Bq/kg 239Pu, 0.012 Bq/kg 240Pu, and 0.012 Bq/kg 239+240Pu. 240Pu/239Pu atom ratios of 0.16-0.19 were obtained for all core intervals containing detectable Pu, which indicates that global fallout is the source of these radionuclides.

Plutonium and uranium in human bones from areas surrounding the Semipalatinsk nuclear test site.

PubMed

Yamamoto, Masayoshi; Hoshi, Masaharu; Sakaguchi, Aya; Shinohara, Kunihiko; Kurihara, Osamu; Apsalikov, Kazbek N; Gusev, Boris I

2006-02-01

To evaluate the present levels of 239,240Pu and U in residents living near the Semipalatinsk nuclear test site, more than 70 bone samples were obtained at autopsy. The subjects ranged in age from 30 to 86 years (mean 59.3+/-12.9). Most of the samples consisted of victims who died of various diseases. Plutonium and U were radiochemically separated and determined by alpha-ray spectrometry. The mean concentrations of 239,240Pu and 238U observed were 0.050+/-0.041 mBq/g-ash (vertebrae 71, long-bones 18) and 0.28+/-0.13 mBq/g-ash (22.8+/-10.6 microg U/kg-ash) (vertebrae 58, long bones 16), respectively. The present 239,240Pu levels were within the range found for human bone samples from other countries due solely to global fallout in the early 1980s. The average U concentration was close to the estimate (mean 22.5 microg U/kg-ash) for the UK, and about 10 times higher than those estimated for residents in New York City and Japan. By assuming that the average concentration of 239,240Pu in bone samples is the value at 45 years after instantaneous inhalation in 1955, the initial total intake and the effective dose for 45 years were estimated as 10 Bq and 0.2 mSv, respectively. The annual intake of total U (234,235,238U) and its effective dose for 60 years were estimated as 30 Bq for adult and 0.1 mSv, respectively, for chronic ingestion.

A Domain of Herpes Simplex Virus pUL33 Required To Release Monomeric Viral Genomes from Cleaved Concatemeric DNA.

PubMed

Yang, Kui; Dang, Xiaoqun; Baines, Joel D

2017-10-15

Monomeric herpesvirus DNA is cleaved from concatemers and inserted into preformed capsids through the actions of the viral terminase. The terminase of herpes simplex virus (HSV) is composed of three subunits encoded by U L 15, U L 28, and U L 33. The U L 33-encoded protein (pU L 33) interacts with pU L 28, but its precise role in the DNA cleavage and packaging reaction is unclear. To investigate the function of pU L 33, we generated a panel of recombinant viruses with either deletions or substitutions in the most conserved regions of U L 33 using a bacterial artificial chromosome system. Deletion of 11 amino acids (residues 50 to 60 or residues 110 to 120) precluded viral replication, whereas the truncation of the last 10 amino acids from the pU L 33 C terminus did not affect viral replication or the interaction of pU L 33 with pU L 28. Mutations that replaced the lysine at codon 110 and the arginine at codon 111 with alanine codons failed to replicate, and the pU L 33 mutant interacted with pU L 28 less efficiently. Interestingly, genomic termini of the large (L) and small (S) components were detected readily in cells infected with these mutants, indicating that concatemeric DNA was cleaved efficiently. However, the release of monomeric genomes as assessed by pulsed-field gel electrophoresis was greatly diminished, and DNA-containing capsids were not observed. These results suggest that pU L 33 is necessary for one of the two viral DNA cleavage events required to release individual genomes from concatemeric viral DNA. IMPORTANCE This paper shows a role for pU L 33 in one of the two DNA cleavage events required to release monomeric genomes from concatemeric viral DNA. This is the first time that such a phenotype has been observed and is the first identification of a function of this protein relevant to DNA packaging other than its interaction with other terminase components. Copyright © 2017 Yang et al.

First measurements of (236)U concentrations and (236)U/(239)Pu isotopic ratios in a Southern Hemisphere soil far from nuclear test or reactor sites.

PubMed

Srncik, M; Tims, S G; De Cesare, M; Fifield, L K

2014-06-01

The variation of the (236)U and (239)Pu concentrations as a function of depth has been studied in a soil profile at a site in the Southern Hemisphere well removed from nuclear weapon test sites. Total inventories of (236)U and (239)Pu as well as the (236)U/(239)Pu isotopic ratio were derived. For this investigation a soil core from an undisturbed forest area in the Herbert River catchment (17°30' - 19°S) which is located in north-eastern Queensland (Australia) was chosen. The chemical separation of U and Pu was carried out with a double column which has the advantage of the extraction of both elements from a relatively large soil sample (∼20 g) within a day. The samples were measured by Accelerator Mass Spectrometry using the 14UD pelletron accelerator at the Australian National University. The highest atom concentrations of both (236)U and (239)Pu were found at a depth of 2-3 cm. The (236)U/(239)Pu isotopic ratio in fallout at this site, as deduced from the ratio of the (236)U and (239)Pu inventories, is 0.085 ± 0.003 which is clearly lower than the Northern Hemisphere value of ∼0.2. The (236)U inventory of (8.4 ± 0.3) × 10(11) at/m(2) was more than an order of magnitude lower than values reported for the Northern Hemisphere. The (239)Pu activity concentrations are in excellent agreement with a previous study and the (239+240)Pu inventory was (13.85 ± 0.29) Bq/m(2). The weighted mean (240)Pu/(239)Pu isotopic ratio of 0.142 ± 0.005 is slightly lower than the value for global fallout, but our results are consistent with the average ratio of 0.173 ± 0.027 for the southern equatorial region (0-30°S). Copyright © 2014 Elsevier Ltd. All rights reserved.

Rapid Mantle Source Variations During the Latest Episode of Kilauea's Prolonged Pu'u O'o Eruption, Hawaii

NASA Astrophysics Data System (ADS)

Marske, J. P.; Garcia, M. O.; Pietruszka, A. J.; Norman, M. D.; Rhodes, J. M.

2006-12-01

Nearly 24 years of continuous geochemical monitoring of lavas from the current Pu'u O'o eruption allow us to probe the mantle processes beneath Kilauea Volcano in unparalleled detail. Here we present new measurements Pb, Sr, and Nd isotope ratios and major- and trace-element abundances for lavas from episode 55 (1997-2006), which marks the longest and most voluminous interval of this eruption. Pu'u O'o lavas erupted since 1985 display systematic decreases in their TiO2, K2O, P2O5 and CaO abundances (normalized to 10 wt. % MgO to correct for olivine control) due to changes in the parental magma composition. Incompatible element ratios (e.g., Ba/Nb and La/Y) also show overall temporal decreases. Earlier erupted Pu'u O'o lavas displayed the most significant decrease in incompatible element ratios with near constant SiO2 contents, and a gradual increase in 87Sr/86Sr ratios. However, episode 55 lavas record significant increases in MgO- normalized SiO2 contents and 87Sr/86Sr with nearly constant (e.g. Ba/Nb) or a slightly reversed (e.g., TiO2 and K2O) trends in incompatible element ratios and abundances. There is little variation of 206Pb/204Pb ratios in lavas (18.38-18.43) erupted since 1985. Neither a single mantle source composition nor a change in partial melting conditions alone can explain these observations. Based on the isotopic and chemical variability, we conclude that early Pu'u O'o lavas originated from two distinct mantle source components: (1) a long-term depleted component (with relatively low 87Sr/86Sr ratios) that originated within the deep source of the Hawaiian plume that characterizes the earlier part of the eruption (1985-1992), and (2) a recently depleted component (i.e. a component that was recently depleted by prior melting) with low abundances of incompatible elements became increasingly important from 1992-1997. More recently, Pu'u O'o has tapped greater proportions of a new (3) long-term less depleted component (with higher 87Sr/86Sr ratios than observed from 1985-1992) that originated within the deep source region of the plume. This third component lies within typical Pb, Sr and Nd isotopic space for Kilauea, but represents a new source composition for the Pu'u O'o eruption. The systematic geochemical evolution of Pu'u O'o lavas reflects changes in the proportions of the mantle source components tapped throughout the eruption. The rapid isotope variations (on a time scale of years) in the most recent lavas suggest the mantle source components are heterogeneous on an extremely small scale, relative to the size of Kilauea's melting region.

ZPR-6 assembly 7 high {sup 240}Pu core experiments : a fast reactor core with mixed (Pu,U)-oxide fuel and a centeral high{sup 240}Pu zone.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lell, R. M.; Morman, J. A.; Schaefer, R.W.

ZPR-6 Assembly 7 (ZPR-6/7) encompasses a series of experiments performed at the ZPR-6 facility at Argonne National Laboratory in 1970 and 1971 as part of the Demonstration Reactor Benchmark Program (Reference 1). Assembly 7 simulated a large sodium-cooled LMFBR with mixed oxide fuel, depleted uranium radial and axial blankets, and a core H/D near unity. ZPR-6/7 was designed to test fast reactor physics data and methods, so configurations in the Assembly 7 program were as simple as possible in terms of geometry and composition. ZPR-6/7 had a very uniform core assembled from small plates of depleted uranium, sodium, iron oxide,more » U{sub 3}O{sub 8} and Pu-U-Mo alloy loaded into stainless steel drawers. The steel drawers were placed in square stainless steel tubes in the two halves of a split table machine. ZPR-6/7 had a simple, symmetric core unit cell whose neutronic characteristics were dominated by plutonium and {sup 238}U. The core was surrounded by thick radial and axial regions of depleted uranium to simulate radial and axial blankets and to isolate the core from the surrounding room. The ZPR-6/7 program encompassed 139 separate core loadings which include the initial approach to critical and all subsequent core loading changes required to perform specific experiments and measurements. In this context a loading refers to a particular configuration of fueled drawers, radial blanket drawers and experimental equipment (if present) in the matrix of steel tubes. Two principal core configurations were established. The uniform core (Loadings 1-84) had a relatively uniform core composition. The high {sup 240}Pu core (Loadings 85-139) was a variant on the uniform core. The plutonium in the Pu-U-Mo fuel plates in the uniform core contains 11% {sup 240}Pu. In the high {sup 240}Pu core, all Pu-U-Mo plates in the inner core region (central 61 matrix locations per half of the split table machine) were replaced by Pu-U-Mo plates containing 27% {sup 240}Pu in the plutonium component to construct a central core zone with a composition closer to that in an LMFBR core with high burnup. The high {sup 240}Pu configuration was constructed for two reasons. First, the composition of the high {sup 240}Pu zone more closely matched the composition of LMFBR cores anticipated in design work in 1970. Second, comparison of measurements in the ZPR-6/7 uniform core with corresponding measurements in the high {sup 240}Pu zone provided an assessment of some of the effects of long-term {sup 240}Pu buildup in LMFBR cores. The uniform core version of ZPR-6/7 is evaluated in ZPR-LMFR-EXP-001. This document only addresses measurements in the high {sup 240}Pu core version of ZPR-6/7. Many types of measurements were performed as part of the ZPR-6/7 program. Measurements of criticality, sodium void worth, control rod worth and reaction rate distributions in the high {sup 240}Pu core configuration are evaluated here. For each category of measurements, the uncertainties are evaluated, and benchmark model data are provided.« less

Solid state reactions of CeO 2, PuO 2, (U,Ce)O 2 and (U,Pu)O 2 with K 2S 2O 8

NASA Astrophysics Data System (ADS)

Keskar, Meera; Kasar, U. M.; Mudher, K. D. Singh; Venugopal, V.

2004-09-01

Solid state reactions of CeO 2, PuO 2 and mixed oxides (U,Ce)O 2 and (U,Pu)O 2 containing different mol.% of Ce and Pu, were carried out with K 2S 2O 8 at different temperatures to identify the formation of various products and to investigate their dissolution behaviour. X-ray, chemical and thermal analysis methods were used to characterise the products formed at various temperatures. The products obtained by heating two moles of K 2S 2O 8 with one mole each of CeO 2, PuO 2, (U,Ce)O 2 and (U,Pu)O 2 at 400 °C were identified as K 4Ce(SO 4) 4, K 4Pu(SO 4) 4, K 4(U,Ce)(SO 4) 4 and K 4(U,Pu)(SO 4) 4, respectively. K 4Ce(SO 4) 4 further decomposed to form K 4Ce(SO 4) 3.5 at 600 °C and mixture of K 2SO 4 and CeO 2 at 950 °C. Thus the products formed during the reaction of 2K 2S 2O 8 + CeO 2 show that cerium undergoes changes in oxidation state from +4 to +3 and again to +4. XRD data of K 4Ce(SO 4) 4 and K 4Ce(SO 4) 3.5 were indexed on triclinic and monoclinic system, respectively. PuO 2 + 2K 2S 2O 8 reacts at 400 °C to form K 4Pu(SO 4) 4 which was stable upto 750 °C and further decomposes to form K 2SO 4 + PuO 2 at 1000 °C. The products formed at 400 °C during the reactions of the oxides and mixed oxides were found to be readily soluble in 1-2 M HNO 3.

A comment on the thermal conductivity of (U,Pu)O 2 and (U,Th)O 2 by molecular dynamics with adjustment for phonon-spin scattering

DOE PAGES

Cooper, Michael William D.; Liu, Xiang -Yang; Stanek, Christopher Richard; ...

2016-07-15

In this study, a new approach for adjusting molecular dynamics results on UO 2 thermal conductivity to include phonon-spin scattering has been used to improve calculations on U x Pu 1–x O 2 and U xTh 1xO 2. We demonstrate that by including spin scattering a strong asymmetry as a function of uranium actinide fraction, x, is obtained. Greater degradation is shown for U xTh 1–xO 2 than U xPu 1-xO 2. Minimum thermal conductivities are predicted at U 0.97Pu 0.03O 2 and U 0.58Th 0.42O 2, although the degradation in U xPu 1–xO 2 is negligible relative to puremore » UO 2.« less

Separation of uranium from (U, Th)O 2 and (U, Pu)O 2 by solid state reactions route

NASA Astrophysics Data System (ADS)

Keskar, Meera; Mudher, K. D. Singh; Venugopal, V.

2005-01-01

Solid state reactions of UO 2, ThO 2, PuO 2 and their mixed oxides (U, Th)O 2 and (U, Pu)O 2 were carried out with sodium nitrate upto 900 °C, to study the formation of various phases at different temperatures, which are amenable for easy dissolution and separation of the actinide elements in dilute acid. Products formed by reacting unsintered as well as sintered UO 2 with NaNO 3 above 500 °C were readily soluble in 2 M HNO 3, whereas ThO 2 and PuO 2 did not react with NaNO 3 to form any soluble products. Thus reactions of mixed oxides (U, Th)O 2 and (U, Pu)O 2 with NaNO 3 were carried out to study the quantitative separation of U from (U, Th)O 2 and (U, Pu)O 2. X-ray diffraction, X-ray fluorescence, thermal analysis and chemical analysis techniques were used for the characterization of the products formed during the reactions.

Ultra-trace determination of plutonium in marine samples using multi-collector inductively coupled plasma mass spectrometry.

PubMed

Lindahl, Patric; Keith-Roach, Miranda; Worsfold, Paul; Choi, Min-Seok; Shin, Hyung-Seon; Lee, Sang-Hoon

2010-06-25

Sources of plutonium isotopes to the marine environment are well defined, both spatially and temporally, which makes Pu a potential tracer for oceanic processes. This paper presents the selection, optimisation and validation of a sample preparation method for the ultra-trace determination of Pu isotopes ((240)Pu and (239)Pu) in marine samples by multi-collector (MC) ICP-MS. The method was optimised for the removal of the interference from (238)U and the chemical recovery of Pu. Comparison of various separation strategies using AG1-X8, TEVA, TRU, and UTEVA resins to determine Pu in marine calcium carbonate samples is reported. A combination of anion-exchange (AG1-X8) and extraction chromatography (UTEVA/TRU) was the most suitable, with a radiochemical Pu yield of 87+/-5% and a U decontamination factor of 1.2 x 10(4). Validation of the method was accomplished by determining Pu in various IAEA certified marine reference materials. The estimated MC-ICP-MS instrumental limit of detection for (239)Pu and (240)Pu was 0.02 fg mL(-1), with an absolute limit of quantification of 0.11 fg. The proposed method allows the determination of ultra-trace Pu, at femtogram levels, in small size marine samples (e.g., 0.6-2.0 g coral or 15-20 L seawater). Finally, the analytical method was applied to determining historical records of the Pu signature in coral samples from the tropical Northwest Pacific and (239+240)Pu concentrations and (240)Pu/(239)Pu atom ratios in seawater samples as part of the 2008 GEOTRACES intercalibration exercise. Copyright 2010 Elsevier B.V. All rights reserved.

Multi-isotopic determination of plutonium (239Pu, 240Pu, 241Pu and 242Pu) in marine sediments using sector-field inductively coupled plasma mass spectrometry.

PubMed

Donard, O F X; Bruneau, F; Moldovan, M; Garraud, H; Epov, V N; Boust, D

2007-03-28

Among the transuranic elements present in the environment, plutonium isotopes are mainly attached to particles, and therefore they present a great interest for the study and modelling of particle transport in the marine environment. Except in the close vicinity of industrial sources, plutonium concentration in marine sediments is very low (from 10(-4) ng kg(-1) for (241)Pu to 10 ng kg(-1) for (239)Pu), and therefore the measurement of (238)Pu, (239)Pu, (240)Pu, (241)Pu and (242)Pu in sediments at such concentration level requires the use of very sensitive techniques. Moreover, sediment matrix contains huge amounts of mineral species, uranium and organic substances that must be removed before the determination of plutonium isotopes. Hence, an efficient sample preparation step is necessary prior to analysis. Within this work, a chemical procedure for the extraction, purification and pre-concentration of plutonium from marine sediments prior to sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS) analysis has been optimized. The analytical method developed yields a pre-concentrated solution of plutonium from which (238)U and (241)Am have been removed, and which is suitable for the direct and simultaneous measurement of (239)Pu, (240)Pu, (241)Pu and (242)Pu by SF-ICP-MS.

Trends in intrusive and eruptive activity during Kilauea's long-lived east rift zone eruption

NASA Astrophysics Data System (ADS)

Orr, T. R.; Patrick, M. R.; Heliker, C.

2011-12-01

Kilauea Volcano's Pu`u `O`o eruption, continuing for nearly three decades, offers a unique opportunity to study trends in eruptive behavior. One such trend, that of uprift intrusion ± eruption, accompanied by crater floor collapse and eruptive hiatus, has been repeated several times at Pu`u `O`o. This includes the February 7, 1993, intrusion; the January 29, 1997, intrusion and eruption; the September 12, 1999, intrusion; and the June 17, 2007, intrusion and eruption. Activity resumed within Pu`u `O`o following each of these events, and crater refilling culminated eventually in the outbreak of lava from new vents on the flank of the Pu`u `O`o cone. The pattern was repeated again in 2011, when a brief fissure eruption uprift from Pu`u `O`o started on March 5. The Pu`u `O`o crater floor dropped about 115 m in response to the eruption, which ceased on March 9. After a short hiatus, lava reappeared in Pu`u `O`o on March 26, and the crater began to fill slowly thereafter by overflow from a central lava lake. Starting in late June 2011, however, the crater floor began to uplift in a wholesale fashion, suggesting an increase in the pressure beneath the Pu`u `O`o edifice. By late July, the lava within the crater had reached its highest level since early 2004, and lava had begun to overflow from the southwestern side of the crater. On August 3, the west side of the Pu`u `O`o cone was abruptly thrust upward as a sill was injected beneath that portion of the cone. Within minutes, lava began to erupt from a crack on the west flank of Pu`u `O`o, completing the pattern of intrusion, crater collapse, refilling, and breakout. During a long-lived eruption, maintaining a detailed observational and geophysical record is essential for recognizing patterns that may emerge. Recognizing such a pattern allowed Hawaiian Volcano Observatory scientists to prepare a response well in advance of the August 3, 2011 event, and provides guidance for responding to future eruption crises at Pu`u `O`o that evolve similarly.

Coordination Chemistry of Homoleptic Actinide(IV)-Thiocyanate Complexes

DOE PAGES

Carter, Tyler J.; Wilson, Richard E.

2015-09-10

Here, the synthesis, X-ray crystal structure, vibrational and optical spectroscopy for the eight-coordinate thiocyanate compounds, [Et 4N] 4[Pu IV(NCS) 8], [Et 4N] 4[Th IV(NCS) 8], and [Et 4N] 4[Ce III(NCS) 7(H 2O)] are reported. Thiocyanate was found to rapidly reduce plutonium to Pu III in acidic solutions (pH<1) in the presence of NCS –. The optical spectrum of [Et 4N][SCN] containing Pu III solution was indistinguishable from that of aquated Pu III suggesting that inner-sphere complexation with [Et 4N][SCN] does not occur in water. However, upon concentration, the homoleptic thiocyanate complex [Et 4N] 4[Pu IV(NCS) 8] was crystallized when amore » large excess of [Et 4N][NCS] was present. This compound, along with its U IV analogue, maintains inner-sphere thiocyanate coordination in acetonitrile based on the observation of intense ligand-to-metal charge-transfer bands. Spectroscopic and crystallographic data do not support the interaction of the metal orbitals with the ligand π system, but support an enhanced An IV–NCS interaction, as the Lewis acidity of the metal ion increases from Th to Pu.« less

ECCO: Th/U/Pu/Cm Dating of Galactic Cosmic Ray Nuclei

NASA Technical Reports Server (NTRS)

Westphal, A. J.; Weaver, B. A.; Solarz, M.; Dominquez, G.; Craig, N.; Adams, J. H.; Barbier, L. M.; Christian, E. R.; Mitchell, J. W.; Binns, W. R.;

Chemical resolution of Pu+ from U+ and Am+ using a band-pass reaction cell inductively coupled plasma mass spectrometer.

PubMed

Tanner, Scott D; Li, Chunsheng; Vais, Vladimir; Baranov, Vladimir I; Bandura, Dmitry R

2004-06-01

Determination of the concentration and distribution of the Pu and Am isotopes is hindered by the isobaric overlaps between the elements themselves and U, generally requiring time-consuming chemical separation of the elements. A method is described in which chemical resolution of the elemental ions is obtained through ion-molecule reactions in a reaction cell of an ICPMS instrument. The reactions of "natural" U(+), (242)Pu(+), and (243)Am(+) with ethylene, carbon dioxide, and nitric oxide are reported. Since the net sensitivities to the isotopes of an element are similar, chemical resolution is inferred when one isobaric element reacts rapidly with a given gas and the isobar (or in this instance surrogate isotope) is unreactive or slowly reactive. Chemical resolution of the m/z 238 isotopes of U and Pu can be obtained using ethylene as a reaction gas, but little improvement in the resolution of the m/z 239 isobars is obtained. However, high efficiency of reaction of U(+) and UH(+) with CO(2), and nonreaction of Pu(+), allows the sub-ppt determination of (239)Pu, (240)Pu, and (242)Pu (single ppt for (238)Pu) in the presence of 7 orders of magnitude excess U matrix without prior chemical separation. Similarly, oxidation of Pu(+) by NO, and nonreaction of Am(+), permit chemical resolution of the isobars of Pu and Am over 2-3 orders of magnitude relative concentration. The method provides the potential for analysis of the actinides with reduced sample matrix separation.

Summary of a joint US-Japan study of potential approaches to reduce the attractiveness of various nuclear materials for use in a nuclear explosive device by a terrorist group

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bathke, C.G.; Inoue, N.; Kuno, Y.

2013-07-01

This paper summarizes the results of a joint US-Japan study to establish a mutual understanding, through scientific-based study, of potential approaches to reduce the attractiveness of various nuclear materials for use in a terrorist nuclear explosive device (NED). 4 approaches that can reduce materials attractiveness with a very high degree of effectiveness are: -) diluting HEU with natural or depleted U to an enrichment of less than 10% U-235; -) storing Pu in nuclear fuel that is not man portable and with a dose rate greater or equal to 10 Gy/h at 1 m; -) storing Pu or HEU inmore » heavy items, i.e. not transportable, provided the removal of the Pu or HEU from the item requires a purification/processing capability; and -) converting Pu and HEU to very dilute forms (such as wastes) that, without any security barriers, would require very long acquisition times to acquire a Category I quantity of Pu or of HEU. 2 approaches that can reduce materials attractiveness with a high degree of effectiveness are: -) converting HEU-fueled research reactors into LEU-fueled research reactors or dilute HEU with natural or depleted U to an enrichment of less than 20% U-235; -) converting U/Al reactor fuel into U/Si reactor fuel. Other approaches have been assessed as moderately or totally inefficient to reduce the attractiveness of nuclear materials.« less

Isotopic compositions of (236)U and Pu isotopes in "black substances" collected from roadsides in Fukushima prefecture: fallout from the Fukushima Dai-ichi nuclear power plant accident.

PubMed

Sakaguchi, Aya; Steier, Peter; Takahashi, Yoshio; Yamamoto, Masayoshi

2014-04-01

Black-colored road dusts were collected in high-radiation areas in Fukushima Prefecture. Measurement of (236)U and Pu isotopes and (134,137)Cs in samples was performed to confirm whether refractory elements, such as U and Pu, from the fuel core were discharged and to ascertain the extent of fractionation between volatile and refractory elements. The concentrations of (134,137)Cs in all samples were exceptionally high, ranging from 0.43 to 17.7 MBq/kg, respectively. (239+240)Pu was detected at low levels, ranging from 0.15 to 1.14 Bq/kg, and with high (238)Pu/(239+240)Pu activity ratios of 1.64-2.64. (236)U was successfully determined in the range of (0.28 to 6.74) × 10(-4) Bq/kg. The observed activity ratios for (236)U/(239+240)Pu were in reasonable agreement with those calculated for the fuel core inventories, indicating that trace amounts of U from the fuel cores were released together with Pu isotopes but without large fractionation. The quantities of U and (239+240)Pu emitted to the atmosphere were estimated as 3.9 × 10(6) Bq (150 g) and 2.3 × 10(9) Bq (580 mg), respectively. With regard to U, this is the first report to give a quantitative estimation of the amount discharged. Appreciable fractionation between volatile and refractory radionuclides associated with the dispersal/deposition processes with distance from the Fukushima Dai-ichi Nuclear Power Plant was found.

Evaluations of Energy Spectra of Neutrons Emitted Promptly in Neutron-induced Fission of 235 U and 239 Pu

DOE PAGES

Neudecker, Denise; Talou, Patrick; Kawano, Toshihiko; ...

2018-02-01

The energy spectra of neutrons emitted promptly in the neutron-induced fission reactions of 235U and 239Pu were re-evaluated for ENDF/B-VIII.0. The evaluations presented here are based on a careful modeling of all relevant physics processes, an extensive analysis of experimental data and a detailed quantification of pertinent uncertainties. Energy spectra of neutrons emitted in up to fourth chance fission are considered and both compound and pre-equilibrium processes are included. Also, important nuclear model parameters, such as the average total kinetic energy of the fission fragments and the multiple chance fission probabilities, and their uncertainties are estimated based on experimental knowledge,more » model information and evaluated data. In addition to experimental information already available for ENDF/B-VII.1, these new evaluations make use of recently published experimental data either of high precision or spanning a broad incident energy range, information on legacy measurements explaining discrepancies and recently measured data of the average total kinetic energy as a function of incident neutron energy. The resulting evaluated data and covariances agree well with the experimental database used for the evaluation. However, the evaluated spectra are softer than the 235U and 239Pu ENDF/B-VII.1, JENDL-4.0 and JEFF-3.2 evaluations for incident neutron energies E inc ≤ 1.5 MeV and E inc ≤ 5 MeV, respectively. For E inc > 5 MeV, the evaluated spectra show structures due to the improved modeling which are not present in ENDF/B-VII.1 and JEFF-3.2 but can be observed in JENDL-4.0 evaluations. Part of these new evaluations were adopted for ENDF/B-VIII.0, while the ENDF/B-VII.1 239Pu PFNS was retained for E inc ≤ 5 MeV awaiting more conclusive experimental evidence.« less

Evaluations of Energy Spectra of Neutrons Emitted Promptly in Neutron-induced Fission of 235 U and 239 Pu

DOE Office of Scientific and Technical Information (OSTI.GOV)

Neudecker, Denise; Talou, Patrick; Kawano, Toshihiko

The energy spectra of neutrons emitted promptly in the neutron-induced fission reactions of 235U and 239Pu were re-evaluated for ENDF/B-VIII.0. The evaluations presented here are based on a careful modeling of all relevant physics processes, an extensive analysis of experimental data and a detailed quantification of pertinent uncertainties. Energy spectra of neutrons emitted in up to fourth chance fission are considered and both compound and pre-equilibrium processes are included. Also, important nuclear model parameters, such as the average total kinetic energy of the fission fragments and the multiple chance fission probabilities, and their uncertainties are estimated based on experimental knowledge,more » model information and evaluated data. In addition to experimental information already available for ENDF/B-VII.1, these new evaluations make use of recently published experimental data either of high precision or spanning a broad incident energy range, information on legacy measurements explaining discrepancies and recently measured data of the average total kinetic energy as a function of incident neutron energy. The resulting evaluated data and covariances agree well with the experimental database used for the evaluation. However, the evaluated spectra are softer than the 235U and 239Pu ENDF/B-VII.1, JENDL-4.0 and JEFF-3.2 evaluations for incident neutron energies E inc ≤ 1.5 MeV and E inc ≤ 5 MeV, respectively. For E inc > 5 MeV, the evaluated spectra show structures due to the improved modeling which are not present in ENDF/B-VII.1 and JEFF-3.2 but can be observed in JENDL-4.0 evaluations. Part of these new evaluations were adopted for ENDF/B-VIII.0, while the ENDF/B-VII.1 239Pu PFNS was retained for E inc ≤ 5 MeV awaiting more conclusive experimental evidence.« less

Specificity of DNA vaccines against the U and M genogroups of infectious hematopoietic necrosis virus (IHNV) in rainbow trout (Oncorhynchus mykiss)

USGS Publications Warehouse

Penaranda, M.M.D.; LaPatra, S.E.; Kurath, G.

2011-01-01

Infectious hematopoietic necrosis virus (IHNV) is a fish rhabdovirus that causes significant mortality in salmonid species. In North America IHNV has three major genogroups designated U, M, and L. Host-specificity of the M and U genogroups of IHNV has been established both in the field and in experimental challenges, with M isolates being more prevalent and more virulent in rainbow trout (Oncorhynchus mykiss), and U isolates being more prevalent and highly virulent in sockeye salmon (Oncorhynchus nerka). In this study, efficacy of DNA vaccines containing either M (pM) or U (pU) virus glycoprotein genes was investigated during intra- and cross-genogroup challenges in rainbow trout. In virus challenges at 7 days post-vaccination (early antiviral response), both pM and pU were highly protective against either M or U IHNV. In challenges at 28 days post-vaccination (specific antiviral response), both pM and pU were protective against M IHNV but the homologous pM vaccine was significantly more protective than pU in one of two experiments. At this stage both pM and pU induced comparably high protection against U IHNV challenge. Correlates of protection were also investigated by assessing the expression of the interferon-stimulated gene Mx-1 and the production of neutralizing antibodies (NAbs) following pM or pU DNA vaccination. Mx-1 gene expression, measured at 4 and 7 days post-vaccination as an indicator of the host innate immune response, was found to be significantly higher after pM than pU vaccination in some cases. Neutralizing antibody was produced in response to the two vaccines, but antibody titers did not show consistent correlation with protection. The results show that the rainbow trout innate and adaptive immune responses have some ability to distinguish between the U and M genogroup IHNV, but overall the pM and pU vaccines were protective against both homologous and cross-genogroup challenges.

Temporal geochemical variations in lavas from Kīlauea's Pu`u `Ō`ō eruption (1983-2010): Cyclic variations from melting of source heterogeneities

NASA Astrophysics Data System (ADS)

Greene, Andrew R.; Garcia, Michael O.; Pietruszka, Aaron J.; Weis, Dominique; Marske, Jared P.; Vollinger, Michael J.; Eiler, John

2013-11-01

Geochemical time series analysis of lavas from Kīlauea's ongoing Pu`u `Ō`ō eruption chronicle mantle and crustal processes during a single, prolonged (1983 to present) magmatic event, which has shown nearly two-fold variation in lava effusion rates. Here we present an update of our ongoing monitoring of the geochemical variations of Pu`u `Ō`ō lavas for the entire eruption through 2010. Oxygen isotope measurements on Pu`u `Ō`ō lavas show a remarkable range (δ18O values of 4.6-5.6‰), which are interpreted to reflect moderate levels of oxygen isotope exchange with or crustal contamination by hydrothermally altered Kīlauea lavas, probably in the shallow reservoir under the Pu`u `Ō`ō vent. This process has not measurably affected ratios of radiogenic isotope or incompatible trace elements, which are thought to vary due to mantle-derived changes in the composition of the parental magma delivered to the volcano. High-precision Pb and Sr isotopic measurements were performed on lavas erupted at ˜6 month intervals since 1983 to provide insights about melting dynamics and the compositional structure of the Hawaiian plume. The new results show systematic variations of Pb and Sr isotope ratios that continued the long-term compositional trend for Kīlauea until ˜1990. Afterward, Pb isotope ratios show two cycles with ˜10 year periods, whereas the Sr isotope ratios continued to increase until ˜2003 and then shifted toward slightly less radiogenic values. The short-term periodicity of Pb isotope ratios may reflect melt extraction from mantle with a fine-scale pattern of repeating source heterogeneities or strands, which are about 1-3 km in diameter. Over the last 30 years, Pu`u `Ō`ō lavas show 15% and 25% of the known isotopic variation for Kīlauea and Mauna Kea, respectively. This observation illustrates that the dominant time scale of mantle-derived compositional variation for Hawaiian lavas is years to decades.

Next-generation purex flowsheets with acetohydroxamic acid as complexant for FBR and thermal-fuel reprocessing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kumar, Shekhar; Koganti, S.B.

2008-07-01

Acetohydroxamic acid (AHA) is a novel complexant for recycle of nuclear-fuel materials. It can be used in ordinary centrifugal extractors, eliminating the need for electro-redox equipment or complex maintenance requirements in a remotely maintained hot cell. In this work, the effect of AHA on Pu(IV) distribution ratios in 30% TBP system was quantified, modeled, and integrated in SIMPSEX code. Two sets of batch experiments involving macro Pu concentrations (conducted at IGCAR) and one high-Pu flowsheet (literature) were simulated for AHA based U-Pu separation. Based on the simulation and validation results, AHA based next-generation reprocessing flowsheets are proposed for co-processing basedmore » FBR and thermal-fuel reprocessing as well as evaporator-less macro-level Pu concentration process required for MOX fuel fabrication. Utilization of AHA results in significant simplification in plant design and simpler technology implementations with significant cost savings. (authors)« less

Chemical potential of carbon in the system UPuCON: Measurements and calculation

NASA Astrophysics Data System (ADS)

Anthonysamy, S.; Ananthasivan, K.; Kahappan, I.; Chandramouli, V.; Vasudeva Rao, P. R.; Mathews, C. K.; Jacob, K. T.

1995-05-01

The carbon potential of (U,Pu) mixed carbides with Pu/(U + Pu) ratios of 0.55 and 0.70 was measured in the temperature range 973 to 1173 K by employing a methane-hydrogen gas equilibration technique. The technique was validated by measuring the Gibbs energy of formation of WC. The compatibility of the mixed carbides with the stainless steel clad was analysed by using the measured carbon potentials. The carbon potentials of mixed carbides of other compositions were calculated theoretically in order to assess their compatibility. The calculations assume ideal solution behavior for all the solid solutions present in the UPuCON system.

Recent advances in the study of the UO2-PuO2 phase diagram at high temperatures

NASA Astrophysics Data System (ADS)

Böhler, R.; Welland, M. J.; Prieur, D.; Cakir, P.; Vitova, T.; Pruessmann, T.; Pidchenko, I.; Hennig, C.; Guéneau, C.; Konings, R. J. M.; Manara, D.

2014-05-01

Recently, novel container-less laser heating experimental data have been published on the melting behaviour of pure PuO2 and PuO2-rich compositions in the uranium dioxide-plutonium dioxide system. Such data showed that previous data obtained by more traditional furnace heating techniques were affected by extensive interaction between the sample and its containment. It is therefore paramount to check whether data so far used by nuclear engineers for the uranium-rich side of the pseudo-binary dioxide system can be confirmed or not. In the present work, new data are presented both in the UO2-rich part of the phase diagram, most interesting for the uranium-plutonium dioxide based nuclear fuel safety, and in the PuO2 side. The new results confirm earlier furnace heating data in the uranium-dioxide rich part of the phase diagram, and more recent laser-heating data in the plutonium-dioxide side of the system. As a consequence, it is also confirmed that a minimum melting point must exist in the UO2-PuO2 system, at a composition between x(PuO2) = 0.4 and x(PuO2) = 0.7 and 2900 K ⩽ T ⩽ 3000 K. Taking into account that, especially at high temperature, oxygen chemistry has an effect on the reported phase boundary uncertainties, the current results should be projected in the ternary U-Pu-O system. This aspect has been extensively studied here by X-ray diffraction and X-ray absorption spectroscopy. The current results suggest that uncertainty bands related to oxygen behaviour in the equilibria between condensed phases and gas should not significantly affect the qualitative trend of the current solid-liquid phase boundaries.

Ultra low-level measurements of actinides by sector field ICP-MS.

PubMed

Pointurier, F; Baglan, N; Hémet, P

2004-01-01

In the present work, a double-focusing sector field inductively coupled plasma-mass spectrometer was optimised for ultra trace and isotopic analyses of actinide long-lived isotopes in low concentration solutions of the fgml(-1) to the ngml(-1) range. Sensitivities of about 3GHz/(microgml(-1)), with as low a background as 0.1cps, were obtained for U using a conventional concentric pneumatic nebuliser. Detection limits are below the fg range for 239Pu and 240Pu. With natural U, a precision lower than 0.5% RSD is currently obtained for 235U/238U isotopic ratio at the 200pgml(-1) level.

Vaporization chemistry of hypo-stoichiometric (U,Pu)O 2

NASA Astrophysics Data System (ADS)

Viswanathan, R.; Krishnaiah, M. V.

2001-04-01

Calculations were performed on hypo-stoichiometric uranium plutonium di-oxide to examine its vaporization behavior as a function of O/ M ( M= U+ Pu) ratio and plutonium content. The phase U (1- y) Pu yO z was treated as an ideal solid solution of (1- y)UO 2+ yPuO (2- x) such that x=(2- z)/ y. Oxygen potentials for different desired values of y, z, and temperature were used as the primary input to calculate the corresponding partial pressures of various O-, U-, and Pu-bearing gaseous species. Relevant thermodynamic data for the solid phases UO 2 and PuO (2- x) , and the gaseous species were taken from the literature. Total vapor pressure varies with O/M and goes through a minimum. This minimum does not indicate a congruently vaporizing composition. Vaporization behavior of this system can at best be quasi-congruent. Two quasi-congruently vaporizing compositions (QCVCs) exist, representing the equalities (O/M) vapor=(O/M) mixed-oxide and (U/Pu) vapor=(U/Pu) mixed-oxide, respectively. The (O/M) corresponding to QCVC1 is lower than that corresponding to QCVC2, but very close to the value where vapor pressure minimum occurs. The O/M values of both QCVCs increase with decrease in plutonium content. The vaporization chemistry of this system, on continuous vaporization under dynamic condition, is discussed.

Association of actinides with microorganisms and clay: Implications for radionuclide migration from waste-repository sites

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ohnuki, T.; Francis, A.; Kozai, N.

2010-04-01

We conducted a series of basic studies on the microbial accumulation of actinides to elucidate their migration behavior around backfill materials used in the geological disposal of radioactive wastes. We explored the interactions of U(VI) and Pu(VI) with Bacillus subtilis, kaolinite clay, and within a mixture of the two, directly analyzing their association with the bacterium in the mixture by transmission electron microscopy (TEM) and scanning electron microscopy (SEM). The accumulation of U by the mixture rose as the numbers of B. subtilis cells increased. Treating the kaolinite with potassium acetate (CH{sub 3}COOK) removed approximately 80% of the associated uraniummore » while only 65% was removed in the presence of B. subtilis. TEM-EDS analysis confirmed that most of the U taken from solution was associated with B. subtilis. XANES analyses revealed that the oxidation state of uranium associated with B. subtilis, kaolinite, and with the mixture containing both was U(VI). The amount of Pu sorbed by B. subtilis increased with time, but did not reach equilibrium in 48 h; in kaolinite alone, equilibrium was attained within 8 h. After 48 h, the oxidation state of Pu in the solutions exposed to B. subtilis and to the mixture had changed to Pu(V), whereas the oxidation state of the Pu associated with both was Pu(IV). In contrast, there was no change in the oxidation state of Pu in the solution nor on kaolinite after exposure to Pu(VI). SEM-EDS analysis indicated that most of the Pu in the mixture was associated with the bacteria. These results suggest that U(VI) and Pu(VI) preferentially are sorbed to bacterial cells in the presence of kaolinite clay, and that the mechanism of accumulation of U and Pu differs. U(VI) is sorbed directly to the bacterial cells, whereas Pu(VI) first is reduced to Pu(V) and then to Pu(IV), and the latter is associated with the cells. These results have important implications on the migrations of radionuclides around the repository sites of geological disposal. Microbial cells compete with clay colloids for radionuclides accumulation, and because of their higher affinity and larger size, the microbes accumulate radionuclides and migrate much slower than do the clay colloids. Additionally, biofilm coatings formed on the fractured rock surfaces also accumulate radionuclides, thereby retarding radionuclide migration.« less

Melting behavior of mixed U-Pu oxides under oxidizing conditions

NASA Astrophysics Data System (ADS)

Strach, Michal; Manara, Dario; Belin, Renaud C.; Rogez, Jacques

2016-05-01

In order to use mixed U-Pu oxide ceramics in present and future nuclear reactors, their physical and chemical properties need to be well determined. The behavior of stoichiometric (U,Pu)O2 compounds is relatively well understood, but the effects of oxygen stoichiometry on the fuel performance and stability are often still obscure. In the present work, a series of laser melting experiments were carried out to determine the impact of an oxidizing atmosphere, and in consequence the departure from a stoichiometric composition on the melting behavior of six mixed uranium plutonium oxides with Pu content ranging from 14 to 62 wt%. The starting materials were disks cut from sintered stoichiometric pellets. For each composition we have performed two laser melting experiments in pressurized air, each consisting of four shots of different duration and intensity. During the experiments we recorded the temperature at the surface of the sample with a pyrometer. Phase transitions were qualitatively identified with the help of a reflected blue laser. The observed phase transitions occur at a systematically lower temperature, the lower the Pu content of the studied sample. It is consistent with the fact that uranium dioxide is easily oxidized at elevated temperatures, forming chemical species rich in oxygen, which melt at a lower temperature and are more volatile. To our knowledge this campaign is a first attempt to quantitatively determine the effect of O/M on the melting temperature of MOX.

Improved precision and accuracy in quantifying plutonium isotope ratios by RIMS

DOE PAGES

Isselhardt, B. H.; Savina, M. R.; Kucher, A.; ...

2015-09-01

Resonance ionization mass spectrometry (RIMS) holds the promise of rapid, isobar-free quantification of actinide isotope ratios in as-received materials (i.e. not chemically purified). Recent progress in achieving this potential using two Pu test materials is presented. RIMS measurements were conducted multiple times over a period of two months on two different Pu solutions deposited on metal surfaces. Measurements were bracketed with a Pu isotopic standard, and yielded absolute accuracies of the measured 240Pu/ 239Pu ratios of 0.7% and 0.58%, with precisions (95% confidence intervals) of 1.49% and 0.91%. In conclusion, the minor isotope 238Pu was also quantified despite the presencemore » of a significant quantity of 238U in the samples.« less

Extinct Plutonium Geochemistry of Ancient Hadean Zircons

NASA Astrophysics Data System (ADS)

Turner, G.; Gilmour, J.; Crowther, S.; Busfield, A.; Mojzsis, S.; Harrison, M.

2005-12-01

The abundance of 244Pu in the early solar system has important implications for r-process nucleosynthesis and models of noble gas transport within the Earth's mantle. Our recent discovery(1) of xenon isotopes from the in-situ decay of 244Pu in ancient Jack Hills zircons promises to provide a new time-sensitive window on the first 500 Ma of Earth history. We have extended this initial work by the use of resonance ioniisation mass spectrometry to analyse xenon released by stepped heating from 17 individual zircons with Pb-Pb ages in the range 3.95 to 4.18 Ga. Our immediate objectives are to determine the causes of variations in the inferred Pu/U ratios and in the longer term to determine the initial Pu/U ratio of the Earth. The Pu/U ratios calculated for individual zircons may be expected to vary as a result of igneous fractionation and also from differential loss of Pu and U fission xenon in the last 4 Ga. We have studied the effects of xenon loss by irradiating the zircons with thermal neutrons to generate xenon from 235U neutron fission in order to determine U/Xe ratios and apparent ages. 131Xe/134Xe and 132Xe/134Xe ratios can be used to calculate the relative contributions from 244Pu and 238U spontaneous fission and 235U neutron fission. The measured Pu/U ratios (back calculated to 4.56 Ga on the basis of the individual Pb-Pb ages) range from zero to 0.012. The highest ratio in our initial study was 0.008 (note that the published ratio has been revised upwards on the basis of improved decay parameters for 238U spontaneous fission). Comparison of Pb-Pb and U-Xe ages indicate varying amounts of xenon loss, over 50% in some cases. While this accounts for some of the variability in the inferred Pu/U, igneous fractionation may also play a part, and we are currently attempting to investigate this by a comparison with REE abundances. Reference: (1) Turner et al. (2004) Science, 306, 89-91.

Chemical potential of oxygen in (U, Pu) mixed oxide with Pu/(U+Pu) = 0.46

NASA Astrophysics Data System (ADS)

Dawar, Rimpi; Chandramouli, V.; Anthonysamy, S.

2016-05-01

Chemical potential of oxygen in (U,Pu) mixed oxide with Pu/(U + Pu) = 0.46 was measured for the first time using H2/H2O gas equilibration combined with solid electrolyte EMF technique at 1073, 1273 and 1473 K covering an oxygen potential range of -525 to -325 kJ mol-1. The effect of oxygen potential on the oxygen to metal ratio was determined. Increase in oxygen potential increases the O/M. In this study the minimum O/M obtained was 1.985 below which reduction was not possible. Partial molar enthalpy ΔHbar O2 and entropy ΔSbar O2 of oxygen were calculated from the oxygen potential data. The values of -752.36 kJ mol-1 and 0.25 kJ mol-1 were obtained for ΔHbar O2 and ΔSbar O2 respectively.

Actinide abundances in ordinary chondrites

USGS Publications Warehouse

Hagee, B.; Bernatowicz, T.J.; Podosek, F.A.; Johnson, M.L.; Burnett, D.S.; Tatsumoto, M.

1990-01-01

Measurements of 244Pu fission Xe, U, Th, and light REE (LREE) abundances, along with modal petrographic determinations of phosphate abundances, were carried out on equilibrated ordinary chondrites in order to define better the solar system Pu abundance and to determine the degree of variation of actinide and LREE abundances. Our data permit comparison of the directly measured Pu/ U ratio with that determined indirectly as (Pu/Nd) ?? (Nd/U) assuming that Pu behaves chemically as a LREE. Except for Guaren??a, and perhaps H chondrites in general, Pu concentrations are similar to that determined previously for St. Se??verin, although less precise because of higher trapped Xe contents. Trapped 130Xe 136Xe ratios appear to vary from meteorite to meteorite, but, relative to AVCC, all are similar in the sense of having less of the interstellar heavy Xe found in carbonaceous chondrite acid residues. The Pu/U and Pu/Nd ratios are consistent with previous data for St. Se??verin, but both tend to be slightly higher than those inferred from previous data on Angra dos Reis. Although significant variations exist, the distribution of our Th/U ratios, along with other precise isotope dilution data for ordinary chondrites, is rather symmetric about the CI chondrite value; however, actinide/(LREE) ratios are systematically lower than the CI value. Variations in actinide or LREE absolute and relative abundances are interpreted as reflecting differences in the proportions and/or compositions of more primitive components (chondrules and CAI materials?) incorporated into different regions of the ordinary chondrite parent bodies. The observed variations of Th/U, Nd/U, or Ce/U suggest that measurements of Pu/U on any single equilibrated ordinary chondrite specimen, such as St. Se??verin, should statistically be within ??20-30% of the average solar system value, although it is also clear that anomalous samples exist. ?? 1990.

The basic features of a closed fuel cycle without fast reactors

NASA Astrophysics Data System (ADS)

Bobrov, E. A.; Alekseev, P. N.; Teplov, P. S.

2017-01-01

In this paper the basic features of a closed fuel cycle with thermal reactors are considered. The three variants of multiple Pu and U recycling in VVER reactors was investigated. The comparison of MOX and REMIX fuel approaches for closed fuel cycle with thermal reactors is presented. All variants make possible to recycle several times the total amount of Pu and U obtained from spent fuel. The reported study was funded by RFBR according to the research project № 16-38-00021

Fractionation in the solar nebula. II - Condensation of Th, U, Pu and Cm

NASA Technical Reports Server (NTRS)

Boynton, W. V.

1978-01-01

Reasonable assumptions concerning activity coefficients allow the calculation of the relative volatility of the actinide elements under conditions expected during the early history of the solar system. Several of the light rare earths have volatilities similar to Pu and Cm and can be used as indicators of the degree of fractionation of these extinct elements. Uranium is considerably more volatile than either Pu or Cm, leading to fractionations of about a factor of 50 and 90 in the Pu/U and Cm/U ratio in the earliest condensates from the solar nebula. Ca,Al-rich inclusions from the Allende meteorite, including the coarse-grained inclusions, have a depletion of U relative to La of about a factor of three, suggesting that these inclusions may have been isolated from the nebular gas before condensation of U was complete. The inclusions, however, can be used to determine solar Pu/U and Cm/U ratios if the rare earth patterns are determined in addition to the other normal measurements.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vorobev, A.M.; Kuzmina, V.P.

A method is described for determining Pu in the presence of large quantities of U. Pu is extracted using thenoyltrifluoroacetone (TTA) and precipitated using bismuth phosphate. In contrast to U (VI), plutonium (IV) is easily separated by TTA from 1M nitric acid and lends itself to quantitative precipitation. The yield of Pu amounted to 90%. The presence of U/sup 235/ in quantities exceeding 200-fold the Pu content did not influence the determination in 10-mg specimens. The order of error was plus or minus 20%. (R.V.J.)

The June-July 2007 collapse and refilling of Puʻu ʻŌʻō Crater, Kilauea Volcano, Hawaiʻi

USGS Publications Warehouse

Orr, Tim R.

2014-01-01

Episode 57 of Kīlauea’s long-lived east rift zone eruption was characterized by lava effusion and spattering within the crater at Puʻu ʻŌʻō that lasted from July 1 to July 20, 2007. This eruptive episode represented a resumption of activity following a 12-day eruptive hiatus on Kīlauea associated with the episode 56 intrusion and eruption near Kāne Nui o Hamo cone, uprift from Puʻu ʻŌʻō, on June 17–19, 2007. The withdrawal of magma from beneath Puʻu ʻŌʻō led to the collapse of Puʻu ʻŌʻō’s crater floor, forming a concave depression ~85 m deep. After the hiatus, episode 57 lava began to erupt from two vents within Puʻu ʻŌʻō, quickly constructing a lava lake and filling the crater to within 5 m of the precollapse lava level (25 m of the pre-collapse crater floor). Starting July 8, effusion waned as the crater floor began to rise. As uplift progressed, new vents opened along a circumferential fracture that accommodated the displacement. The bulk volume of filling within the Puʻu ʻŌʻō crater and flank pits during episode 57, including both surficial lava accumulation and endogenous growth, is estimated at 1.3×106 m3. This volume equates to a time-averaged dense rock equivalent accumulation rate of 0.6 m3 s-1, which is an order of magnitude less than the supply rate to the volcano at that time, suggesting that most of the magma entering the volcano was being stored. Eruptive activity in Puʻu ʻŌʻō ended late on July 20, and the floor of the crater began to subside rapidly. Shortly afterward, early on July 21, a new fissure eruption started on the northeast flank of Puʻu ʻŌʻō, marking the onset of episode 58. The June–July 2007 collapse and refilling of the Puʻu ʻŌʻō crater, culminating in a new breakout outside of Puʻu ʻŌʻō, illustrates the response of a long-lived eruptive center in Kīlauea’s East Rift Zone to an uprift intrusion. Variations of this pattern occurred several times at Puʻu ʻŌʻō before 2007 and have occurred again since. Recognition of this pattern has improved the monitoring capability of the Hawaiian Volcano Observatory and will aid in future eruption response efforts.

Specificity of DNA vaccines against the U and M genogroups of infectious hematopoietic necrosis virus (IHNV) in rainbow trout (Oncorhynchus mykiss).

PubMed

Peñaranda, Ma Michelle D; Lapatra, Scott E; Kurath, Gael

2011-07-01

Infectious hematopoietic necrosis virus (IHNV) is a fish rhabdovirus that causes significant mortality in salmonid species. In North America IHNV has three major genogroups designated U, M, and L. Host-specificity of the M and U genogroups of IHNV has been established both in the field and in experimental challenges, with M isolates being more prevalent and more virulent in rainbow trout (Oncorhynchus mykiss), and U isolates being more prevalent and highly virulent in sockeye salmon (Oncorhynchus nerka). In this study, efficacy of DNA vaccines containing either M (pM) or U (pU) virus glycoprotein genes was investigated during intra- and cross-genogroup challenges in rainbow trout. In virus challenges at 7 days post-vaccination (early antiviral response), both pM and pU were highly protective against either M or U IHNV. In challenges at 28 days post-vaccination (specific antiviral response), both pM and pU were protective against M IHNV but the homologous pM vaccine was significantly more protective than pU in one of two experiments. At this stage both pM and pU induced comparably high protection against U IHNV challenge. Correlates of protection were also investigated by assessing the expression of the interferon-stimulated gene Mx-1 and the production of neutralizing antibodies (NAbs) following pM or pU DNA vaccination. Mx-1 gene expression, measured at 4 and 7 days post-vaccination as an indicator of the host innate immune response, was found to be significantly higher after pM than pU vaccination in some cases. Neutralizing antibody was produced in response to the two vaccines, but antibody titers did not show consistent correlation with protection. The results show that the rainbow trout innate and adaptive immune responses have some ability to distinguish between the U and M genogroup IHNV, but overall the pM and pU vaccines were protective against both homologous and cross-genogroup challenges. Copyright © 2011 Elsevier Ltd. All rights reserved.

Effect of Spin-Orbit Coupling on the Actinide Dioxides AnO2 (An=Th, Pa, U, Np, Pu, and Am): A Screened Hybrid Density Functional Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wen, Xiaodong; Martin, Richard L.; Roy, Lindsay E.

2012-10-21

We present a systematic comparison of the lattice structures, electronic density of states, and band gaps of actinide dioxides, AnO₂ (An=Th, Pa, U, Np, Pu, and Am) predicted by the Heyd-Scuseria-Ernzerhof screened hybrid density functional (HSE) with the self-consistent inclusion of spin-orbit coupling(SOC). The computed HSE lattice constants and band gaps of AnO₂ are in consistently good agreement with the available experimental data across the series, and differ little from earlier HSE results without SOC. ThO₂ is a simple band insulator (f⁰), while PaO₂, UO₂, and NpO₂ are predicted to be Mott insulators. The remainders (PuO₂ and AmO₂) show considerablemore » O2p/An5f mixing and are classified as charge-transfer insulators. We also compare our results for UO₂, NpO₂, and PuO₂with the PBE+U, self interaction correction (SIC), and dynamic mean-field theory (DMFT) many-body approximations.« less

Transmission of magmatic pressure changes at Kilauea volcano

NASA Astrophysics Data System (ADS)

Montagna, C. P.; Gonnermann, H. M.

2012-12-01

Volcanic eruptions are often accompanied by spatiotemporal migration of ground deformation, a consequence of pressure changes within magma reservoirs and pathways. We have modeled the propagation of such pressure variations, caused by eruptive magma withdrawal during the early eruptive episodes of the ongoing Pu`u `O`o-Kupaianaha eruption of Kilauea volcano. Tilt measurements show that the onset of eruptive episodes at Pu`u `O`o was typically accompanied by abrupt deflation and followed by a sudden onset of gradual re-inflation, once the eruptive episode ended. Tilt of Kilauea's summit underwent similar patterns of deflation and inflation, albeit with a time delay of several hours during most episodes. The observed delay times can be reproduced by a numerical model of pressure variations within an elastic-walled dike that connects Kilauea's summit to its east rift zone. As pressure changes travel through the dike, the interplay between elastic response of the dike wall and viscous resistance of the fluid determines the delay time. An example of the ability of the model to reproduce observed tilt data is presented in Figure 1, which shows measured tilt at Pu`u `O`o during episode 18, together with measured and modeled tilt at Kilauea's summit. Magma withdrawal beneath Pu`u `O`o causes a decrease in pressure and deflation. This pressure change is estimated from observed ground deformation, and it constitutes the time-dependent model boundary condition at Pu`u `O`o, which propagates to Kilauea's summit. The resultant increase in magma flux causes deflation of Kilauea's Halema`uma`u magma reservoir and the change and time delay of tilt are reproduced by the model. The time delay depends on elasticity of the wall rock, dike dimensions, magma viscosity, as well as magnitude and duration of the pressure variations themselves. In addition, these parameters also affect the attenuation of the amplitude of the pressure variation, as it travels between Puu Oo and summit. Pressure changes propagate noticeably faster (slower) in a slightly wider (narrower) dike, as a consequence of smaller (larger) viscous dissipation. Time delays and amplitude of deflation-inflation events at Kilauea have the potential to provide information on effective transport properties of magmatic pathways and changes thereof over time.bserved and modeled change in normalized tilt at Pu`u `O`o and summit for episode 18 of the Pu`u `O`o eruption

Deviation between the chemistry of Ce(IV) and Pu(IV) and routes to ordered and disordered heterobimetallic 4f/5f and 5f/5f phosphonates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Diwu, Juan; Wang, Shuao; Good, Justin J.

2011-06-06

The heterobimetallic actinide compound UO₂Ce(H₂O)[C₆H₄(PO₃H)₂]₂·H₂O was prepared via the hydrothermal reaction of U(VI) and Ce(IV) in the presence of 1,2-phenylenediphosphonic acid. We demonstrate that this is a kinetic product that is not stable with respect to decomposition to the monometallic compounds. Similar reactions have been explored with U(VI) and Ce(III), resulting in the oxidation of Ce(III) to Ce(IV) and the formation of the Ce(IV) phosphonate, Ce[C₆H₄(PO₃H)(PO₃H₂)][C₆H₄(PO₃H)(PO₃)]·2H₂O, UO₂Ce(H₂O)[C₆H₄(PO₃H)₂]₂·H₂O, and UO₂[C₆H₄(PO₃H)₂](H₂O)·H₂O. In comparison, the reaction of U(VI) with Np(VI) only yields Np[C₆H₄(PO₃H)₂]₂·2H₂O and aqueous U(VI), whereas the reaction of U(VI) with Pu(VI) yields the disordered U(VI)/Pu(VI) compound, (U 0.9Pu 0.1)O₂[C₆H₄(PO₃H)₂](H₂O)·H₂O, and themore » Pu(IV) phosphonate, Pu[C₆H₄(PO₃H)(PO₃H₂)][C₆H₄(PO₃H)(PO₃)]·2H₂O. The reactions of Ce(IV) with Np(VI) yield disordered heterobimetallic phosphonates with both M[C₆H₄(PO₃H)(PO₃H₂)][C₆H₄(PO₃H)(PO₃)]·2H₂O (M = Ce, Np) and M[C₆H₄(PO₃H)₂]₂·2H₂O (M = Ce, Np) structures, as well as the Ce(IV) phosphonate Ce[C₆H₄(PO₃H)(PO₃H₂)][C₆H₄(PO₃H)(PO₃)]·2H₂O. Ce(IV) reacts with Pu(IV) to yield the Pu(VI) compound, PuO₂[C₆H₄(PO₃H)₂](H₂O)·3H₂O, and a disordered heterobimetallic Pu(IV)/Ce(IV) compound with the M[C₆H₄(PO₃H)(PO₃H₂)][C₆H₄(PO₃H)(PO₃)]·2H₂O (M = Ce, Pu) structure. Mixtures of Np(VI) and Pu(VI) yield disordered heterobimetallic Np(IV)/Pu(IV) phosphonates with both the An[C₆H₄(PO₃H)(PO₃H₂)][C₆H₄(PO₃H)(PO₃)]·2H₂O (M = Np, Pu) and An[C₆H₄(PO₃H)₂]₂·2H₂O (M = Np, Pu) formulas.« less

Results of irradiation of (U0.55Pu0.45)N and (U0.4Pu0.6)N fuels in BOR-60 up to ˜12 at.% burn-up

NASA Astrophysics Data System (ADS)

Rogozkin, B. D.; Stepennova, N. M.; Fedorov, Yu. Ye.; Shishkov, M. G.; Kryukov, F. N.; Kuzmin, S. V.; Nikitin, O. N.; Belyaeva, A. V.; Zabudko, L. M.

2013-09-01

In the article presented are the results of post-irradiation tests of helium bonded fuel pins with mixed mononitride fuel (U0.55Pu0.45)N and (U0.4Pu0.6)N having 85% density irradiated in BOR-60 reactor. Achieved maximum burn-up was, respectively, equal to 9.4 and 12.1 at.% with max linear heat rates 41.9 and 54.5 kW/m. Maximum irradiation dose was 43 dpa. No damage of claddings made of ChS-68 steel (20% cold worked) was observed, and ductility margin existed. Maximum depth of cladding corrosion was within 15 μm. Swelling rates of (U0.4Pu0.6)N and (U0.55Pu0.45)N were, respectively, ˜1.1% and ˜0.68% per 1 at.%. Gas release rate did not exceed 19.3% and 19%. Pattern of porosity distribution in the fuel influenced fuel swelling and gas release rates. Plutonium and uranium are uniformly distributed in the fuel, local minimum values of their content being caused by pores and cracks in the pellets. The observable peaks in content distribution are probably connected with the local formation of isolated phases (e.g. Mo, Pd) while the minimum values refer to fuel pores and cracks. Xenon and cesium tend to migrate from the hot sections of fuel, and therefore their min content is observed in the central section of the fuel pellets. Phase composition of the fuel was determined with X-ray diffractometer. The X-ray patterns of metallographic specimens were obtained by the scanning method (the step was 0.02°, the step exposition was equal to 2 s). From the X-ray diffraction analysis data, it follows that the nitrides of both fuel types have the single-phase structure with an FCC lattice (see Table 6).

Ground Tilt Time Delays between Kilauea Volcano's Summit and East Rift Zone Caused by Magma Reservoir Buffering

NASA Astrophysics Data System (ADS)

Haney, M. M.; Patrick, M. R.; Anderson, K. R.

2016-12-01

A cyclic pattern of ground deformation, called a deflation-inflation (DI) cycle, is commonly observed at Kilauea Volcano, Hawai`i. These cycles are an important part of Kilauea's eruptive activity because they directly influence the level of the summit lava lake as well as the effusion rate (and resulting lava flow hazard) at the East Rift Zone eruption site at Pu`u `O`o. DI events normally span several days, and are measured both at the summit and at Pu`u `O`o cone (20 km distance). Signals appear first at the summit and are then observed at Pu`u `O`o after an apparent delay of between 0.5 and 10 hours, which has been previously interpreted as reflecting magma transport time. We propose an alternate explanation, in which the apparent delay is an artifact of buffering by the small magma reservoir thought to exist at Pu`u `O`o. Simple Poiseuille flow modeling demonstrates that this apparent delay can be reproduced by the changing balance of inflow (from the summit) and outflow (to surface lava flows) at the Pu`u `O`o magma reservoir. The apparent delay is sensitive to the geometry of the conduit leaving Pu`u `O`o, feeding surface lava flows. We demonstrate how the reservoir buffering is quantitatively equivalent to a causal low-pass filter, which explains both the apparent delay as well as the smoothed, skewed nature of the signal at Pu`u `O`o relative to the summit. By comparing summit and Pu`u `O`o ground tilt signals over an extended time period, it may be possible to constrain the changing geometry of the shallow magmatic system through time.

Nuclear weapons produced 236U, 239Pu and 240Pu archived in a Porites Lutea coral from Enewetak Atoll.

PubMed

Froehlich, M B; Tims, S G; Fallon, S J; Wallner, A; Fifield, L K

2017-11-01

A slice from a Porites Lutea coral core collected inside the Enewetak Atoll lagoon, within 15 km of all major nuclear tests conducted at the atoll, was analysed for 236 U, 239 Pu and 240 Pu over the time interval 1952-1964 using a higher time resolution than previously reported for a parallel slice from the same core. In addition two sediment samples from the Koa and Oak craters were analysed. The strong peaks in the concentrations of 236 U and 239 Pu in the testing years are confirmed to be considerably wider than the flushing time of the lagoon. This is likely due to the growth mechanism of the coral. Following the last test in 1958 atom concentrations of both 236 U and 239 Pu decreased from their peak values by more than 95% and showed a seasonal signal thereafter. Between 1959 and 1964 the weighted average of the 240 Pu/ 239 Pu atom ratio is 0.124 ± 0.008 which is similar to that in the lagoon sediments (0.129 ± 0.006) but quite distinct from the global fallout value of ∼0.18. This, and the high 239,240 Pu and 236 U concentrations in the sediments, provides clear evidence that the post-testing signal in the coral is dominated by remobilisation of the isotopes from the lagoon sediments rather than from global fallout. Copyright © 2017 Elsevier Ltd. All rights reserved.

Oxygen potentials of mixed oxide fuels for fast reactors

NASA Astrophysics Data System (ADS)

Kato, M.; Tamura, T.; Konashi, K.

2009-03-01

Oxygen potentials of homogenous (Pu0.2U0.8)O2-x and (Am0.02Pu0.30Np0.02U0.66)O2-x which have been developed as fuels for fast breeder reactors were measured at temperatures of 1473-1623 K by a gas equilibrium method using an (Ar, H2, H2O) gas mixture. The measured oxygen potentials of (Pu0.2U0.8)O2-x were about 25 kJ mol-1 lower than those of (Pu0.3U0.7)O2-x measured previously and were consistent with the values calculated by Besmann and Lindemer's model. The measured oxygen potentials of (Am0.02Pu0.30Np0.02U0.66)O2-x were slightly higher than those of MOX without minor actinides. No fuel-cladding chemical interaction is affected significantly by adding their minor actinides.

Sun photometer and lidar measurements of the plume from the Hawaii Kilauea Volcano Pu'u O'o vent: Aerosol flux and SO2 lifetime

USGS Publications Warehouse

Porter, J.N.; Horton, K.A.; Mouginis-Mark, P. J.; Lienert, B.; Sharma, S.K.; Lau, E.; Sutton, A.J.; Elias, T.; Oppenheimer, C.

2002-01-01

Aerosol optical depths and lidar measurements were obtained under the plume of Hawaii Kilauea Volcano on August 17, 2001, ???9 km downwind from the erupting Pu'u O'o vent. Measured aerosol optical depths (at 500 nm) were between 0.2-0.4. Aerosol size distributions inverted from the spectral sun photometer measurements suggest the volcanic aerosol is present in the accumulation mode (0.1-0.5 micron diameter), which is consistent with past in situ optical counter measurements. The aerosol dry mass flux rate was calculated to be 53 Mg d-1. The estimated SO2 emission rate during the aerosol measurements was ???1450 Mg d-1. Assuming the sulfur emissions at Pu'u O'o vent are mainly SO2 (not aerosol), this corresponds to a SO2 half-life of 6.0 hours in the atmosphere.

Modelling the thermal conductivity of (U xTh 1-x)O 2 and (U xPu 1-x)O 2

DOE PAGES

Cooper, M. W. D.; Middleburgh, S. C.; Grimes, R. W.

2015-07-15

The degradation of thermal conductivity due to the non-uniform cation lattice of (U xTh 1-x)O 2 and (U xPu 1-x)O 2 solid solutions has been investigated by molecular dynamics, using the non-equilibrium method, from 300 to 2000 K. Degradation of thermal conductivity is predicted in (U xTh 1-x)O 2 and (U xPu 1-x)O 2 as compositions deviate from the pure end members: UO 2, PuO 2 and ThO 2. The reduction in thermal conductivity is most apparent at low temperatures where phonon-defect scattering dominates over phonon-phonon interactions. The effect is greater for (U xTh 1-x)O 2 than U xPu 1-x)Omore » 2 due to the greater mismatch in cation size. Parameters for an analytical expressions have been developed that describe the predicted thermal conductivities over the full temperature and compositional ranges. Finally, these expressions may be used in higher level fuel performance codes.« less

Fission Product Yields of 233U, 235U, 238U and 239Pu in Fields of Thermal Neutrons, Fission Neutrons and 14.7-MeV Neutrons

NASA Astrophysics Data System (ADS)

Laurec, J.; Adam, A.; de Bruyne, T.; Bauge, E.; Granier, T.; Aupiais, J.; Bersillon, O.; Le Petit, G.; Authier, N.; Casoli, P.

2010-12-01

The yields of more than fifteen fission products have been carefully measured using radiochemical techniques, for 235U(n,f), 239Pu(n,f) in a thermal spectrum, for 233U(n,f), 235U(n,f), and 239Pu(n,f) reactions in a fission neutron spectrum, and for 233U(n,f), 235U(n,f), 238U(n,f), and 239Pu(n,f) for 14.7 MeV monoenergetic neutrons. Irradiations were performed at the EL3 reactor, at the Caliban and Prospero critical assemblies, and at the Lancelot electrostatic accelerator in CEA-Valduc. Fissions were counted in thin deposits using fission ionization chambers. The number of fission products of each species were measured by gamma spectrometry of co-located thick deposits.

Calibration of the Lawrence Livermore National Laboratory Passive-Active Neutron Drum Shuffler for Measurement of Highly Enriched Uranium in Oxides within DOE-STD-3013-2000 Containers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mount, M E; O'Connell, W J

2005-06-03

Lawrence Livermore National Laboratory (LLNL) uses the LLNL passive-active neutron drum (PAN) shuffler (Canberra Model JCC-92) for accountability measurement of highly enriched uranium (HEU) oxide and HEU in mixed uranium-plutonium (U-Pu) oxide. In June 2002, at the 43rd Annual Meeting of the Institute of Nuclear Material Management, LLNL reported on an extensive effort to calibrate this shuffler, based on standards measurements and extensive simulations, for HEU oxides and mixed U-Pu oxides in thin-walled primary and secondary containers. In August 2002, LLNL began to also use DOE-STD-3013-2000 containers for HEU oxide and mixed U-Pu oxide. These DOE-STD-3013-2000 containers are comprised ofmore » a stainless steel convenience can enclosed in welded stainless steel primary and secondary containers. Compared to the double thin-walled containers, the DOE-STD-3013-2000 containers have substantially thicker walls, and the density of materials in these containers was found to extend over a greater range (1.35 g/cm{sup 3} to 4.62 g/cm{sup 3}) than foreseen for the double thin-walled containers. Further, the DOE-STD-3013-2000 Standard allows for oxides containing at least 30 wt% Pu plus U whereas the calibration algorithms for thin-walled containers were derived for virtually pure HEU or mixed U-Pu oxides. An initial series of Monte Carlo simulations of the PAN shuffler response to given quantities of HEU oxide and mixed U-Pu oxide in DOE-STD-3013-2000 containers was generated and compared with the response predicted by the calibration algorithms for thin-walled containers. Results showed a decrease on the order of 10% in the count rate, and hence a decrease in the calculated U mass for measured unknowns, with some varying trends versus U mass. Therefore a decision was made to develop a calibration algorithm for the PAN shuffler unique to the DOE-STD-3013-2000 container. This paper describes that effort and selected unknown item measurement results.« less

FCRD Transmutation Fuels Handbook 2015

DOE Office of Scientific and Technical Information (OSTI.GOV)

Janney, Dawn Elizabeth; Papesch, Cynthia Ann

2015-09-01

Transmutation of minor actinides such as Np, Am, and Cm in spent nuclear fuel is of international interest because of its potential for reducing the long-term health and safety hazards caused by the radioactivity of the spent fuel. One important approach to transmutation (currently being pursued by the DOE Fuel Cycle Research & Development Advanced Fuels Campaign) involves incorporating the minor actinides into U-Pu-Zr alloys, which can be used as fuel in fast reactors. It is, therefore, important to understand the properties of U-Pu-Zr alloys, both with and without minor actinide additions. In addition to requiring extensive safety precautions, alloysmore » containing U and Pu are difficult to study for numerous reasons, including their complex phase transformations, characteristically sluggish phase-transformation kinetics, tendency to produce experimental results that vary depending on the histories of individual samples, and sensitivity to contaminants such as oxygen in concentrations below a hundred parts per million. Many of the experimental measurements were made before 1980, and the level of documentation for experimental methods and results varies widely. It is, therefore, not surprising that little is known with certainty about U-Pu-Zr alloys, and that general acceptance of results sometimes indicates that there is only a single measurement for a particular property. This handbook summarizes currently available information about U, Pu, Zr, and alloys of two or three of these elements. It contains information about phase diagrams and related information (including phases and phase transformations); heat capacity, entropy, and enthalpy; thermal expansion; and thermal conductivity and diffusivity. In addition to presenting information about materials properties, it attempts to provide information about how well the property is known and how much variation exists between measurements. Although the handbook includes some references to publications about modeling, its primary focus is experimental data. Most of the data has been published elsewhere (although scattered throughout numerous references, some quite obscure); however, some data is presented here for the first time.« less

Seismic and Infrasound Recordings from Kilauea Volcano: Volcanic Tremor, Lava Outbreaks, and Fissure Eruptions

NASA Astrophysics Data System (ADS)

Fee, D.; Garces, M.; Orr, T.

2007-12-01

The continuous effusion from the Pu'u 'O'o crater complex, the active vent of Kilauea Volcano, Hawaii, produced nearly continuous tremor for years. Recently this tremor was recorded by two infrasound arrays, one at 12.5 km and one at 2.5 km, as well as a broadband seismometer at the closer array. These recordings exhibit significant temporal changes. A sharp, complex spectral peak of ~0.6 Hz is present in nearly the entire dataset, and tends to bifurcate and shift frequency over time. Although the seismic wavefield at Kilauea is complex and path effects appear to play a significant role, this spectral peak is also weakly manifested in the seismic recordings. Array processing of the infrasonic data reveals an abundance of broadband signal as well. Most of the signal appears to originate from the main crater region. However, the 2.5 km array detected the presence of a skylight with growing hornitos ~400 m south of Pu'u 'O'o on the active lava tube system. On June 19th, 2007, the magmatic system at Pu'u 'O'o changed. An intrusion of magma reached the surface 6 km west of the crater complex. The timing and location of the lava outbreak were determined acoustically using array processing. Two distinct acoustic pulses were recorded from the correct azimuth, both exhibiting harmonics. The 7/21 fissure eruption also produced clear infrasound signals. The onset of the fissure eruption east of P'u' 'O'o was apparent beginning around midnight on 7/21 and was focused between ~1.5-5 Hz. Although the fissure eruption continued to produce infrasound, the character of the recorded signal changes over time. A third infrasound array was placed closer to P'u' 'O'o and the fissure to help further constrain the eruption. More detailed results on acoustic signals from the Father's Day Intrusion and Fissure eruption will be presented.

Determination of ultra-low level plutonium isotopes (239Pu, 240Pu) in environmental samples with high uranium.

PubMed

Xing, Shan; Zhang, Weichao; Qiao, Jixin; Hou, Xiaolin

2018-09-01

In order to measure trace plutonium and its isotopes ratio ( 240 Pu/ 239 Pu) in environmental samples with a high uranium, an analytical method was developed using radiochemical separation for separation of plutonium from matrix and interfering elements including most of uranium and ICP-MS for measurement of plutonium isotopes. A novel measurement method was established for extensively removing the isobaric interference from uranium ( 238 U 1 H and 238 UH 2 + ) and tailing of 238 U, but significantly improving the measurement sensitivity of plutonium isotopes by employing NH 3 /He as collision/reaction cell gases and MS/MS system in the triple quadrupole ICP-MS instrument. The results show that removal efficiency of uranium interference was improved by more than 15 times, and the sensitivity of plutonium isotopes was increased by a factor of more than 3 compared to the conventional ICP-MS. The mechanism on the effective suppress of 238 U interference for 239 Pu measurement using NH 3 -He reaction gases was explored to be the formation of UNH + and UNH 2 + in the reactions of UH + and U + with NH 3 , while no reaction between NH 3 and Pu + . The detection limits of this method were estimated to be 0.55 fg mL -1 for 239 Pu, 0.09 fg mL -1 for 240 Pu. The analytical precision and accuracy of the method for Pu isotopes concentration and 240 Pu/ 239 Pu atomic ratio were evaluated by analysis of sediment reference materials (IAEA-385 and IAEA-412) with different levels of plutonium and uranium. The developed method were successfully applied to determine 239 Pu and 240 Pu concentrations and 240 Pu/ 239 Pu atomic ratios in soil samples collected in coastal areas of eastern China. Copyright © 2018 Elsevier B.V. All rights reserved.

Method for separating actinides. [Patent application; stripping of Np from organic extractant

DOEpatents

Friedman, H.A.; Toth, L.M.

1980-11-10

An organic solution used for processing spent nuclear reactor fuels is contacted with an aqueous nitric acid solution to strip Np(VI), U(VI), and Pu(IV) from the organic solution into the acid solution. The acid solution is exposed to ultraviolet light, which reduces Np(VI) to Np(V) without reducing U(VI) and Pu(IV). Since the solubility of Np(V) in the organic solution is much lower than that of Np(VI), U(VI), and Pu(IV), a major part of the Np is stripped from the organic solution while leaving most of the U and Pu therein.

Oxygen chemical diffusion in hypo-stoichiometric MOX

NASA Astrophysics Data System (ADS)

Kato, Masato; Morimoto, Kyoichi; Tamura, Tetsuya; Sunaoshi, Takeo; Konashi, Kenji; Aono, Shigenori; Kashimura, Motoaki

2009-06-01

Kinetics of the oxygen-to-metal ratio change in (U 0.8Pu 0.2)O 2-x and (U 0.7Pu 0.3)O 2-x was evaluated in the temperature range of 1523-1623 K using a thermo-gravimetric technique. The oxygen chemical diffusion coefficients were decided as a function of temperature from the kinetics of the reduction process under a hypo-stoichiometric composition. The diffusion coefficient of (U 0.7Pu 0.3)O 2-x was smaller than that of (U 0.8Pu 0.2)O 2-x. No strong dependence was observed for the diffusion coefficient on the O/M variation of samples.

Characterization of Actinides Complexed to Nuclear Fuel Constituents Using ESI-MS.

PubMed

McDonald, Luther W; Campbell, James A; Vercouter, Thomas; Clark, Sue B

2016-03-01

Electrospray ionization-mass spectrometry (ESI-MS) was tested for its use in monitoring spent nuclear fuel (SNF) constituents including U, Pu, dibutyl phosphate (DBP), and tributyl phosphate (TBP). Both positive and negative ion modes were used to evaluate the speciation of U and Pu with TBP and DBP. Furthermore, apparent stability constants were determined for U complexed to TBP and DBP. In positive ion mode, TBP produced a strong signal with and without complexation to U or Pu, but, in negative ion mode, no TBP, U-TBP, or Pu-TBP complexes were observed. Apparent stability constants were determined for [UO2(NO3)2(TBP)2], [UO2(NO3)2(H2O)(TBP)2], and [UO2(NO3)2(TBP)3]. In contrast DBP, U-DBP, and Pu-DBP complexes were observed in both positive and negative ion modes. Apparent stability constants were determined for the species [UO2(DBP)], [UO2(DBP)3], and [UO2(DBP)4]. Analyzing mixtures of U or Pu with TBP and DBP yielded the formation of ternary complexes whose stoichiometry was directly related to the ratio of TBP to DBP. The ESI-MS protocols used in this study will further demonstrate the utility of ESI-MS and its applicability to process control monitoring in SNF reprocessing facilities.

Development of spent fuel reprocessing process based on selective sulfurization: Study on the Pu, Np and Am sulfurization

NASA Astrophysics Data System (ADS)

Kirishima, Akira; Amano, Yuuki; Nihei, Toshifumi; Mitsugashira, Toshiaki; Sato, Nobuaki

2010-03-01

For the recovery of fissile materials from spent nuclear fuel, we have proposed a novel reprocessing process based on selective sulfurization of fission products (FPs). The key concept of this process is utilization of unique chemical property of carbon disulfide (CS2), i.e., it works as a reductant for U3O8 but works as a sulfurizing agent for minor actinides and lanthanides. Sulfurized FPs and minor actinides (MA) are highly soluble to dilute nitric acid while UO2 and PuO2 are hardly soluble, therefore, FPs and MA can be removed from Uranium and Plutonium matrix by selective dissolution. As a feasibility study of this new concept, the sulfurization behaviours of U, Pu, Np, Am and Eu are investigated in this paper by the thermodynamical calculation, phase analysis of chemical analogue elements and tracer experiments.

Chemical Reduction of SIM MOX in Molten Lithium Chloride Using Lithium Metal Reductant

NASA Astrophysics Data System (ADS)

Kato, Tetsuya; Usami, Tsuyoshi; Kurata, Masaki; Inoue, Tadashi; Sims, Howard E.; Jenkins, Jan A.

2007-09-01

A simulated spent oxide fuel in a sintered pellet form, which contained the twelve elements U, Pu, Am, Np, Cm, Ce, Nd, Sm, Ba, Zr,Mo, and Pd, was reduced with Li metal in a molten LiCl bath at 923 K. More than 90% of U and Pu were reduced to metal to form a porous alloy without significant change in the Pu/U ratio. Small fractions of Pu were also combined with Pd to form stable alloys. In the gap of the porous U-Pu alloy, the aggregation of the rare-earth (RE) oxide was observed. Some amount of the RE elements and the actinoides leached from the pellet. The leaching ratio of Am to the initially loaded amount was only several percent, which was far from about 80% obtained in the previous ones on simple MOX including U, Pu, and Am. The difference suggests that a large part of Am existed in the RE oxide rather than in the U-Pu alloy. The detection of the RE elements and actinoides in the molten LiCl bath seemed to indicate that they dissolved into the molten LiCl bath containing the oxide ion, which is the by-product of the reduction, as solubility of RE elements was measured in the molten LiCl-Li2O previously.

The Consequences of Increased Magma Supply to Kilauea Volcano, Hawai`i

NASA Astrophysics Data System (ADS)

Poland, M.; Miklius, A.; Sutton, A. J.; Orr, T.

2007-12-01

The summer of 2007 was a time of intense activity at Kilauea. By mid-2007, ~4 years of summit inflation had uplifted and extended the caldera by 30 cm and 55 cm, respectively. Lava continued to erupt from the Pu`u `O`o vent on the east rift zone (ERZ) during the inflation. On May 24, 2007, two M4+ normal-faulting earthquakes occurred on caldera-bounding faults southeast of the summit. The seismicity did not affect summit inflation, which continued until June 17 when a dike intruded the upper and middle ERZ, causing a pause in the eruption, collapse of Pu`u `O`o's floor, and a small eruption 6 km uprift of Pu`u `O`o. The inflated state of the summit, relative timing of summit deflation and east rift zone extension, and abundant co-intrusive earthquake activity suggest forcible intrusion of magma. Lava returned to Pu`u `O`o by July 2, forming a lake that gradually refilled much of the collapsed crater. Early on July 21, the lake drained suddenly, the cone began to collapse, and a 2-km-long series of discontinuous eruptive fissures opened on and beyond the east flank of Pu`u `O`o. Sesimicity in Kilauea's south flank has been elevated since June and several M3+ earthquakes have occurred there, including a M5.4 on August 13. An increase in magma supply to Kilauea's shallow magmatic system is the probable cause for the events of summer 2007. Summit inflation since 2003 occurred during a period of constant or increasing magma supply to Pu`u `O`o, based on SO2 emissions from the ERZ. The rate of inflation increased markedly in early 2006, and uplift also began in the southwest rift zone. CO2 emissions at the summit, indicative of the quantity of magma degassing beneath Kilauea's caldera, more than doubled between 2003 and 2006. Also since 2003, the ERZ immediately downrift of Pu`u `O`o extended, and subsidence in the lower ERZ ceased. Together, these factors suggest that the magma supply rate to Kilauea's shallow magmatic system (the summit and rift zones above about 5 km depth) approximately doubled between 2003 and 2006. Subsequent volcanic and earthquake activity, including the events of mid-2007, are probably a result (either directly or indirectly) of this increase.

Dynamics of an unusual cone-building trachyte eruption at Pu`u Wa`awa`a, Hualālai volcano, Hawai`i

NASA Astrophysics Data System (ADS)

Shea, Thomas; Leonhardi, Tanis; Giachetti, Thomas; Lindoo, Amanda; Larsen, Jessica; Sinton, John; Parsons, Elliott

2017-04-01

The Pu`u Wa`awa`a pyroclastic cone and Pu`u Anahulu lava flow are two prominent monogenetic eruptive features assumed to result from a single eruption during the trachyte-dominated early post-shield stage of Hualālai volcano (Hawaíi). Púu Wa`awa`a is composed of complex repetitions of crudely cross-stratified units rich in dark dense clasts, which reversely grade into coarser pumice-rich units. Pyroclasts from the cone are extremely diverse texturally, ranging from glassy obsidian to vesicular scoria or pumice, in addition to fully crystalline end-members. The >100-m thick Pu`u Anahulu flow is, in contrast, entirely holocrystalline. Using field observations coupled with whole rock analyses, this study aimed to test whether the Pu`u Wa`awa`a tephra and Pu`u Anahulu lava flows originated from the same eruption, as had been previously assumed. Crystal and vesicle textures are characterized along with the volatile contents of interstitial glasses to determine the origin of textural variability within Pu`u Wáawáa trachytes (e.g., magma mixing vs. degassing origin). We find that (1) the two eruptions likely originated from distinct vents and magma reservoirs, despite their proximity and similar age, (2) the textural diversity of pyroclasts forming Pu`u Wa`awa`a can be fully explained by variable magma degassing and outgassing within the conduit, (3) the Pu`u Wa`awa`a cone was constructed during explosions transitional in style between violent Strombolian and Vulcanian, involving the formation of a large cone and with repeated disruption of conduit plugs, but without production of large pyroclastic density currents (PDCs), and (4) the contrasting eruption styles of Hawaiian trachytes (flow-, cone-, and PDC-forming) are probably related to differences in the outgassing capacity of the magmas prior to reaching the surface and not in intrinsic compositional or temperature properties. These results further highlight that trachytes are "kinetically faster" magmas compared to dacites or rhyolites, likely degassing and crystallizing more rapidly.

Evaluation of N,N-dialkylamides as promising process extractants

NASA Astrophysics Data System (ADS)

Pathak, P. N.; Prabhu, D. R.; Kanekar, A. S.; Manchanda, V. K.

2010-03-01

Studies carried out at BARC, India on the development of new extractants for reprocessing of spent fuel suggested that while straight chain N,N-dihexyloctanamide (DHOA) is promising alternative to TBP for the reprocessing of irradiated uranium based fuels, branched chain N,N-di(2-ethylhexyl)isobutyramide (D2EHIBA) is suitable for the selective recovery of 233U from irradiated Th. In advanced fuel cycle scenarios, the coprocessing of U/Pu stream appears attractive particularly with respect to development of proliferation resistant technologies. DHOA extracted Pu(IV) more efficiently than TBP, both at trace-level concentration as well as under uranium/plutonium loading conditions. Uranium extraction behavior of DHOA was however, similar to that of TBP during the extraction cycle. Stripping behavior of U and Pu (without any reductant) was better for DHOA than that of TBP. It was observed during batch studies that whereas 99% Pu is stripped in four stages in case of DHOA, only 89% Pu is stripped in case of TBP under identical experimental conditions. DHOA offered better fission product decontamination than that of TBP. GANEX (Group ActiNide EXtraction) and ARTIST (Amide-based Radio-resources Treatment with Interim Storage of Transuranics) processes proposed for actinide partitioning use branched chain amides for the selective extraction of uranium from spent fuel feed solutions. The branched-alkyl monoamide (BAMA) proposed to be used in ARTIST process is N,N-di-(2-ethylhexyl)butyramide (D2EHBA). In this context, the extraction behavior of U(VI) and Pu(IV) were compared using D2EHIBA, TBP, and D2EHBA under similar concentration of nitric acid (0.5 — 6M) and of uranium (0-50g/L). These studies suggested that D2EHIBA is a promising extractant for selective extraction of uranium over plutonium in process streams. Similarly, D2EHIBA offered distinctly better decontamination of 233U over Th and fission products under THOREX feed conditions. The possibility of simultaneous stripping and precipitation of thorium (as oxalate) from loaded organic phase was explored using 0.05M oxalic acid. Ammonium diuranate (ADU) precipitation was performed on the oxalate supernatant for the recovery of uranium. Quantitative recovery (>99.9%) of Th as well as of U was achieved. Radiolytic studies suggested that irradiated DHOA and D2EHIBA behaved better with respect to fission product decontamination as compared to that of TBP.

Photon-induced Fission Product Yield Measurements on 235U, 238U, and 239Pu

NASA Astrophysics Data System (ADS)

Krishichayan, Fnu; Bhike, M.; Tonchev, A. P.; Tornow, W.

2015-10-01

During the past three years, a TUNL-LANL-LLNL collaboration has provided data on the fission product yields (FPYs) from quasi-monoenergetic neutron-induced fission of 235U, 238U, and 239Pu at TUNL in the 0.5 to 15 MeV energy range. Recently, we have extended these experiments to photo-fission. We measured the yields of fission fragments ranging from 85Kr to 147Nd from the photo-fission of 235U, 238U, and 239Pu using 13-MeV mono-energetic photon beams at the HIGS facility at TUNL. First of its kind, this measurement will provide a unique platform to explore the effect of the incoming probe on the FPYs, i.e., photons vs. neutrons. A dual-fission ionization chamber was used to determine the number of fissions in the targets and these samples (along with Au monitor foils) were gamma-ray counted in the low-background counting facility at TUNL. Details of the experimental set-up and results will be presented and compared to the FPYs obtained from neutron-induced fission at the same excitation energy of the compound nucleus. Work supported in part by the NNSA-SSAA Grant No. DE-NA0001838.

Laboratory actinide partitioning - Whitlockite/liquid and influence of actinide concentration levels

NASA Technical Reports Server (NTRS)

Benjamin, T. M.; Jones, J. H.; Heuser, W. R.; Burnett, D. S.

1983-01-01

The partition coefficients between synthetic whitlockite (beta Ca-phosphate) and coexisting silicate melts are determined for the actinide elements Th, U and Pu. Experiments were performed at 1 bar pressure and 1250 C at oxygen fugacities from 10 to the -8.5 to 10 to the -0.7 bars, and partitioning was determined from trace element radiography combined with conventional electron microprobe analysis. Results show Pu to be more readily incorporated into crystalline phases than U or Th under reducing conditions, which is attributed to the observation that Pu exists primarily in the trivalent state, while U and Th are tetravalent. Corrected partition coefficients for whitlockite of 3.6, less than or equal to 0.6, 1.2, 0.5 and less than or equal to 0.002 are estimated for Pu(+3), Pu(+4), Th(+4), U(+4) and U(+6), respectively. Experiments performed at trace levels and percent levels of UO2 indicate that Si is involved in U substitution in whitlockite, and show a reduced partition coefficient at higher concentrations of U that can be explained by effects on melt structure or the fraction of tetravalent U.

Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pacold, J. I.; Lukens, W. W.; Booth, C. H.

Nuclear weapons testing generates large volumes of glassy materials that influence the transport of dispersed actinides in the environment and may carry information on the composition of the detonated device. We determine the oxidation state of U and Fe (which is known to buffer the oxidation state of actinide elements and to affect the redox state of groundwater) in samples of melt glass collected from three U.S. nuclear weapons tests. For selected samples, we also determine the coordination geometry of U and Fe, and we report the oxidation state of Pu from one melt glass sample. We find significant variationsmore » among the melt glass samples and, in particular, find a clear deviation in one sample from the expected buffering effect of Fe(II)/Fe(III) on the oxidation state of uranium. In the first direct measurement of Pu oxidation state in a nuclear test melt glass, we obtain a result consistent with existing literature that proposes Pu is primarily present as Pu(IV) in post-detonation material. In addition, our measurements imply that highly mobile U(VI) may be produced in significant quantities when melt glass is quenched rapidly following a nuclear detonation, though these products may remain immobile in the vitrified matrices. The observed differences in chemical state among the three samples show that redox conditions can vary dramatically across different nuclear test conditions. The local soil composition, associated device materials, and the rate of quenching are all likely to affect the final redox state of the glass. The resulting variations in glass chemistry are significant for understanding and interpreting debris chemistry and the later environmental mobility of dispersed material.« less

Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pacold, J. I.; Lukens, W. W.; Booth, C. H.

We report that nuclear weapons testing generates large volumes of glassy materials that influence the transport of dispersed actinides in the environment and may carry information on the composition of the detonated device. We determine the oxidation state of U and Fe (which is known to buffer the oxidation state of actinide elements and to affect the redox state of groundwater) in samples of melt glass collected from three U.S. nuclear weapons tests. For selected samples, we also determine the coordination geometry of U and Fe, and we report the oxidation state of Pu from one melt glass sample. Wemore » find significant variations among the melt glass samples and, in particular, find a clear deviation in one sample from the expected buffering effect of Fe(II)/Fe(III) on the oxidation state of uranium. In the first direct measurement of Pu oxidation state in a nuclear test melt glass, we obtain a result consistent with existing literature that proposes Pu is primarily present as Pu(IV) in post-detonation material. In addition, our measurements imply that highly mobile U(VI) may be produced in significant quantities when melt glass is quenched rapidly following a nuclear detonation, though these products may remain immobile in the vitrified matrices. The observed differences in chemical state among the three samples show that redox conditions can vary dramatically across different nuclear test conditions. The local soil composition, associated device materials, and the rate of quenching are all likely to affect the final redox state of the glass. Lastly, the resulting variations in glass chemistry are significant for understanding and interpreting debris chemistry and the later environmental mobility of dispersed material.« less

Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing

DOE PAGES

Pacold, J. I.; Lukens, W. W.; Booth, C. H.; ...

2016-05-18

We report that nuclear weapons testing generates large volumes of glassy materials that influence the transport of dispersed actinides in the environment and may carry information on the composition of the detonated device. We determine the oxidation state of U and Fe (which is known to buffer the oxidation state of actinide elements and to affect the redox state of groundwater) in samples of melt glass collected from three U.S. nuclear weapons tests. For selected samples, we also determine the coordination geometry of U and Fe, and we report the oxidation state of Pu from one melt glass sample. Wemore » find significant variations among the melt glass samples and, in particular, find a clear deviation in one sample from the expected buffering effect of Fe(II)/Fe(III) on the oxidation state of uranium. In the first direct measurement of Pu oxidation state in a nuclear test melt glass, we obtain a result consistent with existing literature that proposes Pu is primarily present as Pu(IV) in post-detonation material. In addition, our measurements imply that highly mobile U(VI) may be produced in significant quantities when melt glass is quenched rapidly following a nuclear detonation, though these products may remain immobile in the vitrified matrices. The observed differences in chemical state among the three samples show that redox conditions can vary dramatically across different nuclear test conditions. The local soil composition, associated device materials, and the rate of quenching are all likely to affect the final redox state of the glass. Lastly, the resulting variations in glass chemistry are significant for understanding and interpreting debris chemistry and the later environmental mobility of dispersed material.« less

Chemical speciation of U, Fe, and Pu in melt glass from nuclear weapons testing

NASA Astrophysics Data System (ADS)

Pacold, J. I.; Lukens, W. W.; Booth, C. H.; Shuh, D. K.; Knight, K. B.; Eppich, G. R.; Holliday, K. S.

2016-05-01

Nuclear weapons testing generates large volumes of glassy materials that influence the transport of dispersed actinides in the environment and may carry information on the composition of the detonated device. We determine the oxidation state of U and Fe (which is known to buffer the oxidation state of actinide elements and to affect the redox state of groundwater) in samples of melt glass collected from three U.S. nuclear weapons tests. For selected samples, we also determine the coordination geometry of U and Fe, and we report the oxidation state of Pu from one melt glass sample. We find significant variations among the melt glass samples and, in particular, find a clear deviation in one sample from the expected buffering effect of Fe(II)/Fe(III) on the oxidation state of uranium. In the first direct measurement of Pu oxidation state in a nuclear test melt glass, we obtain a result consistent with existing literature that proposes Pu is primarily present as Pu(IV) in post-detonation material. In addition, our measurements imply that highly mobile U(VI) may be produced in significant quantities when melt glass is quenched rapidly following a nuclear detonation, though these products may remain immobile in the vitrified matrices. The observed differences in chemical state among the three samples show that redox conditions can vary dramatically across different nuclear test conditions. The local soil composition, associated device materials, and the rate of quenching are all likely to affect the final redox state of the glass. The resulting variations in glass chemistry are significant for understanding and interpreting debris chemistry and the later environmental mobility of dispersed material.

Evaluations of Energy Spectra of Neutrons Emitted Promptly in Neutron-induced Fission of 235U and 239Pu

NASA Astrophysics Data System (ADS)

Neudecker, D.; Talou, P.; Kawano, T.; Kahler, A. C.; White, M. C.; Taddeucci, T. N.; Haight, R. C.; Kiedrowski, B.; O'Donnell, J. M.; Gomez, J. A.; Kelly, K. J.; Devlin, M.; Rising, M. E.

2018-02-01

The energy spectra of neutrons emitted promptly in the neutron-induced fission reactions of 235U and 239Pu were re-evaluated for ENDF/B-VIII.0. These evaluations are based on a careful modeling of all relevant physics processes, an extensive analysis of experimental data and a detailed quantification of pertinent uncertainties. Energy spectra of neutrons emitted in up to fourth chance fission are considered and both compound and pre-equilibrium processes are included. Also, important nuclear model parameters, such as the average total kinetic energy of the fission fragments and the multiple chance fission probabilities, and their uncertainties are estimated based on experimental knowledge, model information and evaluated data. In addition to experimental information already available for ENDF/B-VII.1, these new evaluations make use of recently published experimental data either of high precision or spanning a broad incident energy range, information on legacy measurements explaining discrepancies and recently measured data of the average total kinetic energy as a function of incident neutron energy. The resulting evaluated data and covariances agree well with the experimental database used for the evaluation. However, the evaluated spectra are softer than the 235U and 239Pu ENDF/B-VII.1, JENDL-4.0 and JEFF-3.2 evaluations for incident neutron energies Einc ≤ 1.5 MeV and Einc ≤ 5 MeV, respectively. For Einc > 5 MeV, the evaluated spectra show structures due to the improved modeling which are not present in ENDF/B-VII.1 and JEFF-3.2 but can be observed in JENDL-4.0 evaluations. Part of these new evaluations were adopted for ENDF/B-VIII.0, while the ENDF/B-VII.1 239Pu PFNS was retained for Einc ≤ 5 MeV awaiting more conclusive experimental evidence.

Uncertainty Measurement for Trace Element Analysis of Uranium and Plutonium Samples by Inductively Coupled Plasma-Atomic Emission Spectrometry (ICP-AES) and Inductively Coupled Plasma-Mass Spectrometry (ICP-MS)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gallimore, David L.

2012-06-13

The measurement uncertainty estimatino associated with trace element analysis of impurities in U and Pu was evaluated using the Guide to the Expression of Uncertainty Measurement (GUM). I this evalution the uncertainty sources were identified and standard uncertainties for the components were categorized as either Type A or B. The combined standard uncertainty was calculated and a coverage factor k = 2 was applied to obtain the expanded uncertainty, U. The ICP-AES and ICP-MS methods used were deveoped for the multi-element analysis of U and Pu samples. A typical analytical run consists of standards, process blanks, samples, matrix spiked samples,more » post digestion spiked samples and independent calibration verification standards. The uncertainty estimation was performed on U and Pu samples that have been analyzed previously as part of the U and Pu Sample Exchange Programs. Control chart results and data from the U and Pu metal exchange programs were combined with the GUM into a concentration dependent estimate of the expanded uncertainty. Comparison of trace element uncertainties obtained using this model was compared to those obtained for trace element results as part of the Exchange programs. This process was completed for all trace elements that were determined to be above the detection limit for the U and Pu samples.« less

Characterization of Actinides Complexed to Nuclear Fuel Constituents Using ESI-MS

DOE PAGES

McDonald, Luther W.; Campbell, James A.; Vercouter, Thomas; ...

2016-03-01

Electrospray ionization-mass spectrometry (ESI-MS) was tested for its use in monitoring spent nuclear fuel (SNF) constituents including U, Pu, dibutyl phosphate (DBP), and tributyl phosphate (TBP). Both positive and negative ion modes were used to evaluate the speciation of U and Pu with TBP and DBP. Furthermore, apparent stability constants were determined for U complexed to TBP and DBP. In positive ion mode, TBP produced a strong signal with and without complexation to U or Pu, but, in negative ion mode, no TBP, U-TBP, or Pu-TBP complexes were observed. Apparent stability constants were determined for [UO 2(NO 3) 2(TBP) 2],more » [UO 2(NO 3) 2(H 2O)(TBP) 2], and [UO 2(NO 3) 2(TBP) 3]. In contrast DBP, U-DBP, and Pu-DBP complexes were observed in both positive and negative ion modes. Apparent stability constants were determined for the species [UO 2(DBP)], [UO 2(DBP) 3], and [UO 2(DBP) 4]. Analyzing mixtures of U or Pu with TBP and DBP yielded the formation of ternary complexes whose stoichiometry was directly related to the ratio of TBP to DBP. The ESI-MS protocols used in this study will further demonstrate the utility of ESI-MS and its applicability to process control monitoring in SNF reprocessing facilities.« less

(236)U and (239,)(240)Pu ratios from soils around an Australian nuclear weapons test site.

PubMed

Tims, S G; Froehlich, M B; Fifield, L K; Wallner, A; De Cesare, M

2016-01-01

The isotopes (236)U, (239)Pu and (240)Pu are present in surface soils as a result of global fallout from nuclear weapons tests carried out in the 1950's and 1960's. These isotopes potentially constitute artificial tracers of recent soil erosion and sediment movement. Only Accelerator Mass Spectrometry has the requisite sensitivity to measure all three isotopes at these environmental levels. Coupled with its relatively high throughput capabilities, this makes it feasible to conduct studies of erosion across the geographical extent of the Australian continent. In the Australian context, however, global fallout is not the only source of these isotopes. As part of its weapons development program the United Kingdom carried out a series of atmospheric and surface nuclear weapons tests at Maralinga, South Australia in 1956 and 1957. The tests have made a significant contribution to the Pu isotopic abundances present in the region around Maralinga and out to distances ∼1000 km, and impact on the assessment techniques used in the soil and sediment tracer studies. Quantification of the relative fallout contribution derived from detonations at Maralinga is complicated owing to significant contamination around the test site from numerous nuclear weapons safety trials that were also carried out around the site. We show that (236)U can provide new information on the component of the fallout that is derived from the local nuclear weapons tests, and highlight the potential of (236)U as a new fallout tracer. Crown Copyright © 2015. Published by Elsevier Ltd. All rights reserved.

Pu'u 'Ō'ō-Kūpaianaha eruption of Kilauea, November 1991-February 1994; field data and flow maps

USGS Publications Warehouse

Heliker, C. Christina; Mangan, Margaret T.; Mattox, Tari N.; Kauahikaua, James P.

1998-01-01

The Pu'u 'Ō'ō-Kūpaianaha eruption on the east rift zone of Kīlauea, which began in January 1983, is the longest-lived rift zone eruption of the last two centuries. By 1994, a broad field of lava, nearly 1 km3 in volume and 12 km wide at the coast, had buried 87 km2 of the volcano's south flank. The initial six months of fissure eruptions (episodes 1-3) were followed by three years of episodic lava fountaining from the Pu'u 'Ō'ō vent (episodes 4–47). In July 1986, after two days of fissure eruptions up- and downrift from Pu'u 'Ō'ō (episodes 48a and 48b), the eruption shifted to a new vent, Kūpaianaha, 3.5 km downrift. For the next five-and-a-half years (episode 48), Kūpaianaha was the site of nearly continuous low-level effusion. The 49th episode occurred in November 1991, when several fissures opened between Pu'u 'Ō'ō and Kūpaianaha (see Mangan and others, 1995, Bulletin of Volcanology, v. 57, p. 127-135). This three-week-long outburst was the result of the waning output of the Kūpaianaha vent, which finally died in February 1992 (see Kauahikaua and others, 1996, Bulletin of Volcanology, v. 57, p. 641-648). The third epoch of the eruption began ten days later, when vents opened on the uprift slope of the Pu'u 'Ō'ō cone. Several flank vents erupted over the next two years (episodes 50-53). In the first year, from February 1992 through February 1993, the low-level effusion was interrupted by 21 brief pauses. These ended with the beginning of episode 53 in February 1993, and for the next year, lava effusion was continuous. Episode 53 was ongoing at the end of the interval covered by this report. During the years that Kūpaianaha was active, the Pu'u 'Ō'ō conduit gradually evolved into a crater 300 m in diameter as the conduit walls collapsed. Beginning in 1987, an active lava pond was intermittently visible in the bottom of the crater; from 1990 on, the pond was almost continuously present. The Pu'u 'Ō‘ō pond drained at the beginning of episode 49 in November 1991, and the crater floor collapsed. Lava was visible in the crater by early December, and pond overflows resurfaced the crater floor, raising it to its former level of 35 m below the rim by the end of January 1992. This report includes flow-field maps and a table giving a) start and stop times of the eruptive episodes and of pauses in the eruption, b) Pu'u 'Ō'ō lava pond and crater-floor elevations, and c) elevations of the episode 50-53 vents and of the floors of the collapse pits that subsequently formed over these vents. A chronology of this interval of the eruption and an interpretation of the data included in this report can be found in Heliker and others (1998, Bulletin of Volcanology, v. 59, p. 381-393).

The fission cross sections of /sup 230/Th, /sup 232/Th, /sup 233/U, /sup 234/U, /sup 236/U, /sup 238/U, /sup 237/Np, /sup 239/Pu and /sup 242/Pu relative /sup 235/U at 14. 74 MeV neutron energy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meadows, J.W.

1986-12-01

The measurement of the fission cross section ratios of nine isotopes relative to /sup 235/U at an average neutron energy of 14.74 MeV is described with particular attention to the determination of corrections and to sources of error. The results are compared to ENDF/B-V and to other measurements of the past decade. The ratio of the neutron induced fission cross section for these isotopes to the fission cross section for /sup 235/U are: /sup 230/Th - 0.290 +- 1.9%; /sup 232/Th - 0.191 +- 1.9%; /sup 233/U - 1.132 +- 0.7%; /sup 234/U - 0.998 +- 1.0%; /sup 236/U -more » 0.791 +- 1.1%; /sup 238/U - 0.587 +- 1.1%; /sup 237/Np - 1.060 +- 1.4%; /sup 239/Pu - 1.152 +- 1.1%; /sup 242/Pu - 0.967 +- 1.0%. 40 refs., 11 tabs., 9 figs.« less

Controlling Pu behavior on Titania: Implications for LEU Fission-Based Mo-99 Production

DOE Office of Scientific and Technical Information (OSTI.GOV)

Youker, Amanda J.; Brown, M. Alex; Heltemes, Thad A.

Molybdenum-99 is the parent isotope of the most widely used isotope, technetium-99m, in all diagnostic nuclear medicine procedures. Due to proliferation concerns associated with the use of highly enriched uranium (HEU), the preferred method of fission-based Mo-99 production uses low enriched uranium (LEU) targets. Using LEU versus HEU for Mo-99 production produces similar to 30 times more Pu-239, due to neutron capture on U-238 to produce Np-239, which ultimately decays to Pu-239 (t(1/2) = 24,110 yr). Argonne National Laboratory is supporting a potential US Mo-99 producer in their efforts to produce Mo-99 from an LEU solution. In order to mitigatemore » the generation of large volumes of greater-than-class-C (GTCC) low level waste (Pu-239 concentrations greater than 1 nCi/g), we have focused our efforts on the separation chemistry of Pu and Mo with a titania sorbent in sulfate media. Results from batch and column experiments show that temperature and acid wash concentration can be used to control Pu behavior on titania.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

This paper was focused on core design, neutronics evaluation and fuel cycle analysis for Thorium-Uranium Breeding Recycle in current PWRs, without any major change to the fuel lattice and the core internals, but substituting the UOX pellet with Thorium-based pellet. The fuel cycle analysis indicates that Thorium-Uranium Breeding Recycle is technically feasible in current PWRs. A 4-loop, 193-assembly PWR core utilizing 17 x 17 fuel assemblies (FAs) was taken as the model core. Two mixed cores were investigated respectively loaded with mixed reactor grade Plutonium-Thorium (PuThOX) FAs and mixed reactor grade {sup 233}U-Thorium (U{sub 3}ThOX) FAs on the basis ofmore » reference full Uranium oxide (UOX) equilibrium-cycle core. The UOX/PuThOX mixed core consists of 121 UOX FAs and 72 PuThOX FAs. The reactor grade {sup 233}U extracted from burnt PuThOX fuel was used to fabrication of U{sub 3}ThOX for starting Thorium-. Uranium breeding recycle. In UOX/U{sub 3}ThOX mixed core, the well designed U{sub 3}ThOX FAs with 1.94 w/o fissile uranium (mainly {sup 233}U) were located on the periphery of core as a blanket region. U{sub 3}ThOX FAs remained in-core for 6 cycles with the discharged burnup achieving 28 GWD/tHM. Compared with initially loading, the fissile material inventory in U{sub 3}ThOX fuel has increased by 7% via 1-year cooling after discharge. 157 UOX fuel assemblies were located in the inner of UOX/U{sub 3}ThOX mixed core refueling with 64 FAs at each cycle. The designed UOX/PuThOX and UOX/U{sub 3}ThOX mixed core satisfied related nuclear design criteria. The full core performance analyses have shown that mixed core with PuThOX loading has similar impacts as MOX on several neutronic characteristic parameters, such as reduced differential boron worth, higher critical boron concentration, more negative moderator temperature coefficient, reduced control rod worth, reduced shutdown margin, etc.; while mixed core with U{sub 3}ThOX loading on the periphery of core has no visible impacts on neutronic characteristics compared with reference full UOX core. The fuel cycle analysis has shown that {sup 233}U mono-recycling with U{sub 3}ThOX fuel could save 13% of natural uranium resource compared with UOX once through fuel cycle, slightly more than that of Plutonium single-recycling with MOX fuel. If {sup 233}U multi-recycling with U{sub 3}ThOX fuel is implemented, more natural uranium resource would be saved. (authors)« less

A DFT+U study of Pu immobilization in Gd2Zr2O7

NASA Astrophysics Data System (ADS)

Zhao, F. A.; Xiao, H. Y.; Jiang, M.; Liu, Z. J.; Zu, X. T.

2015-12-01

The solubility of Pu in Gd2Zr2O7 has been investigated by the density functional theory plus Hubbard U correction. It is found that the formation of PuGdZr2O7, Gd2PuZrO7 and Gd2Pu1.5Zr0.5O7 are exothermic, whereas Pu0.5Gd1.5Zr2O7, Pu1.5Gd0.5Zr2O7 and Gd2Pu0.5Zr1.5O7 are energetically less stable than their respective separated states. The calculations show that both the Gd and Zr lattice sites can be substituted by the Pu, which is consistent with the immobilization behavior of uranium in Gd2Zr2O7 observed experimentally. The site preference of Pu in Gd2Zr2O7 is found to be dependent on the chemical environment, i.e., Pu prefers to substitute for Gd-site under Gd-rich and O2-rich conditions and for Zr-site under Zr-rich and O2-rich conditions.

DETERMINATION OF REPORTABLE RADIONUCLIDES FOR DWPF SLUDGE BATCH 7B (MACROBATCH 9)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Crawford, C. L.; Diprete, D. P.

The Waste Acceptance Product Specifications (WAPS) 1.2 require that “The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115”. As part of the strategy to comply with WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production throughmore » the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP) and Waste Form Qualification Report (WQR). However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu- 242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the heel from Sludge Batch 7a (SB7a) and Sludge Batch 7b (SB7b) that was transferred to Tank 40 from Tank 51. The blend of sludge in Tank 40 is also referred to as Macrobatch 9 (MB9). This report develops the list of reportable radionuclides and associated activities as a function of time. The DWPF will use this list and the activities as one of the inputs for the development of the Production Records that relate to radionuclide inventory. This work was initiated through Technical Task Request (TTR) HLW-DWPF-TTR-2011-0004; Rev. 0 entitled Sludge Batch 7b Qualification Studies. Specifically, this report details results from performing Subtask II, Item 2 of the TTR and, in part, meets Deliverable 6 of the TTR. The work was performed following the Task Technical and Quality Assurance Plan (TTQAP), SRNL-RP-2011-00247, Rev. 0 and Analytical Study Plan (ASP), SRNL-RP-2011-00248, Rev. 0. In order to determine the reportable radionuclides for SB7b (MB9), a list of radioisotopes that may meet the criteria as specified by the Department of Energy’s (DOE) WAPS was developed. All radioactive U- 235 fission products and all radioactive activation products that could be in the SRS HLW were considered. In addition, all U and Pu isotopes identified in WAPS 1.6 were included in the list. This list was then evaluated and some isotopes were excluded from the projection calculations. Based on measurements and analytical detection limits, 27 radionuclides have been identified as reportable for DWPF SB7b as specified by WAPS 1.2. The WCP and WQR require that all of the radionuclides present in the Design Basis glass be considered as the initial set of reportable radionuclides. For SB7b, all of the radionuclides in the Design Basis glass are reportable except for three radionuclides: Pd-107, Cs-135, and Th-230. At no time during the 1100- year period between 2015 and 3115 did any of these three radionuclides contribute to more than 0.01% of the radioactivity on a Curie basis. Two additional uranium isotopes (U-235 and -236) must be added to the list of reportable radionuclides in order to meet WAPS 1.6. All of the Pu isotopes (Pu-238, -239, -240, -241, and -242) and other U isotopes (U-233, -234, and -238) identified in WAPS 1.6 were already determined to be reportable according to WAPS 1.2 This brings the total number of reportable radionuclides for SB7b to 29. The radionuclide measurements made for SB7b are similar to those performed in the previous SB7a MB8 work. Some method development/refinement occurred during the conduct of these measurements, leading to lower detection limits and more accurate measurement of some isotopes than was previously possible. Improvement in the analytical measurements will likely continue, and this in turn should lead to improved detection limit values for some radionuclides and actual measurements for still others.« less

Determination Of Reportable Radionuclides For DWPF Sludge Batch 7B (Macrobatch 9)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Crawford, C. L.; DiPrete, D. P.

The Waste Acceptance Product Specifications (WAPS) 1.2 require that “The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115”. As part of the strategy to comply with WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production throughmore » the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP) and Waste Form Qualification Report (WQR). However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu-242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the heel from Sludge Batch 7a (SB7a) and Sludge Batch 7b (SB7b) that was transferred to Tank 40 from Tank 51. The blend of sludge in Tank 40 is also referred to as Macrobatch 9 (MB9). This report develops the list of reportable radionuclides and associated activities as a function of time. The DWPF will use this list and the activities as one of the inputs for the development of the Production Records that relate to radionuclide inventory. This work was initiated through Technical Task Request (TTR) HLW-DWPF-TTR-2011-0004; Rev. 0 entitled Sludge Batch 7b Qualification Studies. Specifically, this report details results from performing Subtask II, Item 2 of the TTR and, in part, meets Deliverable 6 of the TTR. The work was performed following the Task Technical and Quality Assurance Plan (TTQAP), SRNL-RP-2011-00247, Rev. 0 and Analytical Study Plan (ASP), SRNL-RP-2011-00248, Rev. 0. In order to determine the reportable radionuclides for SB7b (MB9), a list of radioisotopes that may meet the criteria as specified by the Department of Energy’s (DOE) WAPS was developed. All radioactive U-235 fission products and all radioactive activation products that could be in the SRS HLW were considered. In addition, all U and Pu isotopes identified in WAPS 1.6 were included in the list. This list was then evaluated and some isotopes were excluded from the projection calculations. Based on measurements and analytical detection limits, 27 radionuclides have been identified as reportable for DWPF SB7b as specified by WAPS 1.2. The WCP and WQR require that all of the radionuclides present in the Design Basis glass be considered as the initial set of reportable radionuclides. For SB7b, all of the radionuclides in the Design Basis glass are reportable except for three radionuclides: Pd-107, Cs-135, and Th-230. At no time during the 1100-year period between 2015 and 3115 did any of these three radionuclides contribute to more than 0.01% of the radioactivity on a Curie basis. Two additional uranium isotopes (U-235 and -236) must be added to the list of reportable radionuclides in order to meet WAPS 1.6. All of the Pu isotopes (Pu-238, -239, -240, -241, and -242) and other U isotopes (U-233, -234, and -238) identified in WAPS 1.6 were already determined to be reportable according to WAPS 1.2 This brings the total number of reportable radionuclides for SB7b to 29. The radionuclide measurements made for SB7b are similar to those performed in the previous SB7a MB8 work. Some method development/refinement occurred during the conduct of these measurements, leading to lower detection limits and more accurate measurement of some isotopes than was previously possible. Improvement in the analytical measurements will likely continue, and this in turn should lead to improved detection limit values for some radionuclides and actual measurements for still others.« less

Analytical Capability of Plasma Spectrometry Team

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gallimore, David L.

2012-07-19

Samples analyzed were: (1) Pu and U metal; (2) Pu oxide for nuclear fuel; (3) {sup 238}Pu oxide for heat source; and (4) Nuclear forensic samples - filters, swipes. Sample preparations that we did were: metal dissolution, marple filter dissolution, Pu oxide closed vessel acid digestion, and column separation to remove Pu.

Non-destructive Assay Measurements Using the RPI Lead Slowing Down Spectrometer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Becker, Bjorn; Weltz, Adam; Kulisek, Jonathan A.

2013-10-01

The use of a Lead Slowing-Down Spectrometer (LSDS) is consid- ered as a possible option for non-destructive assay of fissile material of used nuclear fuel. The primary objective is to quantify the 239Pu and 235U fissile content via a direct measurement, distinguishing them through their characteristic fission spectra in the LSDS. In this pa- per, we present several assay measurements performed at the Rensse- laer Polytechnic Institute (RPI) to demonstrate the feasibility of such a method and to provide benchmark experiments for Monte Carlo cal- culations of the assay system. A fresh UOX fuel rod from the RPI Criticality Researchmore » Facility, a 239PuBe source and several highly en- riched 235U discs were assayed in the LSDS. The characteristic fission spectra were measured with 238U and 232Th threshold fission cham- bers, which are only sensitive to fission neutron with energy above the threshold. Despite the constant neutron and gamma background from the PuBe source and the intense interrogation neutron flux, the LSDS system was able to measure the characteristic 235U and 239Pu responses. All measurements were compared to Monte Carlo simula- tions. It was shown that the available simulation tools and models are well suited to simulate the assay, and that it is possible to calculate the absolute count rate in all investigated cases.« less

REDUCTION OF PLUTONIUM VALUES IN AN ACIDIC AQUEOUS SOLUTION WITH FORMALDEHYDE

DOEpatents

Olson, C.M.

1959-06-01

A method is given for reducing Pu to the tetravalent state and lowering the high acidity of dissolver solutions containing U and Pu. Formaldehyde is added to the HNO/sub 3/ solution of U and Pu to effect a formaldehyde to HNO/sub 3/ molar ratio of 0.375:1 to 1.5:1. The Pu can then be removed from the solution by carrier precipitation using BiPO/sub 4/ or by ion exchange. (T.R.H.)

Analysis and application of heavy isotopes in the environment

NASA Astrophysics Data System (ADS)

Steier, Peter; Dellinger, Franz; Forstner, Oliver; Golser, Robin; Knie, Klaus; Kutschera, Walter; Priller, Alfred; Quinto, Francesca; Srncik, Michaela; Terrasi, Filippo; Vockenhuber, Christof; Wallner, Anton; Wallner, Gabriele; Wild, Eva Maria

2010-04-01

A growing number of AMS laboratories are pursuing applications of actinides. We discuss the basic requirements of the AMS technique of heavy (i.e., above ˜150 amu) isotopes, present the setup at the Vienna Environmental Research Accelerator (VERA) which is especially well suited for the isotope 236U, and give a comparison with other AMS facilities. Special emphasis will be put on elaborating the effective detection limits for environmental samples with respect to other mass spectrometric methods. At VERA, we have carried out measurements for radiation protection and environmental monitoring ( 236U, 239,240,241,242,244Pu), astrophysics ( 182Hf, 236U, 244Pu, 247Cm), nuclear physics, and a search for long-lived super-heavy elements ( Z > 100). We are pursuing the environmental distribution of 236U, as a basis for geological applications of natural 236U.

Exploratory study of fission product yields of neutron-induced fission of 235U , 238U , and 239Pu at 8.9 MeV

NASA Astrophysics Data System (ADS)

Bhatia, C.; Fallin, B. F.; Gooden, M. E.; Howell, C. R.; Kelley, J. H.; Tornow, W.; Arnold, C. W.; Bond, E.; Bredeweg, T. A.; Fowler, M. M.; Moody, W.; Rundberg, R. S.; Rusev, G. Y.; Vieira, D. J.; Wilhelmy, J. B.; Becker, J. A.; Macri, R.; Ryan, C.; Sheets, S. A.; Stoyer, M. A.; Tonchev, A. P.

2015-06-01

Using dual-fission chambers each loaded with a thick (200 -400 -mg /c m2) actinide target of 235 ,238U or 239Pu and two thin (˜10 -100 -μ g /c m2) reference foils of the same actinide, the cumulative yields of fission products ranging from 92Sr to 147Nd have been measured at En= 8.9 MeV . The 2H(d ,n ) 3He reaction provided the quasimonoenergetic neutron beam. The experimental setup and methods used to determine the fission product yield (FPY) are described, and results for typically eight high-yield fission products are presented. Our FPYs for 235U(n ,f ) , 238U(n ,f ) , and 239Pu(n ,f ) at 8.9 MeV are compared with the existing data below 8 MeV from Glendenin et al. [Phys. Rev. C 24, 2600 (1981), 10.1103/PhysRevC.24.2600], Nagy et al. [Phys. Rev. C 17, 163 (1978), 10.1103/PhysRevC.17.163], Gindler et al. [Phys. Rev. C 27, 2058 (1983), 10.1103/PhysRevC.27.2058], and those of Mac Innes et al. [Nucl. Data Sheets 112, 3135 (2011), 10.1016/j.nds.2011.11.009] and Laurec et al. [Nucl. Data Sheets 111, 2965 (2010), 10.1016/j.nds.2010.11.004] at 14.5 and 14.7 MeV, respectively. This comparison indicates a negative slope for the energy dependence of most fission product yields obtained from 235U and 239Pu , whereas for 238U the slope issue remains unsettled.

Mass Yields and Average Total Kinetic Energy Release in Fission for 235U, 238U, and 239Pu

NASA Astrophysics Data System (ADS)

Duke, Dana

2015-10-01

Mass yield distributions and average total kinetic energy (TKE) in neutron induced fission of 235U, 238U, and 239Pu targets were measured with a gridded ionization chamber. Despite decades of fission research, our understanding of how fragment mass yields and TKE depend on incident neutron energy is limited, especially at higher energies (above 5-10 MeV). Improved accuracy in these quantities is important for nuclear technology as it enhances our simulation capabilities and increases the confidence in diagnostic tools. The data can also guide and validate theoretical fission models where the correlation between the fragment mass and TKE is of particular value for constraining models. The Los Alamos Neutron Science Center - Weapons Neutron Research (LANSCE - WNR) provides a neutron beam with energies from thermal to hundreds of MeV, well-suited for filling in the gaps in existing data and exploring fission behavior in the fast neutron region. The results of the studies on target nuclei 235U, 238U, and 239Pu will be presented with a focus on exploring data trends as a function of neutron energy from thermal through 30 MeV. Results indicate clear evidence of structure due to multi-chance fission in the TKE . LA-UR-15-24761.

Method for selectively reducing plutonium values by a photochemical process

DOEpatents

Friedman, Horace A.; Toth, Louis M.; Bell, Jimmy T.

1978-01-01

The rate of reduction of Pu(IV) to Pu(III) in nitric acid solution containing a reducing agent is enhanced by exposing the solution to 200-500 nm electromagnetic radiation. Pu values are recovered from an organic extractant solution containing Pu(IV) values and U(VI) values by the method of contacting the extractant solution with an aqueous nitric acid solution in the presence of a reducing agent and exposing the aqueous solution to electromagnetic radiation having a wavelength of 200-500 nm. Under these conditions, Pu values preferentially distribute to the aqueous phase and U values preferentially distribute to the organic phase.

Deviation between the chemistry of Ce(IV) and Pu(IV) and routes to ordered and disordered heterobimetallic 4f/5f and 5f/5f phosphonates.

PubMed

Diwu, Juan; Wang, Shuao; Good, Justin J; DiStefano, Victoria H; Albrecht-Schmitt, Thomas E

2011-06-06

The heterobimetallic actinide compound UO(2)Ce(H(2)O)[C(6)H(4)(PO(3)H)(2)](2)·H(2)O was prepared via the hydrothermal reaction of U(VI) and Ce(IV) in the presence of 1,2-phenylenediphosphonic acid. We demonstrate that this is a kinetic product that is not stable with respect to decomposition to the monometallic compounds. Similar reactions have been explored with U(VI) and Ce(III), resulting in the oxidation of Ce(III) to Ce(IV) and the formation of the Ce(IV) phosphonate, Ce[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O, UO(2)Ce(H(2)O)[C(6)H(4)(PO(3)H)(2)](2)·H(2)O, and UO(2)[C(6)H(4)(PO(3)H)(2)](H(2)O)·H(2)O. In comparison, the reaction of U(VI) with Np(VI) only yields Np[C(6)H(4)(PO(3)H)(2)](2)·2H(2)O and aqueous U(VI), whereas the reaction of U(VI) with Pu(VI) yields the disordered U(VI)/Pu(VI) compound, (U(0.9)Pu(0.1))O(2)[C(6)H(4)(PO(3)H)(2)](H(2)O)·H(2)O, and the Pu(IV) phosphonate, Pu[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O. The reactions of Ce(IV) with Np(VI) yield disordered heterobimetallic phosphonates with both M[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O (M = Ce, Np) and M[C(6)H(4)(PO(3)H)(2)](2)·2H(2)O (M = Ce, Np) structures, as well as the Ce(IV) phosphonate Ce[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O. Ce(IV) reacts with Pu(IV) to yield the Pu(VI) compound, PuO(2)[C(6)H(4)(PO(3)H)(2)](H(2)O)·3H(2)O, and a disordered heterobimetallic Pu(IV)/Ce(IV) compound with the M[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O (M = Ce, Pu) structure. Mixtures of Np(VI) and Pu(VI) yield disordered heterobimetallic Np(IV)/Pu(IV) phosphonates with both the An[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O (M = Np, Pu) and An[C(6)H(4)(PO(3)H)(2)](2)·2H(2)O (M = Np, Pu) formulas. © 2011 American Chemical Society

Chemical bonds and vibrational properties of ordered (U, Np, Pu) mixed oxides

NASA Astrophysics Data System (ADS)

Yang, Yu; Zhang, Ping

2013-01-01

We use density functional theory +U to investigate the chemical bonding characters and vibrational properties of the ordered (U, Np, Pu) mixed oxides (MOXs), UNpO4,NpPuO4, and UPuO4. It is found that the 5f electronic states of different actinide elements keep their localized characters in all three MOXs. The occupied 5f electronic states of different actinide elements do not overlap with each other and tend to distribute over the energy band gap of the other actinide element's 5f states. As a result, the three ordered MOXs all show smaller band gaps than those of the component dioxides, with values of 0.91, 1.47, and 0.19 eV for UNpO4,NpPuO4, and UPuO4, respectively. Through careful charge density analysis, we further show that the U-O and Pu-O bonds in MOXs show more ionic character than in UO2 and PuO2, while the Np-O bonds show more covalent character than in NpO2. The change in covalencies in the chemical bonds leads to vibrational frequencies of oxygen atoms that are different in MOXs.

Enhanced expression of the urokinase-type plasminogen activator gene and reduced colony formation in soft agar by ectopic expression of PU.1 in HT1080 human fibrosarcoma cells.

PubMed Central

Kondoh, N.; Yamada, T.; Kihara-Negishi, F.; Yamamoto, M.; Oikawa, T.

1998-01-01

To investigate the cell biological function of PU.1, a member of the Ets family of transcription factors, a vector capable of expressing the protein was transfected into HT1080 human fibrosarcoma cells. Exogenous expression of PU.1 in HT1080 cells reduced colony-forming efficiency but stimulated cell migration in soft agar, although it did not affect cell growth in adherent culture. Expression of the urokinase-type plasminogen activator (uPA) mRNA, which is known to be correlated with cell migration and invasion, was enhanced in PU.1 transfectants compared with mock transfectants. Run-on analysis demonstrated that uPA transcription was unaffected by PU.1, suggesting that this enhancement mainly occurs at a post-transcriptional level. On the other hand, treatment of HT1080 cells with the synthetic glucocorticoid dexamethasone (DEX; 10(-7) M) significantly reduced uPA gene expression at a transcriptional level. Furthermore, DEX inhibited cell migration in soft agar without affecting cell growth. These negative effects of DEX on uPA expression and cell migration were alleviated by the expression of PU.1 in HT1080 cells, whereas expression of the N-ras oncogene, which is responsible for maintenance of the transformed phenotypes in HT1080 cells, was unaffected by PU.1 expression or DEX treatment in the cells. Our results suggest that expression of PU.1 can stimulate uPA gene expression at the post-transcriptional level, which may subsequently lead to activation of cell motility and/or reduced cell-cell adhesion, but reduces anchorage-independent growth of HT1080 cells. Images Figure 1 Figure 2 Figure 3 Figure 4 PMID:9743289

The character of long-term eruptions: Inferences from episodes 50-53 of the Pu'u 'Ō'ō-Kūpaianaha eruption of Kīlauea volcano

USGS Publications Warehouse

Heliker, C.C.; Mangan, M.T.; Mattox, T.N.; Kauahikaua, J.P.; Helz, R.T.

1998-01-01

The Pu'u 'Ō'ō-Kūpaianaha eruption on the east rift zone of Kīlauea began in January 1983. The first 9 years of the eruption were divided between the Pu'u 'Ō'ō (1983–1986) and Kūpaianaha (1986–1992) vents, each characterized by regular, predictable patterns of activity that endured for years. In 1990 a series of pauses in the activity disturbed the equilibrium of the eruption, and in 1991, the output from Kūpaianaha steadily declined and a short-lived fissure eruption broke out between Kūpaianaha and Pu'u 'Ō'ō. In February 1992 the Kūpaianaha vent died, and, 10 days later, eruptive episode 50 began as a fissure opened on the uprift flank of the Pu'u 'Ō'ō cone. For the next year, the eruption was marked by instability as more vents opened on the flank of the cone and the activity was repeatedly interrupted by brief pauses in magma supply to the vents. Episodes 50–53 constructed a lava shield 60 m high and 1.3 km in diameter against the steep slope of the Pu'u 'Ō'ō cone. By 1993 the shield was pockmarked by collapse pits as vents and lava tubes downcut as much as 29 m through the thick deposit of scoria and spatter that veneered the cone. As the vents progressively lowered, the level of the Pu'u 'Ō'ō pond also dropped, demonstrating the hydraulic connection between the two. The downcutting helped to undermine the prominent Pu'u 'Ō'ō cone, which has diminished in size both by collapse, as a large pit crater formed over the conduit, and by burial of its flanks. Intervals of eruptive instability, such as that of 1991–1993, accelerate lateral expansion of the subaerial flow field both by producing widely spaced vents and by promoting surface flow activity as lava tubes collapse and become blocked during pauses.

Natural and artificial radionuclides in a marine core. First results of 236U in North Atlantic Ocean sediments.

PubMed

Villa-Alfageme, M; Chamizo, E; Santos-Arévalo, F J; López-Gutierrez, J M; Gómez-Martínez, I; Hurtado-Bermúdez, S

2018-06-01

There are very few data available of 236 U in marine sediment cores. In this study we present the results from the first oceanic depth profile of 236 U in a sediment core sampled in the North Atlantic Ocean, at the PAP site (4500 m depth, Porcupine Abyssal Plain (PAP) site, 49°0' N, 16°30' W). Additionally, the sediment core was radiologically characterized through the measurement of anthropogenic 137 Cs, 239 Pu, 240 Pu, 129 I and 14 C and natural 210 Pb, 40 K and 226 Ra. The measured 236 U concentrations decrease from about 90·10 6  at g -1 at the seafloor down to 0.5·10 6  at g -1 at 6 cm depth. They are several orders of magnitude lower than the reported values for soils from the Northern Hemisphere solely influenced by global fallout (i.e. from 2700·10 6 to 7500·10 6  at g -1 ). 236 U/ 238 U atom ratios measured are at least three orders of magnitude above the estimated level for the naturally occurring dissolved uranium. The obtained inventories are 1·10 12  at m -2 for 236 U, 80 Bq m -2 for 137 Cs, 45 Bq m -2 for 239+240 Pu and 2.6·10 12  at m -2 for 129 I. Atomic ratios for 236 U/ 239 Pu, 137 Cs/ 236 U and 129 I/ 236 U, obtained from the inventories are 0.036, 0.11 and 2.5 respectively. Concentration profiles show mobilization probably due to bioturbation from the abundant detritivore holothurian species living at the PAP site sea-floor. The range of 236 U, 137 Cs, 239+240 Pu and 129 I values, inventories and ratios of these anthropogenic radionuclides are more similar to the values due to fall-out than values from a contribution from the Nuclear Fuel Reprocessing Plants dispersed to the south-west of the North Atlantic Ocean. However, signs of an additional source are detected and might be associated to the nuclear wastes dumped on the Eastern North Atlantic Ocean. Copyright © 2017 Elsevier Ltd. All rights reserved.

Measurement of the 242Pu neutron capture cross section

NASA Astrophysics Data System (ADS)

Buckner, M. Q.; Wu, C. Y.; Henderson, R. A.; Bucher, B.; Bredeweg, T. A.; Baramsai, B.; Couture, A.; Jandel, M.; Mosby, S.; O'Donnell, J. M.; Ullmann, J. L.; Chyzh, A.; Dance Collaboration

2015-10-01

Precision (n,f) and (n, γ) cross sections are important for the network calculations of the radiochemical diagnostic chain for the U.S. DOE's Stockpile Stewardship Program. 242Pu(n, γ) cross section is relevant to the network calculations of Pu and Am. Additionally, new reactor concepts have catalyzed considerable interest in the measurement of improved cross sections for neutron-induced reactions on key actinides. To date, little or no experimental data has been reported on 242Pu(n, γ) for incident neutron energy below 50 keV. A new measurement of the 242Pu(n, γ) reaction was performed with the DANCE together with an improved PPAC for fission-fragment detection at LANSCE during FY14. The relative scale of the 242Pu(n, γ) cross section spans four orders of magnitude for incident neutron energies from thermal to ~ 30 keV. The absolute scale of the 242Pu(n, γ) cross section is set according to the measured 239Pu(n,f) resonance at 7.8 eV; the target was spiked with 239Pu for this measurement. The absolute 242Pu(n, γ) neutron capture cross section is ~ 30% higher than the cross section reported in ENDF for the 2.7 eV resonance. Latest results to be reported. Funded by U.S. DOE Contract No. DE-AC52-07NA27344 (LLNL) and DE-AC52-06NA25396 (LANL). U.S. DOE/NNSA Office of Defense Nuclear Nonproliferation Research and Development. Isotopes (ORNL).

New prompt fission gamma-ray spectral data from 239Pu(nth, f) in response to a high priority request from OECD Nuclear Energy Agency

NASA Astrophysics Data System (ADS)

Gatera, Angélique; Belgya, Tamás; Geerts, Wouter; Göök, Alf; Hambsch, Franz-Josef; Lebois, Matthieu; Maróti, Boglárka; Oberstedt, Stephan; Oberstedt, Andreas; Postelt, Frederik; Qi, Liqiang; Szentmiklósi, Laszló; Vidali, Marzio; Zeiser, Fabio

2017-09-01

Benchmark reactor calculations have revealed an underestimation of γ-heat following fission of up to 28%. To improve the modelling of new nuclear reactors, the OECD/NEA initiated a nuclear data High Priority Request List (HPRL) entry for the major isotopes (235U, 239Pu). In response to that HPRL entry, we executed a dedicated measurement program on prompt fission γ-rays employing state-of-the-art lanthanum bromide (LaBr3) detectors with superior timing and good energy resolution. Our new results from 252Cf(sf), 235U(nth,f) and 241Pu(nth,f) provide prompt fission γ-ray spectra characteristics : average number of photons per fission, average total energy per fission and mean photon energy; all within 2% of uncertainty. We present preliminary results on 239Pu(nth,f), recently measured at the Budapest Neutron Centre and supported by the CHANDA Trans-national Access Activity, as well as discussing our different published results in comparison to the historical data and what it says about the discrepancy observed in the benchmark calculations.

Covariance generation and uncertainty propagation for thermal and fast neutron induced fission yields

NASA Astrophysics Data System (ADS)

Terranova, Nicholas; Serot, Olivier; Archier, Pascal; De Saint Jean, Cyrille; Sumini, Marco

2017-09-01

Fission product yields (FY) are fundamental nuclear data for several applications, including decay heat, shielding, dosimetry, burn-up calculations. To be safe and sustainable, modern and future nuclear systems require accurate knowledge on reactor parameters, with reduced margins of uncertainty. Present nuclear data libraries for FY do not provide consistent and complete uncertainty information which are limited, in many cases, to only variances. In the present work we propose a methodology to evaluate covariance matrices for thermal and fast neutron induced fission yields. The semi-empirical models adopted to evaluate the JEFF-3.1.1 FY library have been used in the Generalized Least Square Method available in CONRAD (COde for Nuclear Reaction Analysis and Data assimilation) to generate covariance matrices for several fissioning systems such as the thermal fission of U235, Pu239 and Pu241 and the fast fission of U238, Pu239 and Pu240. The impact of such covariances on nuclear applications has been estimated using deterministic and Monte Carlo uncertainty propagation techniques. We studied the effects on decay heat and reactivity loss uncertainty estimation for simplified test case geometries, such as PWR and SFR pin-cells. The impact on existing nuclear reactors, such as the Jules Horowitz Reactor under construction at CEA-Cadarache, has also been considered.

Multirecycling of Plutonium from LMFBR Blanket in Standard PWRs Loaded with MOX Fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sonat Sen; Gilles Youinou

2013-02-01

It is now well-known that, from a physics standpoint, Pu, or even TRU (i.e. Pu+M.A.), originating from LEU fuel irradiated in PWRs can be multirecycled also in PWRs using MOX fuel. However, the degradation of the isotopic composition during irradiation necessitates using enriched U in conjunction with the MOX fuel either homogeneously or heterogeneously to maintain the Pu (or TRU) content at a level allowing safe operation of the reactor, i.e. below about 10%. The study is related to another possible utilization of the excess Pu produced in the blanket of a LMFBR, namely in a PWR(MOX). In this casemore » the more Pu is bred in the LMFBR, the more PWR(MOX) it can sustain. The important difference between the Pu coming from the blanket of a LMFBR and that coming from a PWR(LEU) is its isotopic composition. The first one contains about 95% of fissile isotopes whereas the second one contains only about 65% of fissile isotopes. As it will be shown later, this difference allows the PWR fed by Pu from the LMFBR blanket to operate with natural U instead of enriched U when it is fed by Pu from PWR(LEU)« less

ANALYSIS OF 2H-EVAPORATOR SCALE WALL [HTF-13-82] AND POT BOTTOM [HTF-13-77] SAMPLES

DOE Office of Scientific and Technical Information (OSTI.GOV)

Oji, L.

2013-06-21

Savannah River Remediation (SRR) is planning to remove a buildup of sodium aluminosilicate scale from the 2H-evaporator pot by loading and soaking the pot with heated 1.5 M nitric acid solution. Sampling and analysis of the scale material has been performed so that uranium and plutonium isotopic analysis can be input into a Nuclear Criticality Safety Assessment (NCSA) for scale removal by chemical cleaning. Historically, since the operation of the Defense Waste Processing Facility (DWPF), silicon in the DWPF recycle stream combines with aluminum in the typical tank farm supernate to form sodium aluminosilicate scale mineral deposits in the 2Hevaporatormore » pot and gravity drain line. The 2H-evaporator scale samples analyzed by Savannah River National Laboratory (SRNL) came from the bottom cone sections of the 2H-evaporator pot [Sample HTF-13-77] and the wall 2H-evaporator [sample HTF-13-82]. X-ray diffraction analysis (XRD) confirmed that both the 2H-evaporator pot scale and the wall samples consist of nitrated cancrinite (a crystalline sodium aluminosilicate solid) and clarkeite (a uranium oxy-hydroxide mineral). On “as received” basis, the bottom pot section scale sample contained an average of 2.59E+00 ± 1.40E-01 wt % total uranium with a U-235 enrichment of 6.12E-01 ± 1.48E-02 %, while the wall sample contained an average of 4.03E+00 ± 9.79E-01 wt % total uranium with a U-235 enrichment of 6.03E-01% ± 1.66E-02 wt %. The bottom pot section scale sample analyses results for Pu-238, Pu-239, and Pu-241 are 3.16E- 05 ± 5.40E-06 wt %, 3.28E-04 ± 1.45E-05 wt %, and <8.80E-07 wt %, respectively. The evaporator wall scale samples analysis values for Pu-238, Pu-239, and Pu-241 averages 3.74E-05 ± 6.01E-06 wt %, 4.38E-04 ± 5.08E-05 wt %, and <1.38E-06 wt %, respectively. The Pu-241 analyses results, as presented, are upper limit values. These results are provided so that SRR can calculate the equivalent uranium-235 concentrations for the NCSA. Results confirm that the uranium contained in the scale remains depleted with respect to natural uranium. SRNL did not calculate an equivalent U-235 enrichment, which takes into account other fissionable isotopes U-233, Pu-239 and Pu-241. The applicable method for calculation of equivalent U-235 will be determined in the NCSA.« less

Exploratory study of fission product yields of neutron-induced fission of U 235 ,   U 238 , and Pu 239 at 8.9 MeV

DOE PAGES

Bhatia, C.; Fallin, B. F.; Gooden, M. E.; ...

2015-06-05

Using dual-fission chambers each loaded with a thick (200–400–mg/cm 2) actinide target of 235,238U or 239Pu and two thin (~10–100–μg/cm 2) reference foils of the same actinide, the cumulative yields of fission products ranging from 92Sr to 147Nd have been measured at E n = 8.9MeV. The 2H(d,n) 3He reaction provided the quasimonoenergetic neutron beam. Here, the experimental setup and methods used to determine the fission product yield (FPY) are described, and results for typically eight high-yield fission products are presented.

Sintering of compacts of UN, (U,Pu)N, and PuN

DOEpatents

Tennery, V.J.; Godfrey, T.G.; Bomar, E.S.

1973-10-16

>A method is provided for preparing a densified compact of a metal nitride selected from the group consisting of UN, (U,Pu)N, and PuN which comprises heating a green compact of at least one selected nitride in the mononitride single-phase region, as displayed by a phase diagram of the mononitride of said compact, in a nitrogen atmosphere at a pressure of nitrogen less than 760 torr. At a given temperature, this process produces a singlephase structure and a maximal sintered density as measured by mercury displacement. (Official Gazette)

Characterization and preparation of p(U-MMA-An) interpenetrating polymer network damping and absorbing material.

PubMed

Liu, Jun; Li, Qingshan; Zhuo, Yuguo; Hong, Wei; Lv, Wenfeng; Xing, Guangzhong

2014-06-01

P(U-MMA-ANI) interpenetrating polymer network (IPN) damping and absorbing material is successfully synthesized by PANI particles served as an absorbing agent with the microemulsion polymerization and P(U-MMA) foam IPN network structure for substrate materials with foaming way. P(U-MMA-ANI) IPN is characterized by the compression mechanical performance testing, TG-DSC, and DSC. The results verify that the P(U-MMA) IPN foam damping material has a good compressive strength and compaction cycle property, and the optimum content of PMMA was 40% (mass) with which the SEM graphs do not present the phase separation on the macro level between PMMA and PU, while the phase separation was observed on the micro level. The DTG curve indicates that because of the formation of P(U-MMA) IPN, the decomposition temperature of PMMA and the carbamate in PU increases, while that of the polyol segment in PU has almost no change. P(U-MMA-ANI) IPN foam damping and absorbing material is obtained by PANI particles served as absorbing agent in the form of filler, and PMMA in the form of micro area in substrate material. When the content of PANI was up to 2.0% (mass), the dissipation factor of composites increased, and with the increasing of frequency the dissipation factor increased in a straight line.

Deformation Associated With the July 21 Fissure Eruption at Kilauea Volcano, Hawai`i

NASA Astrophysics Data System (ADS)

Poland, M.; Orr, T.; Miklius, A.

2007-12-01

Deformation measurements at the Pu`u `O`o cone on Kilauea volcano indicate that the vent is underlain by a shallow magma storage reservoir fed by magma transported from Kilauea's summit. The Pu`u `O`o reservoir was drained during the "Father's&pDay" intrusion of June 17-19, 2007, causing Pu`u `O`o's floor to collapse. Following the intrusion, the reservoir gradually refilled and lava reappeared on July 1-2. A lava lake grew in the crater during July 2-20, steadily raising the elevation of the crater floor. The crater interior and adjoining walls began to uplift on July 10, and 2 days later lava began to vent above the level of the lava lake along the margins of the crater. The number of crater margin vents and the magnitude of their activity increased until July 21, by which time crater uplift amounted to about 8 meters. Early that morning, the lava pond at Pu`u `O`o drained suddenly and an eruptive fissure opened on the east flank of the cone. The fissure propagated 2 km downrift, and within a few hours the eruption had localized on three fissure segments between 1 and 2 km east of Pu`u `O`o. Lava erupting from this series of vents formed a system of perched lava ponds feeding long `a`a flows. Deformation associated with the July 21 fissure was exceptionally well-documented by a borehole tiltmeter on the north flank of Pu`u `O`o and 7 continuous GPS stations within 2 km of the cone (the fissure propagated between two of these GPS stations). The time series of geodetic measurements suggests that deflation of Pu`u `O`o began at about 2250 HST (Hawaiian Standard Time - UTC minus 10 hours) on July 20, while a camera looking into Pu`u `O`o crater recorded draining of the lava lake starting at around 2355 HST. Deformation associated with opening of the fissure was apparent in the tilt and GPS records by 0012 HST, with the camera showing glow in the direction of the eruption site by 0039 HST on July 21. Localized deformation from InSAR suggests that the fissure has a shallow source, probably within 1 km of the surface; this interpretation is also supported by kinematic GPS results collected from points around Pu`u `O`o in July 2006 and July 2007.

Coordination chemistry of 2,2'-biphenylenedithiophosphinate and diphenyldithiophosphinate with U, Np, and Pu

DOE PAGES

Macor, Joseph A.; Brown, Jessie L.; Cross, Justin Neil; ...

2015-01-01

New members of the dithiophosphinic acid family of potential actinide extractants were prepared: heterocyclic 2,2'-biphenylenedithiophosphinic acids of stoichiometry HS 2P(R 2C 12H 6) (R = H or tBu). The time- and atom-efficient syntheses afforded multigram quantities of pure HS 2P(R 2C 12H 6) in reasonable yields (~60%). These compounds differed from other diaryldithiophosphinic acid extractants in that the two aryl groups were connected to one another at the ortho positions to form a 5-membered dibenzophosphole ring. These 2,2'-biphenylenedithiophosphinic acids were readily deprotonated to form S 2P(R 2C 12H 6) 1- anions, which were crystallized as salts with tetraphenylpnictonium cations (ZPhmore » 4 1+; Z = P or As). Coordination chemistry between [S 2P( tBu 2C 12H 6)] 1- and [S 2P(C 6H 5)2] 1- with U, Np, and Pu was comparatively investigated. The results showed that dithiophosphinate complexes of UIV and NpIV were redox stable relative to those of UIII, whereas reactions involving PuIV gave intractable material. For instance, reactions involving UIV and NpIV generated An[S 2P( tBu 2C 12H 6)] 4 and An[S 2P(C 6H 5) 2] 4 whereas reactions between PuIV and [S 2P(C 6H 5) 2] 1- generated a mixture of products from which we postulated a transient PuIII species based on UV-Vis spectroscopy. However, the trivalent Pu[S 2P(C 6H 5) 2] 3(NC 5H 5) 2 compound is stable and could be isolated from reactions between [S 2P(C 6H 5) 2] 1- and the trivalent PuI 3(NC 5H 5) 4 starting material. Attempts to synthesize analogous trivalent compounds with UIII provided the tetravalent U[S 2P(C 6H 5 )2] 4 oxidation product.« less

Enhancement of the volcanogenic "bromine explosion" via reactive nitrogen chemistry (Kīlauea volcano, Hawai'i)

NASA Astrophysics Data System (ADS)

Salerno, G. G.; Oppenheimer, C.; Tsanev, V. I.; Sutton, A. J.; Roberts, T. J.; Elias, T.

2010-04-01

Since the first detection of bromine monoxide in volcanic plumes attention has focused on the atmospheric synthesis and impact of volcanogenic reactive halogens. We report here new measurements of BrO in the volcanic plume emitted from Kīlauea volcano - the first time reactive halogens have been observed in emissions from a hotspot volcano. Observations were carried out by ground-based Differential Optical Absorption Spectroscopy in 2007 and 2008 at Pu'u'O'o crater, and at the 2008 magmatic vent that opened within Halema'uma'u crater. BrO was readily detected in the Halema'uma'u plume (average column amount of 3×1015 molec cm-2) and its abundance was strongly correlated with that of SO2. However, anticorrelation between NO2 and SO2 (and BrO) abundances in the same plume strongly suggest an active role of NOx in reactive halogen chemistry. The calculated SO2/BrO molar ratio of ~1600 is comparable to observations at other volcanoes, although the BrO mixing ratio is roughly double that observed elsewhere. While BrO was not observed in the Pu'u'O'o plume this was probably merely a result of the detection limit of our measurements and based on understanding of the Summit and East Rift magmatic system we expect reactive halogens to be formed also in the Pu'u'O'o emissions. If this is correct then based on the long term SO2 flux from Pu'u'O'o we calculate that Kīlauea emits ~480 Mg yr-1 of reactive bromine and may thus represent an important source to the tropical Pacific troposphere.

The crystal structure of ianthinite, [U 24+(UO 2) 4O 6(OH) 4(H 2O) 4](H 2O) 5: a possible phase for Pu 4+ incorporation during the oxidation of spent nuclear fuel

NASA Astrophysics Data System (ADS)

Burns, Peter C.; Finch, Robert J.; Hawthorne, Frank C.; Miller, Mark L.; Ewing, Rodney C.

1997-10-01

Ianthinite, [U 24+(UO 2) 4O 6(OH) 4(H 2O) 4](H 2O) 5, is the only known uranyl oxide hydrate mineral that contains U 4+, and it has been proposed that ianthinite may be an important Pu 4+-bearing phase during the oxidative dissolution of spent nuclear fuel. The crystal structure of ianthinite, orthorhombic, a = 0.7178(2), b = 1.1473(2), c = 3.039(1) nm, V = 2.5027 nm 3Z = 4, space group P2 1cn, has been solved by direct methods and refined by least-squares methods to an R index of 9.7% and a wR index of 12.6% using 888 unique observed [| F| ≥ 5 σ | F|] reflections. The structure contains both U 4+. The U 6+ cations are present as roughly linear (U 6+O 2) 2+ uranyl ion (Ur) that are in turn coordinated by five O 2- and OH - located at the equatorial positions of pentagonal bipyramids. The U 4+ cations are coordinated by O 2-, OH - and H 2O in a distorted octahedral arrangement. The Ur φ5and U 4+| 6 (φ: O 2-, OH -, H 2O) polyhedra l sharing edges to for two symmetrically distinct sheets at z ≈ 0.0 and z ≈ 0.25 that are parallel to (001). The sheets have the β-U 3O 8 sheet anion-topology. There are five symmetrically distinct H 2O groips located at z ≈ 0.125 between the sheets of U φn polyhedra, and the sheets of U φn polyhedra are linked together only by hydrogen bonding to the intersheet H 2O groups. The crystal-chemical requirements of U 4+ and Pu 4+ are very similar, suggesting that extensive Pu 4+ ↔ U 4+ substitution may occur within the sheets of U φn polyhedra in trh structure of ianthinine.

ADVANCEMENTS IN TIME-SPECTRA ANALYSIS METHODS FOR LEAD SLOWING-DOWN SPECTROSCOPY

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smith, Leon E.; Anderson, Kevin K.; Gesh, Christopher J.

2010-08-11

Direct measurement of Pu in spent nuclear fuel remains a key challenge for safeguarding nuclear fuel cycles of today and tomorrow. Lead slowing-down spectroscopy (LSDS) is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic mass with an uncertainty lower than the approximately 10 percent typical of today’s confirmatory assay methods. Pacific Northwest National Laboratory’s (PNNL) previous work to assess the viability of LSDS for the assay of pressurized water reactor (PWR) assemblies indicated that the method could provide direct assay of Pu-239 and U-235 (and possibly Pu-240 and Pu-241)more » with uncertainties less than a few percent, assuming suitably efficient instrumentation, an intense pulsed neutron source, and improvements in the time-spectra analysis methods used to extract isotopic information from a complex LSDS signal. This previous simulation-based evaluation used relatively simple PWR fuel assembly definitions (e.g. constant burnup across the assembly) and a constant initial enrichment and cooling time. The time-spectra analysis method was founded on a preliminary analytical model of self-shielding intended to correct for assay-signal nonlinearities introduced by attenuation of the interrogating neutron flux within the assembly.« less

Ultra-Sensitive Elemental Analysis Using Plasmas 4.Application of Inductively Coupled Plasma Mass Spectrometry to the Study of Environmental Radioactivity

NASA Astrophysics Data System (ADS)

Yoshida, Satoshi

Applications of inductively coupled plasma mass spectrometry (ICP-MS) to the determination of long-lived radionuclides in environmental samples were summarized. In order to predict the long-term behavior of the radionuclides, related stable elements were also determined. Compared with radioactivity measurements, the ICP-MS method has advantages in terms of its simple analytical procedures, prompt measurement time, and capability of determining the isotope ratio such as240Pu/239Pu, which can not be separated by radiation. Concentration of U and Th in Japanese surface soils were determined in order to determine the background level of the natural radionuclides. The 235U/238U ratio was successfully used to detect the release of enriched U from reconversion facilities to the environment and to understand the source term. The 240Pu/239Pu ratios in environmental samples varied widely depending on the Pu sources. Applications of ICP-MS to the measurement of I and Tc isotopes were also described. The ratio between radiocesium and stable Cs is useful for judging the equilibrium of deposited radiocesium in a forest ecosystem.

The coprecipitation of Pu and other radionuclides with CaCO[sub 3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meece, D.E.; Benninger, L.K.

1993-04-01

The record of fallout plutonium concentrations in annual bands of corals is strikingly similar to the record of atmospheric deposition of [sup 90]Sr. This similarity implies that corals may incorporate Pu from seawater with a constant partition coefficient (constant discrimination). To investigate physicochemical aspects of Pu incorporation, the following have been coprecipitated with CaCO[sub 3] (calcite and aragonite): oxidized and reduced Pu; americium, thorium, and uranium as analogs to Pu oxidation states (III, IV, VI), respectively; and [sup 210]Pb as a particle-reactive nuclide which may be incorporated by corals with constant discrimination. Americium, thorium, and lead adsorb onto both calcitemore » and aragonite, with more than 99% of the recovered activity found associated with the solids. Uranium exhibits a behavior consistent with lattice substitution. Partition coefficients for U in aragonite range from 1.8 to 9.8 and vary inversely with pH and/or rate of precipitation. The partition coefficient for U in calcite is less than 0.2 and may be as low as 0.046. Reduced Pu sorbs with 3 to 4% remaining in solution. Oxidized Pu may both sorb and coprecipitate. The coral record for Pb and U results primarily from biological, rather than physicochemical, effects; it is likely that the PU coral record also reflects biological discrimination. 50 refs., 4 figs., 5 tabs.« less

Rapid Method for Sodium Hydroxide Fusion of Asphalt ...

EPA Pesticide Factsheets

Technical Brief--Addendum to Selected Analytical Methods (SAM) 2012 Rapid method developed for analysis of Americium-241 (241Am), plutonium-238 (238Pu), plutonium-239 (239Pu), radium-226 (226Ra), strontium-90 (90Sr), uranium-234 (234U), uranium-235 (235U) and uranium-238 (238U) in asphalt roofing material samples

Neutronics Benchmarks for the Utilization of Mixed-Oxide Fuel: Joint U.S./ Russian Progress Report for Fiscal Year 1997, Volume 4, Part 8 - Neutron Poison Plates in Assemblies Containing Homogeneous Mixtures of Polystyrene-Moderated Plutonium and Uranium Oxides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yavuz, M.

1999-05-01

In the 1970s at the Battelle Pacific Northwest Laboratory (PNL), a series of critical experiments using a remotely operated Split-Table Machine was performed with homogeneous mixtures of (Pu-U)O{sub 2}-polystyrene fuels in the form of square compacts having different heights. The experiments determined the critical geometric configurations of MOX fuel assemblies with and without neutron poison plates. With respect to PuO{sub 2} content and moderation [H/(Pu+U)atomic] ratio (MR), two different homogeneous (Pu-U) O{sub 2}-polystyrene mixtures were considered: Mixture (1) 14.62 wt% PuO{sub 2} with 30.6 MR, and Mixture (2) 30.3 wt% PuO{sub 2} with 2.8 MR. In all mixtures, the uraniummore » was depleted to about O.151 wt% U{sup 235}. Assemblies contained copper, copper-cadmium or aluminum neutron poison plates having thicknesses up to {approximately}2.5 cm. This evaluation contains 22 experiments for Mixture 1, and 10 for Mixture 2 compacts. For Mixture 1, there are 10 configurations with copper plates, 6 with aluminum, and 5 with copper-cadmium. One experiment contained no poison plate. For Mixture 2 compacts, there are 3 configurations with copper, 3 with aluminum, and 3 with copper-cadmium poison plates. One experiment contained no poison plate.« less

Predictions of Actinide Solubilities under Near-Field Conditions Expected in the WIPP

NASA Astrophysics Data System (ADS)

Brush, L. H.; Xiong, Y.

2009-12-01

The Waste Isolation Pilot Plant (WIPP) is a U.S. Department of Energy (DOE) repository in southeast New Mexico for defense-related transuranic (TRU) waste. The repository, which opened in March 1999, is located at a subsurface depth of 655 m (2150 ft) in the Salado Fm., a Permian bedded-salt formation. The repository will eventually contain the equivalent of 844,000 208 L (55 gal) drums of TRU waste. After filling the rooms and access drifts and installing panel closures, creep closure of the salt will crush the steel waste containers in most cases and encapsulate the waste. The WIPP actinide source term model used for long-term performance assessment (PA) of the repository comprises dissolved and suspended submodels (solubilities and colloids). This presentation will describe the solubilities. From the standpoint of long-term PA, the order of importance of the radioelements in the TRU waste to be emplaced in the WIPP is Pu ~ Am >> U > Th >> Np ~ Cm and fission products. The DOE has included all of these actinides, but not fission products, in the WIPP Actinide Source Term Program (ASTP). Anoxic corrosion of Fe- and Al-base metals and microbial consumption of cellulosic, plastic, and rubber materials will produce gas and create strongly reducing conditions in the WIPP after closure. The use of MgO as an engineered barrier to consume microbially produced CO2 will result in low fCO2 and basic pH. Under these conditions, Th, U, Np, Pu, and Am will speciate essentially entirely as Th(IV), U(IV), Np(IV), Pu(III), and Am(III); or Th(IV), U(VI), Np(V), Pu(IV), and Am(III). The DOE has developed thermodynamic speciation-and-solubility models for +III, +IV, and +V actinides in brines. Experimental data for Nd, Am, and Cm species were used to parameterize the +III Pitzer activity-coefficient model; data for Th species were used for the +IV model; and data for Np(V) species were used for the +V model. These models include the effects of the organic ligands acetate, citrate, EDTA, and oxalate in TRU waste. The oxidation-state analogy was then used to extend the +III model to Pu(III), and the +IV model to Pu(IV), U(IV), and Np(IV). The solubility of U(VI) was estimated. For the recent WIPP Compliance Recertification Application PA Baseline Calculations, we calculated actinide solubilities with fCO2 buffered at 3.14 × 10-6 atm by the brucite-hydromagnesite carbonation reaction, with pH maintained at ~9 by the brucite dissolution-precipitation reaction, and with estimated concentrations of the organic ligands in brines from the Salado and the Castile Fm., which underlies the Salado. The calculated +III, +IV, and +V solubilities are 1.56 × 10-6, 5.64 × 10-8, and 4.07 × 10-7 M, respectively, in Salado brine; and 1.51 × 10-6, 6.98 × 10-8, and 8.75 × 10-7 M in Castile brine. The U(VI) solubility estimated for both brines is 1 × 10-3 M. This research is funded by WIPP programs administered by the U.S. Department of Energy. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy’s National Nuclear Security Administration under contract DE-AC04-94AL85000.

Method for photochemical reduction of uranyl nitrate by tri-N-butyl phosphate and application of this method to nuclear fuel reprocessing

DOEpatents

De Poorter, Gerald L.; Rofer-De Poorter, Cheryl K.

1978-01-01

Uranyl ion in solution in tri-n-butyl phosphate is readily photochemically reduced to U(IV). The product U(IV) may effectively be used in the Purex process for treating spent nuclear fuels to reduce Pu(IV) to Pu(III). The Pu(III) is readily separated from uranium in solution in the tri-n-butyl phosphate by an aqueous strip.

Determining Pu-239 content by resonance transmission analysis using a filtered reactor beam.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Klann, R. T.

A novel technique has been developed at Argonne National Laboratory to determine the {sup 239}Pu content in EBR-II blanket elements using resonance transmission analysis (RTA) with a filtered reactor beam. The technique uses cadmium and gadolinium filters along with a {sup 239}Pu fission chamber to isolate the 0.3 eV resonance in {sup 239}Pu. In the energy range from 0.1 to 0.5 eV, the total microscopic cross-section of {sup 239}Pu is significantly larger than the cross-sections of {sup 238}U and {sup 235}U. This large difference in cross-section allows small amounts of {sup 239}Pu to be detected in uranium samples. Tests usingmore » a direct beam from a 250 kW TRIGA reactor have been performed with stacks of depleted uranium and {sup 239}Pu foils. Preliminary measurement results are in good agreement with the predicted results up to about two weight percent of {sup 239}Pu in the sample. In addition, measured {sup 239}Pu masses were in agreement with actual sample masses with uncertainties less than 3.8 percent.« less

Mass and abundance 236U sensitivities at CIRCE

NASA Astrophysics Data System (ADS)

De Cesare, M.; De Cesare, N.; D'Onofrio, A.; Fifield, L. K.; Gialanella, L.; Terrasi, F.

2015-10-01

The actinides (e.g. 236U and xPu isotopes) are present in environmental samples at the ultra trace level since atmospheric tests of NWs (Nuclear Weapons) performed in the past, deliberate dumping of nuclear waste, nuclear fuel reprocessing, on a large scale and operation of NPPs (Nuclear Power Plants) on a small scale have led to the release of a wide range of radioactive nuclides in the environment. Their detection requires the most sensitive AMS (Accelerator Mass Spectrometry) techniques and at the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy, an upgraded actinide AMS system, based on a 3-MV pelletron tandem accelerator, has been operated. In this paper the progress made in order to push the 236U mass sensitivity and 236U/238U isotopic ratio down to the natural levels is reported. A uranium contamination mass of about 0.05 μg and a 236U/238U isotopic ratio sensitivities at the level of 3.2 × 10-13 are presently achievable.

New Episodes of Volcanism at Kilauea Volcano, Hawaii

NASA Astrophysics Data System (ADS)

Poland, Michael; Miklius, Asta; Orr, Tim; Sutton, Jeff; Thornber, Carl; Wilson, David

2008-01-01

Mid-2007 was a time of intense activity at Kilauea Volcano, Hawaii (see Figure 1). In June, the long-lived Pu`u `Ō`ō-Kupaianaha eruption, a dual-vent system along the east rift zone (ERZ) that has been erupting since 1983 [Heliker et al., 2003], paused due to the outbreak of a new vent farther up the rift (see Figure 2). The Pu`u `Ō`ō vent collapsed following that activity, and the resulting reorganization of the magma plumbing system led to the formation of a second new eruptive vent 2 kilometers downrift of Pu`u `Ō`ō.

Recovery of UO[sub 2]/PuO[sub 2] in IFR electrorefining process

DOEpatents

Tomczuk, Z.; Miller, W.E.

1994-10-18

A process is described for converting PuO[sub 2] and UO[sub 2] present in an electrorefiner to the chlorides, by contacting the PuO[sub 2] and UO[sub 2] with Li metal in the presence of an alkali metal chloride salt substantially free of rare earth and actinide chlorides for a time and at a temperature sufficient to convert the UO[sub 2] and PuO[sub 2] to metals while converting Li metal to Li[sub 2]O. Li[sub 2]O is removed either by reducing with rare earth metals or by providing an oxygen electrode for transporting O[sub 2] out of the electrorefiner and a cathode, and thereafter applying an emf to the electrorefiner electrodes sufficient to cause the Li[sub 2]O to disassociate to O[sub 2] and Li metal but insufficient to decompose the alkali metal chloride salt. The U and Pu and excess lithium are then converted to chlorides by reaction with CdCl[sub 2].

Recovery of UO.sub.2 /Pu O.sub.2 in IFR electrorefining process

DOEpatents

Tomczuk, Zygmunt; Miller, William E.

1994-01-01

A process for converting PuO.sub.2 and UO.sub.2 present in an electrorefiner to the chlorides, by contacting the PuO.sub.2 and UO.sub.2 with Li metal in the presence of an alkali metal chloride salt substantially free of rare earth and actinide chlorides for a time and at a temperature sufficient to convert the UO.sub.2 and PuO.sub.2 to metals while converting Li metal to Li.sub.2 O. Li.sub.2 O is removed either by reducing with rare earth metals or by providing an oxygen electrode for transporting O.sub.2 out of the electrorefiner and a cathode, and thereafter applying an emf to the electrorefiner electrodes sufficient to cause the Li.sub.2 O to disassociate to O.sub.2 and Li metal but insufficient to decompose the alkali metal chloride salt. The U and Pu and excess lithium are then converted to chlorides by reaction with CdCl.sub.2.

Sorption/Desorption Interactions of Plutonium with Montmorillonite

NASA Astrophysics Data System (ADS)

Begg, J.; Zavarin, M.; Zhao, P.; Kersting, A. B.

2012-12-01

Plutonium (Pu) release to the environment through nuclear weapon development and the nuclear fuel cycle is an unfortunate legacy of the nuclear age. In part due to public health concerns over the risk of Pu contamination of drinking water, predicting the behavior of Pu in both surface and sub-surface water is a topic of continued interest. Typically it was assumed that Pu mobility in groundwater would be severely restricted, as laboratory adsorption studies commonly show that naturally occurring minerals can effectively remove plutonium from solution. However, evidence for the transport of Pu over significant distances at field sites highlights a relative lack of understanding of the fundamental processes controlling plutonium behavior in natural systems. At several field locations, enhanced mobility is due to Pu association with colloidal particles that serve to increase the transport of sorbed contaminants (Kersting et al., 1999; Santschi et al., 2002, Novikov et al., 2006). The ability for mineral colloids to transport Pu is in part controlled by its oxidation state and the rate of plutonium adsorption to, and desorption from, the mineral surface. Previously we have investigated the adsorption affinity of Pu for montmorillonite colloids, finding affinities to be similar over a wide range of Pu concentrations. In the present study we examine the stability of adsorbed Pu on the mineral surface. Pu(IV) at an initial concentration of 10-10 M was pre-equilibrated with montmorillonite in a background electrolyte at pH values of 4, 6 and 8. Following equilibration, aliquots of the suspensions were placed in a flow cell and Pu-free background electrolyte at the relevant pH was passed through the system. Flow rates were varied in order to investigate the kinetics of desorption and hence gain a mechanistic understanding of the desorption process. The flow cell experiments demonstrate that desorption of Pu from the montmorillonite surface cannot be modeled as a simple first order process. Furthermore, a pH dependence was observed, with less desorbed at pH 4 compared to pH 8. We suggest the pH dependence is likely controlled by reoxidation of Pu(IV) to Pu(V) and aqueous speciation. We will present models used to describe desorption behavior and discuss the implications for Pu transport. References: Kersting, A.B.; Efurd, D.W.; Finnegan, D.L.; Rokop, D.J.; Smith, D.K.; Thompson J.L. (1999) Migration of plutonium in groundwater at the Nevada Test Site, Nature, 397, 56-59. Novikov A.P.; Kalmykov, S.N.; Utsunomiya, S.; Ewing, R.C.; Horreard, F.; Merkulov, A.; Clark, S.B.; Tkachev, V.V.; Myasoedov, B.F. (2006) Colloid transport of plutonium in the far-field of the Mayak Production Association, Russia, Science, 314, 638-641. Santschi, P.H.; Roberts, K.; Guo, L. (2002) The organic nature of colloidal actinides transported in surface water environments. Environ. Sci. Technol., 36, 3711-3719. This work was funded by U. S. DOE Office of Biological & Environmental Sciences, Subsurface Biogeochemistry Research Program, and performed under the auspices of the U. S. Department of Energy by Lawrence Livermore National Security, LLC under Contract DE-AC52-07NA27344. LLNL-ABS-570161

The Japanese aerial attack on Hanford Engineer Works

NASA Astrophysics Data System (ADS)

Clark, Charles W.

The day before the Pearl Harbor attack, December 6, 1941, the University of Chicago Metallurgical Laboratory was given four goals: design a plutonium (Pu) bomb; produce Pu by irradiation of uranium (U); extract Pu from the irradiated U; complete this in time to be militarily significant. A year later the first controlled nuclear chain reaction was attained in Chicago Pile 1 (CP-1). In January 1943, Hanford, WA was chosen as the site of the Pu factory. Neutron irradiation of 238U was to be used to make 239Pu. This was done by a larger version of CP-1, Hanford Reactor B, which went critical in September 1944. By July 1945 it had made enough Pu for two bombs: one used at the Trinity test in July; the other at Nagasaki, Japan in August. I focus on an ironic sidelight to this story: disruption of hydroelectric power to Reactor B by a Japanese fire balloon attack on March 10, 1945. This activated the costly coal-fired emergency backup plant to keep the reactor coolant water flowing, thwarting disaster and vindicating the conservative design of Hanford Engineer Works. Management of the Hanford Engineer Works in World War II, H. Thayer (ASCE Press 1996).

Optical detection of special nuclear materials: an alternative approach for standoff and remote sensing

NASA Astrophysics Data System (ADS)

Johnson, J. Bruce; Reeve, S. W.; Burns, W. A.; Allen, Susan D.

2010-04-01

Termed Special Nuclear Material (SNM) by the Atomic Energy Act of 1954, fissile materials, such as 235U and 239Pu, are the primary components used to construct modern nuclear weapons. Detecting the clandestine presence of SNM represents an important capability for Homeland Security. An ideal SNM sensor must be able to detect fissile materials present at ppb levels, be able to distinguish between the source of the detected fissile material, i.e., 235U, 239Pu, 233U or other fission source, and be able to perform the discrimination in near real time. A sensor with such capabilities would provide not only rapid identification of a threat but, ultimately, information on the potential source of the threat. For example, current detection schemes for monitoring clandestine nuclear testing and nuclear fuel reprocessing to provide weapons grade fissile material rely largely on passive air sampling combined with a subsequent instrumental analysis or some type of wet chemical analysis of the collected material. It would be highly useful to have a noncontact method of measuring isotopes capable of providing forensic information rapidly at ppb levels of detection. Here we compare the use of Kr, Xe and I as "canary" species for distinguishing between 235U and 239Pu fission sources by spectroscopic methods.

Simulation of radiation driven fission gas diffusion in UO 2, ThO 2 and PuO 2

DOE PAGES

Cooper, Michael William D.; Stanek, Christopher Richard; Turnbull, James Anthony; ...

2016-12-01

Below 1000 K it is thought that fission gas diffusion in nuclear fuel during irradiation occurs through atomic mixing due to radiation damage. Here we present a molecular dynamics (MD) study of Xe, Kr, Th, U, Pu and O diffusion due to irradiation. It is concluded that the ballistic phase does not sufficiently account for the experimentally observed diffusion. Thermal spike simulations are used to confirm that electronic stopping remedies the discrepancy with experiment and the predicted diffusivities lie within the scatter of the experimental data. Here, our results predict that the diffusion coefficients are ordered such that D* 0more » > D* Kr > D* Xe > D* U. For all species >98.5% of diffusivity is accounted for by electronic stopping. Fission gas diffusivity was not predicted to vary significantly between ThO 2, UO 2 and PuO 2, indicating that this process would not change greatly for mixed oxide fuels.« less

Oxygen diffusion in Gd-doped mixed oxides

DOE PAGES

Galvin, C. O. T.; Cooper, M. W. D.; Rushton, M. J. D.; ...

2017-10-23

Molecular dynamics simulations have been performed to investigate oxygen transport in (U xPu x-1) 0.95Gd 0.05O 1.975, (U xTh x-1) 0.95Gd 0.05O 1.975 and (Pu xTh x-1) 0.95Gd 0.05O 1.975 between 1000 and 3200 K. Oxygen diffusivity and corresponding activation energies are examined and compared to values for the undoped (U xPu x-1)O 2, (U xTh x-1)O 2 and (Pu xTh x-1)O 2 systems where compositions between end members display enhanced diffusivity. Below the superionic transition oxygen diffusivity for the Gd doped systems is orders of magnitude greater compared to their undoped counterparts. But, enhanced diffusivity for doped mixed actinidemore » cation compositions is not observed compared to doped end members. Furthermore, changes in activation energy suggest changes in diffusion regime, which correspond to the creation of thermally activated oxygen defects.« less

Oxygen diffusion in Gd-doped mixed oxides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Galvin, C. O. T.; Cooper, M. W. D.; Rushton, M. J. D.

Molecular dynamics simulations have been performed to investigate oxygen transport in (U xPu x-1) 0.95Gd 0.05O 1.975, (U xTh x-1) 0.95Gd 0.05O 1.975 and (Pu xTh x-1) 0.95Gd 0.05O 1.975 between 1000 and 3200 K. Oxygen diffusivity and corresponding activation energies are examined and compared to values for the undoped (U xPu x-1)O 2, (U xTh x-1)O 2 and (Pu xTh x-1)O 2 systems where compositions between end members display enhanced diffusivity. Below the superionic transition oxygen diffusivity for the Gd doped systems is orders of magnitude greater compared to their undoped counterparts. But, enhanced diffusivity for doped mixed actinidemore » cation compositions is not observed compared to doped end members. Furthermore, changes in activation energy suggest changes in diffusion regime, which correspond to the creation of thermally activated oxygen defects.« less

Reactor Neutronics: Impact of Fissile Material

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heidet, F.; Hill, R. N.

Here, given a wide variety of reactor designs and fuel types, it can be difficult to identify the underlying cause of basic performance differences such as flux level and enrichment requirement. In this paper, using solely the definitions of the core multiplication factor and core power, simple relations have been derived allowing estimates of the flux ratio and fissile material concentration ratio for any reactor concept when 235U is replaced with 239Pu or vice-versa. These relations are functions of the neutron non-leakage probability, and one only needs to know number of neutrons emitted per fission, and the fission cross-section ratiomore » between the 235U system and the 239Pu system. It is found that for a reactor concept having significant leakage, the achievable flux level when using 239Pu as fissile material can be up to 45% larger than when using 235U as fissile material, and the required fissile concentration of 239Pu is up to 48% lower than that of 235U to achieve criticality.« less

Reactor Neutronics: Impact of Fissile Material

DOE PAGES

Heidet, F.; Hill, R. N.

2017-06-09

Here, given a wide variety of reactor designs and fuel types, it can be difficult to identify the underlying cause of basic performance differences such as flux level and enrichment requirement. In this paper, using solely the definitions of the core multiplication factor and core power, simple relations have been derived allowing estimates of the flux ratio and fissile material concentration ratio for any reactor concept when 235U is replaced with 239Pu or vice-versa. These relations are functions of the neutron non-leakage probability, and one only needs to know number of neutrons emitted per fission, and the fission cross-section ratiomore » between the 235U system and the 239Pu system. It is found that for a reactor concept having significant leakage, the achievable flux level when using 239Pu as fissile material can be up to 45% larger than when using 235U as fissile material, and the required fissile concentration of 239Pu is up to 48% lower than that of 235U to achieve criticality.« less

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

PubMed

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

2002-11-01

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

Neutron-induced fission cross section of 240Pu from 0.5 MeV to 3 MeV

NASA Astrophysics Data System (ADS)

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

2015-07-01

240Pu has recently been pointed out by a sensitivity study of the Organization for Economic Cooperation and Development (OECD) Nuclear Energy Agency (NEA) to be one of the isotopes whose fission cross section lacks accuracy to meet the upcoming needs for the future generation of nuclear power plants (GEN-IV). In the High Priority Request List (HPRL) of the OECD, it is suggested that the knowledge of the 240Pu(n ,f ) cross section should be improved to an accuracy within 1-3 %, compared to the present 5%. A measurement of the 240Pu cross section has been performed at the Van de Graaff accelerator of the Joint Research Center (JRC) Institute for Reference Materials and Measurements (IRMM) using quasi-monoenergetic neutrons in the energy range from 0.5 MeV to 3 MeV. A twin Frisch-grid ionization chamber (TFGIC) has been used in a back-to-back configuration as fission fragment detector. The 240Pu(n ,f ) cross section has been normalized to three different isotopes: 237Np(n ,f ) , 235U (n ,f ) , and 238U (n ,f ) . Additionally, the secondary standard reactions were benchmarked through measurements against the primary standard reaction 235U (n ,f ) in the same geometry. A comprehensive study of the corrections applied to the data and the associated uncertainties is given. The results obtained are in agreement with previous experimental data at the threshold region. For neutron energies higher than 1 MeV, the results of this experiment are slightly lower than the ENDF/B-VII.1 evaluation, but in agreement with the experiments of Laptev et al. (2004) as well as Staples and Morley (1998).

Physics of hydride fueled PWR

NASA Astrophysics Data System (ADS)

Ganda, Francesco

The first part of the work presents the neutronic results of a detailed and comprehensive study of the feasibility of using hydride fuel in pressurized water reactors (PWR). The primary hydride fuel examined is U-ZrH1.6 having 45w/o uranium: two acceptable design approaches were identified: (1) use of erbium as a burnable poison; (2) replacement of a fraction of the ZrH1.6 by thorium hydride along with addition of some IFBA. The replacement of 25 v/o of ZrH 1.6 by ThH2 along with use of IFBA was identified as the preferred design approach as it gives a slight cycle length gain whereas use of erbium burnable poison results in a cycle length penalty. The feasibility of a single recycling plutonium in PWR in the form of U-PuH2-ZrH1.6 has also been assessed. This fuel was found superior to MOX in terms of the TRU fractional transmutation---53% for U-PuH2-ZrH1.6 versus 29% for MOX---and proliferation resistance. A thorough investigation of physics characteristics of hydride fuels has been performed to understand the reasons of the trends in the reactivity coefficients. The second part of this work assessed the feasibility of multi-recycling plutonium in PWR using hydride fuel. It was found that the fertile-free hydride fuel PuH2-ZrH1.6, enables multi-recycling of Pu in PWR an unlimited number of times. This unique feature of hydride fuels is due to the incorporation of a significant fraction of the hydrogen moderator in the fuel, thereby mitigating the effect of spectrum hardening due to coolant voiding accidents. An equivalent oxide fuel PuO2-ZrO2 was investigated as well and found to enable up to 10 recycles. The feasibility of recycling Pu and all the TRU using hydride fuels were investigated as well. It was found that hydride fuels allow recycling of Pu+Np at least 6 times. If it was desired to recycle all the TRU in PWR using hydrides, the number of possible recycles is limited to 3; the limit is imposed by positive large void reactivity feedback.

Relativistic Coulomb Fission

NASA Technical Reports Server (NTRS)

Norbury, John W.

1992-01-01

Nuclear fission reactions induced by the electromagnetic field of relativistic nuclei are studied for energies relevant to present and future relativistic heavy ion accelerators. Cross sections are calculated for U-238 and Pu-239 fission induced by C-12, Si-28, Au-197, and U-238 projectiles. It is found that some of the cross sections can exceed 10 b.

Feasibility study of 235U and 239Pu characterization in radioactive waste drums using neutron-induced fission delayed gamma rays

NASA Astrophysics Data System (ADS)

Nicol, T.; Pérot, B.; Carasco, C.; Brackx, E.; Mariani, A.; Passard, C.; Mauerhofer, E.; Collot, J.

2016-10-01

This paper reports a feasibility study of 235U and 239Pu characterization in 225 L bituminized waste drums or 200 L concrete waste drums, by detecting delayed fission gamma rays between the pulses of a deuterium-tritium neutron generator. The delayed gamma yields were first measured with bare samples of 235U and 239Pu in REGAIN, a facility dedicated to the assay of 118 L waste drums by Prompt Gamma Neutron Activation Analysis (PGNAA) at CEA Cadarache, France. Detectability in the waste drums is then assessed using the MCNPX model of MEDINA (Multi Element Detection based on Instrumental Neutron Activation), another PGNAA cell dedicated to 200 L drums at FZJ, Germany. For the bituminized waste drum, performances are severely hampered by the high gamma background due to 137Cs, which requires the use of collimator and shield to avoid electronics saturation, these elements being very penalizing for the detection of the weak delayed gamma signal. However, for lower activity concrete drums, detection limits range from 10 to 290 g of 235U or 239Pu, depending on the delayed gamma rays of interest. These detection limits have been determined by using MCNPX to calculate the delayed gamma useful signal, and by measuring the experimental gamma background in MEDINA with a 200 L concrete drum mock-up. The performances could be significantly improved by using a higher interrogating neutron emission and an optimized experimental setup, which would allow characterizing nuclear materials in a wide range of low and medium activity waste packages.

PLUTONIUM-URANIUM ALLOY

DOEpatents

Coffinberry, A.S.; Schonfeld, F.W.

1959-09-01

Pu-U-Fe and Pu-U-Co alloys suitable for use as fuel elements tn fast breeder reactors are described. The advantages of these alloys are ease of fabrication without microcracks, good corrosion restatance, and good resistance to radiation damage. These advantages are secured by limitation of the zeta phase of plutonium in favor of a tetragonal crystal structure of the U/sub 6/Mn type.

Natural and man-made radioactivity in soils and plants around the research reactor of Inshass.

PubMed

Higgy, R H; Pimpl, M

1998-12-01

The specific radioactivities of the U-series, 232Th, 137Cs and 40K were measured in soil samples around the Inshass reactor in Cairo, using a gamma-ray spectrometer with a HpGe detector. The alpha activity of 238U, 234U and 235U was measured in the same soil samples by surface barrier detectors after radiochemical separation and the obtained results were compared with the specific activities determined by gamma-measurements. The alpha-activity of 238Pu, 239+240Pu, 241Am, 242Cm and 244Cm was measured after radiochemical separation by surface barrier detectors for both soil and plant samples. Then beta-activity of 241Pu was measured using liquid scintillation spectrometry.

Study of 236U/238U ratio at CIRCE using a 16-strip silicon detector with a TOF system

NASA Astrophysics Data System (ADS)

De Cesare, M.; De Cesare, N.; D'Onofrio, A.; Gialanella, L.; Terrasi, F.

2015-04-01

Accelerator Mass Spectrometry (AMS) is presently the most sensitive technique for the measurement of long-lived actinides, e.g. 236U and xPu isotopes. A new actinide AMS system, based on a 3-MV pelletron tandem accelerator, is operated at the Center for Isotopic Research on Cultural and Environmental Heritage (CIRCE) in Caserta, Italy. In this paper we report on the procedure adopted to increase the 236U abundance sensitivity as low as possible. The energy and position determinations of the 236U ions, using a 16-strip silicon detector have been obtained. A 236U/238U isotopic ratio background level of about 2.9×10-11 was obtained, summing over all the strips, using a Time of Flight-Energy (TOF-E) system with a 16-strip silicon detector (4.9×10-12 just with one strip).

Thermal conductivity of heterogeneous LWR MOX fuels

NASA Astrophysics Data System (ADS)

Staicu, D.; Barker, M.

2013-11-01

It is generally observed that the thermal conductivity of LWR MOX fuel is lower than that of pure UO2. For MOX, the degradation is usually only interpreted as an effect of the substitution of U atoms by Pu. This hypothesis is however in contradiction with the observations of Duriez and Philiponneau showing that the thermal conductivity of MOX is independent of the Pu content in the ranges 3-15 and 15-30 wt.% PuO2 respectively. Attributing this degradation to Pu only implies that stoichiometric heterogeneous MOX can be obtained, while we show that any heterogeneity in the plutonium distribution in the sample introduces a variation in the local stoichiometry which in turn has a strong impact on the thermal conductivity. A model quantifying this effect is obtained and a new set of experimental results for homogeneous and heterogeneous MOX fuels is presented and used to validate the proposed model. In irradiated fuels, this effect is predicted to disappear early during irradiation. The 3, 6 and 10 wt.% Pu samples have a similar thermal conductivity. Comparison of the results for this homogeneous microstructure with MIMAS (heterogeneous) fuel of the same composition showed no difference for the Pu contents of 3, 5.9, 6, 7.87 and 10 wt.%. A small increase of the thermal conductivity was obtained for 15 wt.% Pu. This increase is of about 6% when compared to the average of the values obtained for 3, 6 and 10 wt.% Pu. For comparison purposes, Duriez also measured the thermal conductivity of FBR MOX with 21.4 wt.% Pu with O/M = 1.982 and a density close to 95% TD and found a value in good agreement with the estimation obtained using the formula of Philipponneau [8] for FBR MOX, and significantly lower than his results corresponding to the range 3-15 wt.% Pu. This difference in thermal conductivity is of about 20%, i.e. higher than the measurement uncertainties.Thus, a significant difference was observed between FBR and PWR MOX fuels, but was not explained. This difference was observed for hypostoichiometric fuels, that correspond to the condition used for irradiation. However, if these two formulas are evaluated for O/M = 2.000, the difference between the predictions is negligible (Fig. 1). The difference becomes significant for non-stoichiometric fuels, as shown for O/M = 1.975 in Fig. 1. The microstructure of the FBR fuel with 21.4 wt.% Pu was not described in the paper of Duriez. Taking into account the rigorous experimental methodology used by Duriez (characterisation of the stoichiometry), a possible explanation is an interaction between the plutonium distribution and the stoichiometry. Another parameter having a strong impact on the conductivity is the porosity correction used to obtain the values for 95% TD. This correction is small in the work of Duriez as the samples density is very close to 95% TD. This was also the case for the samples selected by Philipponneau in order to obtain his recommendation. An effect due to differences in the pores shape can also be excluded, as the results are identical for stoichiometric fuels (Fig. 1). Usually the apparent stoichiometry is obtained by heat treatments and checked before and after the measurements, either by XRD or thermogravimetry. However, for non-perfectly homogeneous samples, the gradients in the plutonium distribution induce a non-uniform oxygen distribution, which is difficult to characterise experimentally. It has been proposed by Baron that the deviation from stoichiometry is the main cause for the differences observed between fresh UO2 and MOX [14,15], this effect is quantified in the next section. In the first model ("Model 1"), the effect of Pu is neglected over the entire relevant Pu compositions range (up to 24 wt.% PuO2), and a correlation obtained for non-stoichiometric homogeneous (U,Pu)O2 is used. In the second model ("Model 2", the effect of Pu is supposed to be present at all compositions, with the stoichiometry effect. The thermal conductivity is described by the correlations of Fink [16] for the UO2 matrix, Duriez at low PuO2 contents (coating phase) and of Philipponneau at high PuO2 contents (agglomerates). For the first model, applying a correlation for non-stoichiometric UO2 would be relevant, but such a correlation does not exist for physical reasons in the hypostoichiometric domain. A correlation for homogeneous (U,Pu)O2+x has to be obtained in order to predict the thermal conductivity of heterogeneous MOX fuel, supposing that the effect of Pu can be neglected, i.e. supposing that the thermal conductivities of homogeneous (U,Pu)O2 and UO2 are equal both for stoichiometric and non-stoichiometric fuels. Such a correlation has to be obtained considering reliable data for stoichiometric UO2 and stoichiometry dependence. Different correlations for non-stoichiometric fuels were reviewed [2,8,12,13,15,35,36]. The correlation of Martin [36], available for hyperstoichiometric UO2, was evaluated in the hypostoichiometric domain and the predictions were found to give a stoichiometry dependence very similar to a correlation already proposed [15]. Investigations by Molecular Dynamics [37] have confirmed the almost symmetric effect of the hypo- and hyper-stoichiometry in UO2. We therefore use the correlation of Martin, with however a correction, as for stoichiometric fuels it over predicts the conductivity of stoichiometric UO2 at high temperatures, when compared to the recommendation of Fink [16] (Fig. 4). Analysis has shown that this over-prediction was due to the high temperature term in the correlation of Martin, and that, if this term is removed, the predictions of Martin and Fink were identical for stoichiometric fuels in the temperature range 500-1500 K. The correlation proposed for homogeneous MOX is therefore given by the following equation. k=(0.035 The series and parallel bounds (Eq. (2)) were calculated using the thermal conductivity values given by Eq. (5) for the heterogeneous MOX constituents and the maximum difference between these two bounds is 2% over the considered temperature range. The predictions obtained with the equations of Maxwell-Eucken (Eq. (3)) and Bergman (Eq. (4)) are equal and are in the interval between the series and parallel bounds. This result shows that the use of a sophisticated analytical or numerical model to predict the thermal conductivity is not justified [38]. The model of Maxwell-Eucken [31] was therefore chosen to predict the equivalent thermal conductivity of the heterogeneous MOX.The equivalent thermal conductivity of the stoichiometric heterogeneous MOX with an average PuO2 content of 7.2 wt.% (constituted by a stoichiometric UO2 matrix containing 15 vol.% of (U0.76Pu0.24)O1.975 agglomerates and 55 vol.% of a coating phase of (U0.94Pu0.06)O1.995) was calculated. The results show that the apparent thermal conductivity of the heterogeneous MOX, calculated using homogeneous MOX data (Eq. (5)) with O/M = 2.000, 1.995 and 1.975 (labeled Model 1 in Fig. 4) is not significantly different from the values measured by Duriez. The latter values are also very similar to the thermal conductivity of homogeneous MOX with O/M = 1.995. This simple model shows that the stoichiometry effect is sufficient to explain the lower thermal conductivity of LWR MOX fuel as compared to UO2. The advantage of this simple model is its consistency, as the calculations for the heterogeneous MOX are based on a unique formula for non-stoichiometric homogeneous (U,Pu)O2.In the second model, the effect of the plutonium is taken into account for the coating phase and for the Pu-rich agglomerates. The thermal conductivity is described by the correlations of Fink [16] for UO2.000, of Duriez et al. [2] for (U0.94Pu0.06)O1.995 (coating phase with low PuO2 content) and of Philipponneau [8] for (U0.76Pu0.24)O1.975 (Pu-rich agglomerates with high PuO2 content). The results (labeled Model 2 in Fig. 5) show that the calculated thermal conductivity of the heterogeneous 'stoichiometric' MOX is lower than UO2 and also lower than for stoichiometric MOX as given by Duriez. Therefore taking into account both the heterogeneity in the oxygen distribution and the Pu content leads to an underprediction of the thermal conductivity of heterogeneous MOX. A possible cause for the lower thermal conductivity of unirradiated heterogeneous MOX is therefore the intrinsic fluctuations of the local stoichiometry and only to a lesser extent the perturbation of the heat transfer due to the substitution of the U by Pu atoms in the crystal lattice. This interpretation was already proposed by Baron [14,15]. This assumption is acceptable if the size of the heterogeneities is much smaller that the thickness of the sample. A theoretical criterion for the impact of these parameters, initially proposed by Kerrish [40], was checked experimentally by Lee and Taylor [41] and was found to be too restrictive. The conclusions resulting from the investigations of Lee are that for diffusivity ratios between 1 and 3.5 and volume fractions up to 30%, a ratio of 5 between the sample thickness and inclusions diameter is sufficient. Our heterogeneous samples fulfill this criterion, taking into account that the thermal diffusivity ratio is close to 1 in MOX, that the volume fraction of Pu rich agglomerates is under 30%, and that the agglomerates have a diameter of less than 200 μm compared to the sample (disc) thickness of 1 mm. The most severe requirement that one could use to define a medium behaving like a homogeneous material is that the heat transfer is not affected by the heterogeneities. This is the case for instance if we have a heterogeneous material where the two constituents have equal thermal diffusivity and no thermal resistance is present at the interfaces. This requirement is very close to be perfectly verified for the heterogeneous MOX, as UO2 and (U,Pu)O2 have very close values of the thermal diffusivity. An effect of the sample heterogeneity can also be excluded from the point of view of the location where the thermograms are recorded: the temperature transients on the rear face of the samples are measured with a pyrometer and the system is provided with a lens assembly which enables a 1 mm diameter spot of the sample surface to be focused onto the signal collecting fibre. The thermograms are therefore averaged over a 1 mm diameter surface, which is much larger than the size of the heterogeneities (Pu rich agglomerates with a size of less than 200 μm).The impact of sample thickness on the measured thermal diffusivity was experimentally investigated for the MIMAS MOX with 7.0 wt.% Pu. For this purpose, discs of 0.5, 1, 2, and 3 mm thickness were cut and the thermal diffusivity was measured. The same investigation was done for standard UO2, in order to verify the accuracy of the inverse technique used for the identification of the thermal diffusivity from the thermograms. The inverse technique [39] explicitly takes into account the sample thickness in the calculation of the heat losses. The results for UO2 (Fig. 6) show that the measured thermal diffusivity does not depend on sample thickness, and is in good agreement with the recommendation of Fink [16]. The results for the heterogeneous MOX (Fig. 7) also show no dependence on sample thickness.

An Episode 56 Perspective on Post-2001 Comagmatic Mixing Along Kilauea's East Rift Zone

NASA Astrophysics Data System (ADS)

Thornber, C.; Orr, T.; Lowers, H.; Heliker, C.; Hoblitt, R.

2007-12-01

A significant change in the petrology of Pu`u `O`o -Kupaianaha lava occurred in April 2001 (3 years after the onset of the decade-long episode 55). Prior to that time all steady-state eruption products were olivine phryic. After that time and until the Kane Nui o Hamo eruption of June 19, 2007 (episode 56), all magma erupted from vents in and around Pu`u `O`o was olivine and pyroxene-phyric containing <1mm, isolated or clustered clinopyroxene (±olivine, ±plagioclase), usually with resorbed edges. Textures, phase chemistry and low-pressure phase relations define a pre-eruptive mixing environment that is driven by continuous recharge of a stagnant, near-cotectic shallow magma body. The comagmatic nature of the cooler component in the post-2001 hybrid magma is verified by low concentrations of incompatible elements relative to MgO. Since the eruption began in 1983, the olivine-saturated liquid-line-of-descent has progressively shifted toward the present-day low concentrations of incompatible elements. Superimposed on this long-term trend are shorter chemical cycles (months to years) which track fractionation and recharge between comagmatic endmembers of ~10 and ~7 wt% MgO. These shorter cycles correspond to heating and cooling events and imply magmatic recharge of a sustained shallow magma reservoir within the eruptive plumbing system. The longest cooling cycle of the entire eruption began in April 1998 after effusion of the hottest and most- primitive lava erupted since 1985 (episodes 30 and 31). Glass temperatures up to 1168°C and bulk MgO of 9.5 wt% steadily declined for 6 years until late 2004 when they bottomed-out at 1140°C and 6.8 wt%. This signaled a stable near-cotectic magma condition. MgO contents and glass temperatures stailized at ~7.1 wt% and 1146°C for the remainder of episode 55, as the hybrid magmas were stirred by a steady influx of summit-derived magma beneath a complex of intermittently active Pu`u O`o vents. During the June 19, 2007 Kane Nui O Hamo eruption (episode 56), as with the January 1997 Napua Crater event (episode 54), the summit deflated and Pu`u O`o collapsed as magma was drawn from either end of the active rift conduit toward a zone of extension. In both cases, magma returned to the Pu`u `O`o vent area after the conduit repressurized. However, in contrast to cool and porphyritic hybrid magma erupted through isolated and chemically evolved rift magma reservoirs at Napau Crater, the episode 56 lava is relatively primitive (8.7 wt% MgO) and 30 to 50°C hotter at 1160°C. This is likely to be summit-derived magma from within the active rift conduit beneath Kane Nui o Hamo. The episode 56 lava is ~15°C hotter than the late episode 55 hybrid magmas with consistently low incompatible elements and likely represents the recharge component that maintained a shallow reservoir at near-cotectic conditions beneath the vicinity of the Pu`u `O`o vents for the last several years. Both lava erupted from Pu`u `O`o in early June, 2007(episode 57), and lava the from the July 21-24 sequence of fissure eruptions down-rift of Pu`u `O`o (early episode 58) contain a distinctly hybrid phenocryst and glomerocryst assemblage, suggesting a flushing of cooler crystal-laden magma from the conduit.

Low intensity hawaiian fountaining as exemplified by the March 2011, Kamoamoa eruption at Kilauea Volcano, Hawai`i (Invited)

NASA Astrophysics Data System (ADS)

Orr, T. R.; Houghton, B. F.; Poland, M. P.; Patrick, M. R.; Thelen, W. A.; Sutton, A. J.; Parcheta, C. E.; Thornber, C. R.

2013-12-01

The latest 'classic' hawaiian high-fountaining activity at Kilauea Volcano occurred in 1983-1986 with construction of the Pu`u `O`o pyroclastic cone. Since then, eruptions at Kilauea have been dominated by nearly continuous effusive activity. Episodes of sustained low hawaiian fountaining have occurred but are rare and restricted to short-lived fissure eruptions along Kilauea's east rift zone. The most recent of these weakly explosive fissure eruptions--the Kamoamoa eruption--occurred 5-9 March 2011. The Kamoamoa eruption was probably the consequence of a decrease in the carrying capacity of the conduit feeding the episode 58 eruptive vent down-rift from Pu`u `O`o in Kilauea's east rift zone. As output from the vent waned, Kilauea's summit magma storage and east rift zone transport system began to pressurize, as manifested by an increase in seismicity along the upper east rift zone, inflation of the summit and Pu`u `O`o, expansion of the east rift zone, and rising lava levels at both the summit and Pu`u `O`o. A dike began propagating towards the surface from beneath Makaopuhi Crater, 6 km west of Pu`u `O`o, at 1342 Hawaiian Standard Time (UTC - 10 hours) on 5 March. A fissure eruption started about 3.5 hours later near Nāpau Crater, 2 km uprift of Pu`u `O`o. Activity initially jumped between numerous en echelon fissure segments before centering on discrete vents near both ends of the 2.4-km-long fissure system for the final two days of the eruption. About 2.6 mcm of lava was erupted over the course of four days with a peak eruption rate of 11 m3/s. The petrologic characteristics of the fissure-fed lava indicate mixing between hotter mantle-derived magma and cooler rift-stored magma, with a greater proportion of the cooler component than was present in east rift zone lava erupting before March 2011. The fissure eruption was accompanied by the highest SO2 emission rates since 1986. Coincidentally, the summit and Pu`u `O`o deflated as magma drained away, causing expansion of the ERZ. The geological, geophysical, and geochemical datasets collected before, during, and after the Kamoamoa eruption provide an unprecedented account of what, at least in recent decades, is the 'normal' mode for hawaiian fountaining at Kilauea--that is, low intensity fissure-fed eruptions. This activity differs from high fountaining in that there is little physical coupling between melt and magmatic gas--for much of the Kamoamoa eruption lava ponded sluggishly over the vents and was weakly disrupted by bursts from trains of very closely spaced gas bubbles. Such eruptions enable us to examine the middle ground between strombolian and classical hawaiian behaviors at basaltic volcanoes.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tylka, M. M.; Willit, J. L.; Williamson, M. A.

This work examines the nucleation and growth behavior of uranium and plutonium from molten LiCl-KCl eutectic on inert electrodes using electrochemical techniques. Current-time transients obtained from chronoamperometric experiments were compared with theoretical models to characterize the type of nucleation (progressive or instantaneous) for deposition of U and Pu, and co-deposition of U-Pu, from molten LiCl-KCl at inert electrodes. It was established that the nucleation mode of actinides present as chlorides in molten chloride salts changes from progressive to instantaneous with an increasing concentration of the trivalent actinide ions in the salt. The effect of the material of the working electrodemore » was investigated, and it was found that changing the material from tungsten to silver improves resolvability of the nucleation peaks and allows more accurate analysis of the experimental measurements. Using the nucleation data, diffusion coefficients were obtained for U 3+ and Pu 3+, and were found to be in very good agreement with the values obtained from other studies. Furthermore, the density of nuclei produced during instantaneous nucleation, the rate of nucleation for progressive nucleation, and the radius of the deposited nuclei were evaluated and examined at different overpotentials.« less

Electrochemical Nucleation and Growth of Uranium and Plutonium from Molten Salts

DOE PAGES

Tylka, M. M.; Willit, J. L.; Williamson, M. A.

2017-07-18

This work examines the nucleation and growth behavior of uranium and plutonium from molten LiCl-KCl eutectic on inert electrodes using electrochemical techniques. Current-time transients obtained from chronoamperometric experiments were compared with theoretical models to characterize the type of nucleation (progressive or instantaneous) for deposition of U and Pu, and co-deposition of U-Pu, from molten LiCl-KCl at inert electrodes. It was established that the nucleation mode of actinides present as chlorides in molten chloride salts changes from progressive to instantaneous with an increasing concentration of the trivalent actinide ions in the salt. The effect of the material of the working electrodemore » was investigated, and it was found that changing the material from tungsten to silver improves resolvability of the nucleation peaks and allows more accurate analysis of the experimental measurements. Using the nucleation data, diffusion coefficients were obtained for U 3+ and Pu 3+, and were found to be in very good agreement with the values obtained from other studies. Furthermore, the density of nuclei produced during instantaneous nucleation, the rate of nucleation for progressive nucleation, and the radius of the deposited nuclei were evaluated and examined at different overpotentials.« less

Carbon dioxide of Pu`u`O`o volcanic plume at Kilauea retrieved by AVIRIS hyperspectral data

USGS Publications Warehouse

Spinetti, C.; Carrere, V.; Buongiorno, M. Fabrizia; Sutton, A.J.; Elias, T.

2008-01-01

A remote sensing approach permits for the first time the derivation of a map of the carbon dioxide concentration in a volcanic plume. The airborne imaging remote sensing overcomes the typical difficulties associated with the ground measurements and permits rapid and large views of the volcanic processes together with the measurements of volatile components exolving from craters. Hyperspectral images in the infrared range (1900-2100??nm), where carbon dioxide absorption lines are present, have been used. These images were acquired during an airborne campaign by the Airborne Visible/Infrared Imaging Spectrometer (AVIRIS) over the Pu`u` O`o Vent situated at the Kilauea East Rift zone, Hawaii. Using a radiative transfer model to simulate the measured up-welling spectral radiance and by applying the newly developed mapping technique, the carbon dioxide concentration map of the Pu`u` O`o Vent plume were obtained. The carbon dioxide integrated flux rate were calculated and a mean value of 396 ?? 138??t d- 1 was obtained. This result is in agreement, within the measurements errors, with those of the ground measurements taken during the airborne campaign. ?? 2008 Elsevier Inc.

Optimization of ISOCS Parameters for Quantitative Non-Destructive Analysis of Uranium in Bulk Form

NASA Astrophysics Data System (ADS)

Kutniy, D.; Vanzha, S.; Mikhaylov, V.; Belkin, F.

2011-12-01

Quantitative calculation of the isotopic masses of fissionable U and Pu is important for forensic analysis of nuclear materials. γ-spectrometry is the most commonly applied tool for qualitative detection and analysis of key radionuclides in nuclear materials. Relative isotopic measurement of U and Pu may be obtained from γ-spectra through application of special software such as MGAU (Multi-Group Analysis for Uranium, LLNL) or FRAM (Fixed-Energy Response Function Analysis with Multiple Efficiency, LANL). If the concentration of U/Pu in the matrix is unknown, however, isotopic masses cannot be calculated. At present, active neutron interrogation is the only practical alternative for non-destructive quantification of fissionable isotopes of U and Pu. An active well coincidence counter (AWCC), an alternative for analyses of uranium materials, has the following disadvantages: 1) The detection of small quantities (≤100 g) of 235U is not possible in many models; 2) Representative standards that capture the geometry, density and chemical composition of the analyzed unknown are required for precise analysis; and 3) Specimen size is severely restricted by the size of the measuring chamber. These problems may be addressed using modified γ-spectrometry techniques based on a coaxial HPGe-detector and ISOCS software (In Situ Object Counting System software, Canberra). We present data testing a new gamma-spectrometry method uniting actinide detection with commonly utilized software, modified for application in determining the masses of the fissionable isotopes in unknown samples of nuclear materials. The ISOCS software, widely used in radiation monitoring, calculates the detector efficiency curve in a specified geometry and range of photon energies. In describing the geometry of the source-detector, it is necessary to clearly describe the distance between the source and the detector, the material and the thickness of the walls of the container, as well as material, density and chemical composition of the matrix of the specimen. Obviously, not all parameters can be characterized when measuring samples of unknown composition or uranium in bulk form. Because of this, and especially for uranium materials, the IAEA developed an ISOCS optimization procedure. The target values for the optimization are Μmatrixfixed, the matrix mass determined by weighing with a known mass container, and Εfixed, the 235U enrichment, determined by MGAU. Target values are fitted by varying the matrix density (ρ), and the concentration of uranium in the matrix of the unknown (w). For each (ρi, wi), an efficiency curve is generated, and the masses of uranium isotopes, Μ235Ui and Μ238Ui, determined using spectral activity data and known specific activities for U. Finally, fitted parameters are obtained for Μmatrixi = Μmatrixfixed ± 1σ, Εi = Εfixed ± 1σ, as well as important parameters (ρi, wi, Μ235Ui, Μ238Ui, ΜUi). We examined multiple forms of uranium (powdered, pressed, and scrap UO2 and U3O8) to test this method for its utility in accurately identifying the mass and enrichment of uranium materials, and will present the results of this research.

Evolution of the Reactor Antineutrino Flux and Spectrum at Daya Bay

DOE PAGES

An, F. P.; Balantekin, A. B.; Band, H. R.; ...

2017-06-19

Here, the Daya Bay experiment has observed correlations between reactor core fuel evolution and changes in the reactor antineutrino flux and energy spectrum. Four antineutrino detectors in two experimental halls were used to identify 2.2 million inverse beta decays (IBDs) over 1230 days spanning multiple fuel cycles for each of six 2.9 GW th reactor cores at the Daya Bay and Ling Ao nuclear power plants. Using detector data spanning effective 239Pu fission fractions F 239 from 0.25 to 0.35, Daya Bay measures an average IBD yield ¯σf of (5.90±0.13)×10 –43 cm 2/fission and a fuel-dependent variation in the IBDmore » yield, dσ f/dF 239, of (–1.86±0.18)×10 –43 cm 2/fission. This observation rejects the hypothesis of a constant antineutrino flux as a function of the 239Pu fission fraction at 10 standard deviations. The variation in IBD yield is found to be energy dependent, rejecting the hypothesis of a constant antineutrino energy spectrum at 5.1 standard deviations. While measurements of the evolution in the IBD spectrum show general agreement with predictions from recent reactor models, the measured evolution in total IBD yield disagrees with recent predictions at 3.1σ. This discrepancy indicates that an overall deficit in the measured flux with respect to predictions does not result from equal fractional deficits from the primary fission isotopes 235U, 239Pu, 238U, and 241Pu. Based on measured IBD yield variations, yields of (6.17±0.17) and (4.27±0.26)×10 –43 cm 2/fission have been determined for the two dominant fission parent isotopes 235U and 239Pu. A 7.8% discrepancy between the observed and predicted 235U yields suggests that this isotope may be the primary contributor to the reactor antineutrino anomaly.« less

Evolution of the Reactor Antineutrino Flux and Spectrum at Daya Bay.

PubMed

An, F P; Balantekin, A B; Band, H R; Bishai, M; Blyth, S; Cao, D; Cao, G F; Cao, J; Chan, Y L; Chang, J F; Chang, Y; Chen, H S; Chen, Q Y; Chen, S M; Chen, Y X; Chen, Y; Cheng, J; Cheng, Z K; Cherwinka, J J; Chu, M C; Chukanov, A; Cummings, J P; Ding, Y Y; Diwan, M V; Dolgareva, M; Dove, J; Dwyer, D A; Edwards, W R; Gill, R; Gonchar, M; Gong, G H; Gong, H; Grassi, M; Gu, W Q; Guo, L; Guo, X H; Guo, Y H; Guo, Z; Hackenburg, R W; Hans, S; He, M; Heeger, K M; Heng, Y K; Higuera, A; Hsiung, Y B; Hu, B Z; Hu, T; Huang, E C; Huang, H X; Huang, X T; Huang, Y B; Huber, P; Huo, W; Hussain, G; Jaffe, D E; Jen, K L; Ji, X P; Ji, X L; Jiao, J B; Johnson, R A; Jones, D; Kang, L; Kettell, S H; Khan, A; Kohn, S; Kramer, M; Kwan, K K; Kwok, M W; Langford, T J; Lau, K; Lebanowski, L; Lee, J; Lee, J H C; Lei, R T; Leitner, R; Leung, J K C; Li, C; Li, D J; Li, F; Li, G S; Li, Q J; Li, S; Li, S C; Li, W D; Li, X N; Li, X Q; Li, Y F; Li, Z B; Liang, H; Lin, C J; Lin, G L; Lin, S; Lin, S K; Lin, Y-C; Ling, J J; Link, J M; Littenberg, L; Littlejohn, B R; Liu, J L; Liu, J C; Loh, C W; Lu, C; Lu, H Q; Lu, J S; Luk, K B; Ma, X Y; Ma, X B; Ma, Y Q; Malyshkin, Y; Martinez Caicedo, D A; McDonald, K T; McKeown, R D; Mitchell, I; Nakajima, Y; Napolitano, J; Naumov, D; Naumova, E; Ngai, H Y; Ochoa-Ricoux, J P; Olshevskiy, A; Pan, H-R; Park, J; Patton, S; Pec, V; Peng, J C; Pinsky, L; Pun, C S J; Qi, F Z; Qi, M; Qian, X; Qiu, R M; Raper, N; Ren, J; Rosero, R; Roskovec, B; Ruan, X C; Steiner, H; Stoler, P; Sun, J L; Tang, W; Taychenachev, D; Treskov, K; Tsang, K V; Tull, C E; Viaux, N; Viren, B; Vorobel, V; Wang, C H; Wang, M; Wang, N Y; Wang, R G; Wang, W; Wang, X; Wang, Y F; Wang, Z; Wang, Z; Wang, Z M; Wei, H Y; Wen, L J; Whisnant, K; White, C G; Whitehead, L; Wise, T; Wong, H L H; Wong, S C F; Worcester, E; Wu, C-H; Wu, Q; Wu, W J; Xia, D M; Xia, J K; Xing, Z Z; Xu, J L; Xu, Y; Xue, T; Yang, C G; Yang, H; Yang, L; Yang, M S; Yang, M T; Yang, Y Z; Ye, M; Ye, Z; Yeh, M; Young, B L; Yu, Z Y; Zeng, S; Zhan, L; Zhang, C; Zhang, C C; Zhang, H H; Zhang, J W; Zhang, Q M; Zhang, R; Zhang, X T; Zhang, Y M; Zhang, Y X; Zhang, Y M; Zhang, Z J; Zhang, Z Y; Zhang, Z P; Zhao, J; Zhou, L; Zhuang, H L; Zou, J H

2017-06-23

The Daya Bay experiment has observed correlations between reactor core fuel evolution and changes in the reactor antineutrino flux and energy spectrum. Four antineutrino detectors in two experimental halls were used to identify 2.2 million inverse beta decays (IBDs) over 1230 days spanning multiple fuel cycles for each of six 2.9 GW_{th} reactor cores at the Daya Bay and Ling Ao nuclear power plants. Using detector data spanning effective ^{239}Pu fission fractions F_{239} from 0.25 to 0.35, Daya Bay measures an average IBD yield σ[over ¯]_{f} of (5.90±0.13)×10^{-43}  cm^{2}/fission and a fuel-dependent variation in the IBD yield, dσ_{f}/dF_{239}, of (-1.86±0.18)×10^{-43}  cm^{2}/fission. This observation rejects the hypothesis of a constant antineutrino flux as a function of the ^{239}Pu fission fraction at 10 standard deviations. The variation in IBD yield is found to be energy dependent, rejecting the hypothesis of a constant antineutrino energy spectrum at 5.1 standard deviations. While measurements of the evolution in the IBD spectrum show general agreement with predictions from recent reactor models, the measured evolution in total IBD yield disagrees with recent predictions at 3.1σ. This discrepancy indicates that an overall deficit in the measured flux with respect to predictions does not result from equal fractional deficits from the primary fission isotopes ^{235}U, ^{239}Pu, ^{238}U, and ^{241}Pu. Based on measured IBD yield variations, yields of (6.17±0.17) and (4.27±0.26)×10^{-43}  cm^{2}/fission have been determined for the two dominant fission parent isotopes ^{235}U and ^{239}Pu. A 7.8% discrepancy between the observed and predicted ^{235}U yields suggests that this isotope may be the primary contributor to the reactor antineutrino anomaly.

Evolution of the Reactor Antineutrino Flux and Spectrum at Daya Bay

NASA Astrophysics Data System (ADS)

An, F. P.; Balantekin, A. B.; Band, H. R.; Bishai, M.; Blyth, S.; Cao, D.; Cao, G. F.; Cao, J.; Chan, Y. L.; Chang, J. F.; Chang, Y.; Chen, H. S.; Chen, Q. Y.; Chen, S. M.; Chen, Y. X.; Chen, Y.; Cheng, J.; Cheng, Z. K.; Cherwinka, J. J.; Chu, M. C.; Chukanov, A.; Cummings, J. P.; Ding, Y. Y.; Diwan, M. V.; Dolgareva, M.; Dove, J.; Dwyer, D. A.; Edwards, W. R.; Gill, R.; Gonchar, M.; Gong, G. H.; Gong, H.; Grassi, M.; Gu, W. Q.; Guo, L.; Guo, X. H.; Guo, Y. H.; Guo, Z.; Hackenburg, R. W.; Hans, S.; He, M.; Heeger, K. M.; Heng, Y. K.; Higuera, A.; Hsiung, Y. B.; Hu, B. Z.; Hu, T.; Huang, E. C.; Huang, H. X.; Huang, X. T.; Huang, Y. B.; Huber, P.; Huo, W.; Hussain, G.; Jaffe, D. E.; Jen, K. L.; Ji, X. P.; Ji, X. L.; Jiao, J. B.; Johnson, R. A.; Jones, D.; Kang, L.; Kettell, S. H.; Khan, A.; Kohn, S.; Kramer, M.; Kwan, K. K.; Kwok, M. W.; Langford, T. J.; Lau, K.; Lebanowski, L.; Lee, J.; Lee, J. H. C.; Lei, R. T.; Leitner, R.; Leung, J. K. C.; Li, C.; Li, D. J.; Li, F.; Li, G. S.; Li, Q. J.; Li, S.; Li, S. C.; Li, W. D.; Li, X. N.; Li, X. Q.; Li, Y. F.; Li, Z. B.; Liang, H.; Lin, C. J.; Lin, G. L.; Lin, S.; Lin, S. K.; Lin, Y.-C.; Ling, J. J.; Link, J. M.; Littenberg, L.; Littlejohn, B. R.; Liu, J. L.; Liu, J. C.; Loh, C. W.; Lu, C.; Lu, H. Q.; Lu, J. S.; Luk, K. B.; Ma, X. Y.; Ma, X. B.; Ma, Y. Q.; Malyshkin, Y.; Martinez Caicedo, D. A.; McDonald, K. T.; McKeown, R. D.; Mitchell, I.; Nakajima, Y.; Napolitano, J.; Naumov, D.; Naumova, E.; Ngai, H. Y.; Ochoa-Ricoux, J. P.; Olshevskiy, A.; Pan, H.-R.; Park, J.; Patton, S.; Pec, V.; Peng, J. C.; Pinsky, L.; Pun, C. S. J.; Qi, F. Z.; Qi, M.; Qian, X.; Qiu, R. M.; Raper, N.; Ren, J.; Rosero, R.; Roskovec, B.; Ruan, X. C.; Steiner, H.; Stoler, P.; Sun, J. L.; Tang, W.; Taychenachev, D.; Treskov, K.; Tsang, K. V.; Tull, C. E.; Viaux, N.; Viren, B.; Vorobel, V.; Wang, C. H.; Wang, M.; Wang, N. Y.; Wang, R. G.; Wang, W.; Wang, X.; Wang, Y. F.; Wang, Z.; Wang, Z.; Wang, Z. M.; Wei, H. Y.; Wen, L. J.; Whisnant, K.; White, C. G.; Whitehead, L.; Wise, T.; Wong, H. L. H.; Wong, S. C. F.; Worcester, E.; Wu, C.-H.; Wu, Q.; Wu, W. J.; Xia, D. M.; Xia, J. K.; Xing, Z. Z.; Xu, J. L.; Xu, Y.; Xue, T.; Yang, C. G.; Yang, H.; Yang, L.; Yang, M. S.; Yang, M. T.; Yang, Y. Z.; Ye, M.; Ye, Z.; Yeh, M.; Young, B. L.; Yu, Z. Y.; Zeng, S.; Zhan, L.; Zhang, C.; Zhang, C. C.; Zhang, H. H.; Zhang, J. W.; Zhang, Q. M.; Zhang, R.; Zhang, X. T.; Zhang, Y. M.; Zhang, Y. X.; Zhang, Y. M.; Zhang, Z. J.; Zhang, Z. Y.; Zhang, Z. P.; Zhao, J.; Zhou, L.; Zhuang, H. L.; Zou, J. H.; Daya Bay Collaboration

2017-06-01

The Daya Bay experiment has observed correlations between reactor core fuel evolution and changes in the reactor antineutrino flux and energy spectrum. Four antineutrino detectors in two experimental halls were used to identify 2.2 million inverse beta decays (IBDs) over 1230 days spanning multiple fuel cycles for each of six 2.9 G Wth reactor cores at the Daya Bay and Ling Ao nuclear power plants. Using detector data spanning effective 239Pu fission fractions F239 from 0.25 to 0.35, Daya Bay measures an average IBD yield σ¯f of (5.90 ±0.13 )×10-43 cm2/fission and a fuel-dependent variation in the IBD yield, d σf/d F239, of (-1.86 ±0.18 )×10-43 cm2/fission . This observation rejects the hypothesis of a constant antineutrino flux as a function of the 239Pu fission fraction at 10 standard deviations. The variation in IBD yield is found to be energy dependent, rejecting the hypothesis of a constant antineutrino energy spectrum at 5.1 standard deviations. While measurements of the evolution in the IBD spectrum show general agreement with predictions from recent reactor models, the measured evolution in total IBD yield disagrees with recent predictions at 3.1 σ . This discrepancy indicates that an overall deficit in the measured flux with respect to predictions does not result from equal fractional deficits from the primary fission isotopes 235U, 239Pu, 238U, and 241Pu. Based on measured IBD yield variations, yields of (6.17 ±0.17 ) and (4.27 ±0.26 )×10-43 cm2 /fission have been determined for the two dominant fission parent isotopes 235U and 239Pu. A 7.8% discrepancy between the observed and predicted 235U yields suggests that this isotope may be the primary contributor to the reactor antineutrino anomaly.

Evolution of the Reactor Antineutrino Flux and Spectrum at Daya Bay

DOE Office of Scientific and Technical Information (OSTI.GOV)

An, F. P.; Balantekin, A. B.; Band, H. R.

Here, the Daya Bay experiment has observed correlations between reactor core fuel evolution and changes in the reactor antineutrino flux and energy spectrum. Four antineutrino detectors in two experimental halls were used to identify 2.2 million inverse beta decays (IBDs) over 1230 days spanning multiple fuel cycles for each of six 2.9 GW th reactor cores at the Daya Bay and Ling Ao nuclear power plants. Using detector data spanning effective 239Pu fission fractions F 239 from 0.25 to 0.35, Daya Bay measures an average IBD yield ¯σf of (5.90±0.13)×10 –43 cm 2/fission and a fuel-dependent variation in the IBDmore » yield, dσ f/dF 239, of (–1.86±0.18)×10 –43 cm 2/fission. This observation rejects the hypothesis of a constant antineutrino flux as a function of the 239Pu fission fraction at 10 standard deviations. The variation in IBD yield is found to be energy dependent, rejecting the hypothesis of a constant antineutrino energy spectrum at 5.1 standard deviations. While measurements of the evolution in the IBD spectrum show general agreement with predictions from recent reactor models, the measured evolution in total IBD yield disagrees with recent predictions at 3.1σ. This discrepancy indicates that an overall deficit in the measured flux with respect to predictions does not result from equal fractional deficits from the primary fission isotopes 235U, 239Pu, 238U, and 241Pu. Based on measured IBD yield variations, yields of (6.17±0.17) and (4.27±0.26)×10 –43 cm 2/fission have been determined for the two dominant fission parent isotopes 235U and 239Pu. A 7.8% discrepancy between the observed and predicted 235U yields suggests that this isotope may be the primary contributor to the reactor antineutrino anomaly.« less

Distinguishing Fissile From Non-Fissile Materials Using Linearly Polarized Gamma Rays

NASA Astrophysics Data System (ADS)

Mueller, J. M.; Ahmed, M. W.; Karwowski, H. J.; Myers, L. S.; Sikora, M. H.; Weller, H. R.; Zimmerman, W. R.; Randrup, J.; Vogt, R.

2014-03-01

Photofission of 232Th, 233 , 235 , 238U, 237Np, and 239,240Pu was induced by nearly 100% linearly polarized, high intensity (~107 γs per second), and nearly-monoenergetic γ-ray beams of energies between 5.3 and 7.6 MeV at the High Intensity γ-ray Source (HI γS). An array of 12-18 liquid scintillating detectors was used to measure prompt fission neutron yields. The ratio of prompt fission neutron yields parallel to the plane of beam polarization to the yields perpendicular to this plane was measured as a function of beam and neutron energy. A ratio near unity was found for 233,235U, 237Np, and 239Pu while a significant ratio (~1.5-3) was found for 232Th, 238U, and 240Pu. This large difference could be used to distinguish fissile isotopes (such as 233,235U and 239Pu) from non-fissile isotopes (such as 232Th, 238U, and 240Pu). The measured ratios agree with the results of a fission calculation (FREYA) which used with previously measured photofission fragment angular distributions as input. Partially supported by DHS (2010-DN-077-ARI046-02), DOE (DE-AC52-07NA27344 and DE-AC02-05CH11231), and the DOE Office of Science Graduate Fellowship Program (DOE SCGF).

Actinide abundances in ordinary chondrites

NASA Technical Reports Server (NTRS)

Hagee, B.; Bernatowicz, T. J.; Podosek, F. A.; Johnson, M. L.; Burnett, D. S.

1990-01-01

Measurements of actinide and light REE (LREE) abundances and of phosphate abundances in equilibrated ordinary chondrites were obtained and were used to define the Pu abundance in the solar system and to determine the degree of variation of actinide and LREE abundances. The results were also used to compare directly the Pu/U ratio with the earlier obtained ratio determined indirectly, as (Pu/Nd)x(Nd/U), assuming that Pu behaves chemically as a LREE. The data, combined with high-accuracy isotope-dilution data from the literature, show that the degree of gram-scale variability of the Th, U, and LREE abundances for equilibrated ordinary chondrites is a factor of 2-3 for absolute abundances and up to 50 percent for relative abundances. The observed variations are interpreted as reflecting the differences in the compositions and/or proportions of solar nebula components accreted to ordinary chondrite parent bodies.

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

DOE PAGES

Lucena, Ana F.; Bandeira, Nuno A. G.; Pereira, Claudia C. L.; ...

2017-01-01

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

Uranium-series constraints on radionuclide transport and groundwater flow at the Nopal I uranium deposit, Sierra Pena Blanca, Mexico.

PubMed

Goldstein, Steven J; Abdel-Fattah, Amr I; Murrell, Michael T; Dobson, Patrick F; Norman, Deborah E; Amato, Ronald S; Nunn, Andrew J

2010-03-01

Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low ( approximately 10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that (230)Th/(238)U activity ratios range from 0.005 to 0.48 and (226)Ra/(238)U activity ratios range from 0.006 to 113. (239)Pu/(238)U mass ratios for the saturated zone are <2 x 10(-14), and Pu mobility in the saturated zone is >1000 times lower than the U mobility. Saturated zone mobility decreases in the order (238)U approximately (226)Ra > (230)Th approximately (239)Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit.

Analysis Of 2H-Evaporator Scale Wall [HTF-13-82] And Pot Bottom [HTF-13-77] Samples

DOE Office of Scientific and Technical Information (OSTI.GOV)

Oji, L. N.

2013-09-11

Savannah River Remediation (SRR) is planning to remove a buildup of sodium aluminosilicate scale from the 2H-evaporator pot by loading and soaking the pot with heated 1.5 M nitric acid solution. Sampling and analysis of the scale material has been performed so that uranium and plutonium isotopic analysis can be input into a Nuclear Criticality Safety Assessment (NCSA) for scale removal by chemical cleaning. Historically, since the operation of the Defense Waste Processing Facility (DWPF), silicon in the DWPF recycle stream combines with aluminum in the typical tank farm supernate to form sodium aluminosilicate scale mineral deposits in the 2H-evaporatormore » pot and gravity drain line. The 2H-evaporator scale samples analyzed by Savannah River National Laboratory (SRNL) came from two different locations within the evaporator pot; the bottom cone sections of the 2H-evaporator pot [Sample HTF-13-77] and the wall 2H-evaporator [sample HTF-13-82]. X-ray diffraction analysis (XRD) confirmed that both the 2H-evaporator pot scale and the wall samples consist of nitrated cancrinite (a crystalline sodium aluminosilicate solid) and clarkeite (a uranium oxyhydroxide mineral). On ''as received'' basis, the bottom pot section scale sample contained an average of 2.59E+00 {+-} 1.40E-01 wt % total uranium with a U-235 enrichment of 6.12E-01 {+-} 1.48E-02 %, while the wall sample contained an average of 4.03E+00 {+-} 9.79E-01 wt % total uranium with a U-235 enrichment of 6.03E-01% {+-} 1.66E-02 wt %. The bottom pot section scale sample analyses results for Pu-238, Pu-239, and Pu-241 are 3.16E-05 {+-} 5.40E-06 wt %, 3.28E-04 {+-} 1.45E-05 wt %, and <8.80E-07 wt %, respectively. The evaporator wall scale samples analysis values for Pu-238, Pu-239, and Pu-241 averages 3.74E-05 {+-} 6.01E-06 wt %, 4.38E-04 {+-} 5.08E-05 wt %, and <1.38E-06 wt %, respectively. The Pu-241 analyses results, as presented, are upper limit values. For these two evaporator scale samples obtained at two different locations within the evaporator pot the major radioactive components (on a mass basis) in the additional radionuclide analyses were Sr-90, Cs-137 Np-237, Pu-239/240 and Th-232. Small quantities of americium and curium were detected in the blanks used for Am/Cm method for these radionuclides. These trace radionuclide amounts are assumed to come from airborne contamination in the shielded cells drying or digestion oven, which has been replaced. Therefore, the Am/Cm results, as presented, may be higher than the true Am/Cm values for these samples. These results are provided so that SRR can calculate the equivalent uranium-235 concentrations for the NCSA. Results confirm that the uranium contained in the scale remains depleted with respect to natural uranium. SRNL did not calculate an equivalent U-235 enrichment, which takes into account other fissionable isotopes U-233, Pu-239 and Pu-241. The applicable method for calculation of equivalent U-235 will be determined in the NCSA. With a few exceptions, a comparison of select radionuclides measurements from this 2013 2H evaporator scale characterization (pot bottom and wall scale samples) with those measurements for the same radionuclides in the 2010 2H evaporator scale analysis shows that the radionuclide analysis for both years are fairly comparable; the analyses results are about the same order of magnitude.« less

Kilauea's Ongoing Eruption: 25th Year Brings Major Changes

NASA Astrophysics Data System (ADS)

Orr, T. R.

2007-12-01

2007 marks the 25th year of nearly continuous eruption on Kilauea's east rift zone. Episodic high lava fountains, which built the Pu`u `O`o cone during the first three years of the eruption, ended in 1986. Activity then migrated downrift and the Kupaianaha shield was formed by passive effusion of lava. The change in eruptive style resulted in a switch at Pu`u `O`o from cone construction to cone collapse that has been ongoing for the last two decades. Activity at Kupaianaha ceased in 1992, and the eruption resumed at Pu`u `O`o. The eruptive style established at Kupaianaha continued, however, with continuous effusion from vents on the southwest flank of the Pu`u `O`o cone. The last 15 years have been characterized by the formation of relatively stable tube systems---broken only by a brief fissure eruption uprift of Pu`u `O`o in 1997---that have carried lava from the flank vents to the ocean about 9 km away. The Prince Kuhio Kalanianaole (PKK) tube, the most recent of these tube systems to develop, was active from March 2004 to June 2007. The PKK flow was emplaced almost entirely on older flows of this eruption and entered the ocean in several locations over a span of 6 km. The "Father's Day" intrusion of June 17--19, 2007, robbed the supply of magma to Pu`u `O`o and, thus, the active flow field. The floor of the Pu`u `O`o crater dropped 80--100 m, the PKK tube system drained, and the active flows and ocean entry quickly stagnated. On June 19, a short-lived fissure eruption broke out low on the east flank of Kane Nui o Hamo, about 6 km uprift of Pu`u `O`o, burying only 0.22 hectares. The eruption at Kilauea paused from June 20 through July 1 or 2, when lava returned to Pu`u `O`o and began refilling the collapsed crater. Near midnight on July 20--21, after at least 19 days of lava lake growth, the lava pond within the Pu`u `O`o crater drained suddenly when a series of fissures opened on the east flank of the cone and propagated ~2 km downrift. The new activity, dubbed the July 21 eruption, initially fed `a`a and pahoehoe flows but, within a few days, developed into a system of perched lava ponds. By the end of July, the perched pond over the easternmost fissure evolved into an open channel feeding a series of `a`a flows heading downrift around the north side of the Kupaianaha shield. The lava supply from other fissure segments declined and stagnated within a few days of the lava channel's formation. As of September 4, 2007, `a`a flows have extended up to ~6 km from the fissure and have covered more than 600 hectares. Unless the eruption supply rate increases, `a`a flows fed by the open channel will likely travel no more than a few kilometers from the vent and pose no threat to those living downslope. If the eruptive style changes, however, to one characterized by tube-fed pahoehoe, then downslope communities could be directly impacted.

Nuclear reactor for breeding U.sup.233

DOEpatents

Bohanan, Charles S.; Jones, David H.; Raab, Jr., Harry F.; Radkowsky, Alvin

1976-01-01

A light-water-cooled nuclear reactor capable of breeding U.sup.233 for use in a light-water breeder reactor includes physically separated regions containing U.sup.235 fissile material and U.sup.238 fertile material and Th.sup.232 fertile material and Pu.sup.239 fissile material, if available. Preferably the U.sup.235 fissile material and U.sup.238 fertile material are contained in longitudinally movable seed regions and the Pu.sup.239 fissile material and Th.sup.232 fertile material are contained in blanket regions surrounding the seed regions.

Multispectral thermal infrared mapping of sulfur dioxide plumes: A case study from the East Rift Zone of Kilauea Volcano, Hawaii

NASA Astrophysics Data System (ADS)

Realmuto, V. J.; Sutton, A. J.; Elias, T.

1997-07-01

The synoptic perspective and rapid mode of data acquisition provided by remote sensing are well suited for the study of volcanic SO2 plumes. In this paper we describe a plume-mapping procedure that is based on image data acquired with NASA's airborne thermal infrared multispectral scanner (TIMS) and apply the procedure to TIMS data collected over the East Rift Zone of Kilauea Volcano, Hawaii, on September 30, 1988. These image data covered the Pu`u `O `o and Kupaianaha vents and a skylight in the lava tube that was draining the Kupaianaha lava pond. Our estimate of the SO2 emission rate from Pu`u `O `o (17-20 kg s-1) is roughly twice the average of estimates derived from correlation spectrometer (COSPEC) measurements collected 10 days prior to the TIMS overflight (10 kg s-1). The agreement between the TIMS and COSPEC results improves when we compare SO2 burden estimates, which are relatively independent of wind speed. We demonstrate the feasibility of mapping Pu`u `O `o - scale SO2 plumes from space in anticipation of the 1998 launch of the advanced spaceborne thermal emission and reflectance radiometer (ASTER).

DFT+U Study of Chemical Impurities in PuO 2

DOE PAGES

Hernandez, Sarah C.; Holby, Edward F.

2016-05-24

In this paper, we employ density functional theory to explore the effects of impurities in the fluorite crystal structure of PuO 2. The impurities that were considered are known impurities that exist in metallic δ-phase Pu, including H, C, Fe, and Ga. These impurities were placed at various high-symmetry sites within the PuO 2 structure including an octahedral interstitial site, an interstitial site with coordination to two neighboring O atoms, an O substitutional site, and a Pu substitutional site. Incorporation energies were calculated to be energetically unfavorable for all sites except the Pu substitutional site. When impurities were placed inmore » a Pu substitutional site, complexes incorporating the impurities and O formed within the PuO 2 structure. The observed defect-oxygen structures were OH, CO 3, FeO 5, and GaO 3. The presence of these defects led to distortion of the surrounding O atoms within the structure, producing long-range disorder of O atoms. In contrast, perturbations of Pu atoms had a relatively short-range effect on the relaxed structures. These effects are demonstrated via radial distribution functions for O and Pu vacancies. Calculated electronic structure revealed hybridization of the impurity atom with the O valence states and a relative decrease in the Pu 5f states. Minor differences in band gaps were observed for the defected PuO 2 structures containing H, C, and Ga. Finally, Fe-containing structures, however, were calculated to have a significantly decreased band gap, where the implementation of a Hubbard U parameter on the Fe 3d orbitals will maintain the calculated PuO 2 band gap.« less

Radionuclide concentrations in benthic invertebrates from Amchitka and Kiska Islands in the Aleutian Chain, Alaska.

PubMed

Burger, Joanna; Gochfeld, Michael; Jewett, Stephen C

2007-05-01

Concentrations of 13 radionuclides (137Cs, 129I, 60Co, 152Eu, 90Sr, 99Tc, 241Am, 238Pu, 239,249Pu, 234U, 235U, 236U, 238U) were examined in seven species of invertebrates from Amchitka and Kiska Islands, in the Aleutian Chain of Alaska, using gamma spectroscopy, inductively coupled plasma mass spectroscopy, and alpha spectroscopy. Amchitka Island was the site of three underground nuclear test (1965-1971), and we tested the null hypotheses that there were no differences in radionuclide concentrations between Amchitka and the reference site (Kiska) and there were no differences among species. The only radionuclides where composite samples were above the Minimum Detectable Activity (MDA) were 137Cs, 241Am, 239,249Pu, 234U, 235U, 236U, and 238U. Green sea urchin (Strongylocentrotus polyacanthus), giant chiton (Cryptochiton stelleri), plate limpets (Tectura scutum) and giant Pacific octopus (Enteroctopus dofleini) were only tested for 137Cs; octopus was the only species with detectable levels of 137Cs (0.262 +/- 0.029 Bq/kg, wet weight). Only rock jingle (Pododesmus macroschisma), blue mussel (Mytilus trossulus) and horse mussel (Modiolus modiolus) were analyzed for the actinides. There were no interspecific differences in 241Am and 239,240Pu, and almost no samples above the MDA for 238Pu and 236U. Horse mussels had significantly higher concentrations of 234U (0.844 +/- 0.804 Bq/kg) and 238U (0.730 +/- 0.646) than the other species (both isotopes are naturally occurring). There were no differences in actinide concentrations between Amchitka and Kiska. In general, radionuclides in invertebrates from Amchitka were similar to those from uncontaminated sites in the Northern Hemisphere, and below those from the contaminated Irish Sea. There is a clear research need for authors to report the concentrations of radionuclides by species, rather than simply as 'shellfish', for comparative purposes in determining geographical patterns, understanding possible effects, and for estimating risk to humans from consuming different biota.

Application of Compton-suppressed self-induced XRF to spent nuclear fuel measurement

NASA Astrophysics Data System (ADS)

Park, Se-Hwan; Jo, Kwang Ho; Lee, Seung Kyu; Seo, Hee; Lee, Chaehun; Won, Byung-Hee; Ahn, Seong-Kyu; Ku, Jeong-Hoe

2017-11-01

Self-induced X-ray fluorescence (XRF) is a technique by which plutonium (Pu) content in spent nuclear fuel can be directly quantified. In the present work, this method successfully measured the plutonium/uranium (Pu/U) peak ratio of a pressurized water reactor (PWR)'s spent nuclear fuel at the Korea atomic energy research institute (KAERI)'s post irradiation examination facility (PIEF). In order to reduce the Compton background in the low-energy X-ray region, the Compton suppression system additionally was implemented. By use of this system, the spectrum's background level was reduced by a factor of approximately 2. This work shows that Compton-suppressed selfinduced XRF can be effectively applied to Pu accounting in spent nuclear fuel.

Uranium and plutonium in anoxic marine sediments of the Santiago River mouth (Eastern Pacific, Mexico).

PubMed

Almazán-Torres, María Guadalupe; Ordóñez-Regil, Eduardo; Ruiz-Fernández, Ana Carolina

2016-11-01

The uranium (U) and plutonium (Pu) content with depth in a sediment core collected in the continental shelf off the mouth of the Santiago River in the Mexican Pacific was studied to evaluate the contamination effects of the effluent of the Santiago-Lerma River as it moves into the sea. The large mass of terrestrial detritus delivered by the river influences the physicochemical and geochemical processes in the seafloor. Abnormal concentrations of U and Pu in sediments were examined as indicative of the effects of anoxic conditions. One of the indicators of pollution of seawater is the bacterial activity of the shallow seabed layer; and among the prevailing bacteria, the magnetotactic ones induce the formation of euhedral and framboidal shapes (pyrite). These pyrite entities are by-products of anoxic environments loaded with decomposing detrital material and are very abundant in the surface layers of the sediment core analyzed. The pyrite formation is the result of a biochemical reaction between iron and organic sulphur reduced by bacteria, and the pyrite entities precipitate to the seafloor. In the same upper zone of the profile, 238 U is readily immobilized, while 234 U is oxidized and dissolved in seawater by the effect of hot atom chemistry. This may cause the activity ratio (AR) 234 U/ 238 U disequilibrium (near 0.41). Furthermore, in the shallow layer of the sediment core, an abnormally high concentration of 239+240 Pu was detected. In this upper layer, the activity concentrations found were 3.19 Bq kg -1 for 238 U, 1.32 kg -1 for 234 U and 2.78 Bq kg -1 for 239+240 Pu. In the lower fractions of the sediment core, normal values of AR 234 U/ 238 U (≈1) were found, with traces of 239+240 Pu. Copyright © 2016 Elsevier Ltd. All rights reserved.

Criticality Safety Controls for 55-Gallon Drums with a Mass Limit of 200 grams Pu-239

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chou, P

The following 200-gram Pu drum criticality safety controls are applicable to RHWM drum storage operations: (1) Mass (Fissile/Pu) - each 55-gallon drum or its equivalent shall be limited to 200 gram Pu or Pu equivalent; (2) Moderation - Hydrogen materials with a hydrogen density greater than that (0.133 g H/cc) of polyethylene and paraffin are not allowed and hydrogen materials with a hydrogen density no greater than that of polyethylene and paraffin are allowed with unlimited amounts; (3) Interaction - a spacing of 30-inches (76 cm) is required between arrays and 200-gram Pu drums shall be placed in arrays formore » 200-gram Pu drums only (no mingling of 200-gram Pu drums with other drums not meeting the drum controls associated with the 200-gram limit); (4) Reflection - no beryllium and carbon/graphite (other than the 50-gram waiver amount) is allowed, (note that Nat-U exceeding the waiver amount is allowed when its U-235 content is included in the fissile mass limit of 200 grams); and (5) Geometry - drum geometry, only 55-gallon drum or its equivalent shall be used and array geometry, 55-gallon drums are allowed for 2-high stacking. Steel waste boxes may be stacked 3-high if constraint.« less

Synthesis, Crystal Chemistry, and Physical Properties of Ternary Intermetallic Compounds An2T2X( An=Pu, Am; X=ln, Sn; T=Co, Ir, Ni, Pd, Pt, Rh)

NASA Astrophysics Data System (ADS)

Pereira, L. C. J.; Wastin, F.; Winand, J. M.; Kanellakopoulos, B.; Rebizant, J.; Spirlet, J. C.; Almeida, M.

1997-11-01

The synthesis, structural, and physical characterization of nine new ternary intermetallic compounds belonging to the isostructural An2T2Xfamily with the transuranium Pu and Am elements, namely, Pu 2Ni 2In, Pu 2Pd 2In, Pu 2Pt 2In, Pu 2Rh 2In, Pu 2Ni 2Sn, Pu 2Pd 2Sn, Pu 2Pt 2Sn, Am 2Ni 2Sn, and Am 2Pd 2Sn, are reported. From these compounds only Pu 2Rh 2In, Am 2Ni 2Sn, and Am 2Pd 2Sn melt incongruently. All of these compounds crystallize in a tetragonal U 3Si 2-type structure, with the space group P4/ mbm, ( Z=2) as most of the U and Np 2-2-1 compounds already found. In this structure, Anatoms occupy the 4 h( x1, x1+0.5, 0.5), Tthe 4 g( x2, x2+0.5, 0), and Xthe 2 a(0, 0, 0) positions. The average values of x1and x2are, respectively, 0.17 and 0.37. Single-crystal X-ray data were refined to R/ RW=0.045/0.066, 0.043/0.072, 0.066/0.080, 0.070/0.098, 0.029/0.048, 0.055/0.080, 0.073/0.096, 0.048/0.086, 0.048/0.065 for Pu 2Ni 2In, Pu 2Pd 2In, Pu 2Pt 2In, Pu 2Rh 2In, Pu 2Ni 2Sn, Pu 2Pd 2Sn, Pu 2Pt 2Sn, Am 2Ni 2Sn, and Am 2Pd 2Sn, respectively, for seven variables. The variation of the lattice parameters and the range of stability of the 2-2-1 phase are discussed in terms of the substitution of different An(actinide), T(transition metal), and X( p-electron) elements in their crystal structure. The possible role of spin fluctuations in the low-temperature behavior of the Pu samples is indicated by magnetic and electrical resistivity measurements.

Unique reversibility in extraction mechanism of U compared to solvent extraction for sorption of U(VI) and Pu(IV) by a novel solvent impregnated resin containing trialkyl phosphine oxide functionalized ionic liquid.

PubMed

Paramanik, M; Panja, S; Dhami, P S; Yadav, J S; Kaushik, C P; Ghosh, S K

2018-07-15

Novel Solvent Impregnated Resin (SIR) material was prepared by impregnating a trialkyl phosphine oxide functionalized ionic liquid (IL) into an inert polymeric material XAD-7. A series of SIR materials were prepared by varying the IL quantity. Sorption of both U(VI) and Pu(IV) were found to increase with increasing IL concentration in SIR up to an optimum IL concentration of 435 mg g -1 of SIR beyond which no effect of IL concentration was observed. A change of mechanism of sorption for U(VI) by SIR was observed in comparison to solvent extraction. The dependency of U(VI) sorption with nitric acid concentration showed a reverse trend compared to solvent extraction studies while for Pu(IV) the trend remained same as observed with solvent extraction. Sorption of both the radionuclides was found to follow pseudo second order mechanism and Langmuir adsorption isotherm. Distribution co-efficient measurements on IL impregnated SIR showed highly selective sorption of U(VI) and Pu(IV) over other trivalent f-elements and fission products from nitric acid medium. Copyright © 2018 Elsevier B.V. All rights reserved.

Electronic-structure theory of plutonium chalcogenides

NASA Astrophysics Data System (ADS)

Shick, Alexander; Havela, Ladislav; Gouder, Thomas; Rebizant, Jean

2009-03-01

The correlated band theory methods, the around-mean-field LDA + U and dynamical LDA + HIA (Hubbard-I), are applied to investigate the electronic structure of Pu chalcogenides. The LDA + U calculations for PuX (X = S, Se, Te) provide non-magnetic ground state in agreement with the experimental data. Non-integer filling of 5 f-manifold (from approx. 5.6 in PuS to 5.7 PuTe). indicates a mixed valence ground state which combines f5 and f6 multiplets. Making use of the dynamical LDA+HIA method the photoelectron spectra are calculated in good agreement with experimental data. The three-peak feature near EF attributed to 5 f-manifold is well reproduced by LDA + HIA, and follows from mixed valence character of the ground state.

Group Constants Generation of the Pseudo Fission Products for Fast Reactor Burnup Calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gil, Choong-Sup; Kim, Do Heon; Chang, Jonghwa

The pseudo fission products for the burnup calculations of the liquid metal fast reactor were generated. The cross-section data and fission product yield data of ENDF/B-VI were used for the pseudo fission product data of U-235, U-238, Pu-239, Pu-240, Pu-241, and Pu-242. The pseudo fission product data can be used with the KAFAX-F22 or -E66, which are the MATXS-format libraries for analyses of the liquid metal fast reactor at KAERI and were distributed through the OECD/NEA. The 80-group MATXS-format libraries of the 172 fission products were generated and the burnup chains for generation of the pseudo fission products were prepared.

Infrasound from the 2007 fissure eruptions of Kīlauea Volcano, Hawai'i

NASA Astrophysics Data System (ADS)

Fee, David; Garces, Milton; Orr, Tim; Poland, Mike

2011-03-01

Varied acoustic signals were recorded at Kīlauea Volcano in mid-2007, coincident with dramatic changes in the volcano's activity. Prior to this time period, Pu'u 'Ō'ō crater produced near-continuous infrasonic tremor and was the primary source of degassing and lava effusion at Kīlauea. Collapse and draining of Pu'u 'Ō'ō crater in mid-June produced impulsive infrasonic signals and fluctuations in infrasonic tremor. Fissure eruptions on 19 June and 21 July were clearly located spatially and temporally using infrasound arrays. The 19 June eruption from a fissure approximately mid-way between Kīlauea's summit and Pu'u 'Ō'ō produced infrasound for ˜30 minutes—the only observed geophysical signal associated with the fissure opening. The infrasound signal from the 21 July eruption just east of Pu'u 'Ō'ō shows a clear azimuthal progression over time, indicative of fissure propagation over 12.9 hours. The total fissure propagation rate is relatively slow at 164 m/hr, although the fissure system ruptured discontinuously. Individual fissure rupture times are estimated using the acoustic data combined with visual observations.

Infrasound from the 2007 fissure eruptions of Kīlauea Volcano, Hawai'i

USGS Publications Warehouse

Fee, D.; Garces, M.; Orr, T.; Poland, M.

2011-01-01

Varied acoustic signals were recorded at Kīlauea Volcano in mid-2007, coincident with dramatic changes in the volcano's activity. Prior to this time period, Pu'u 'Ō'ō crater produced near-continuous infrasonic tremor and was the primary source of degassing and lava effusion at Kīlauea. Collapse and draining of Pu'u 'Ō'ō crater in mid-June produced impulsive infrasonic signals and fluctuations in infrasonic tremor. Fissure eruptions on 19 June and 21 July were clearly located spatially and temporally using infrasound arrays. The 19 June eruption from a fissure approximately mid-way between Kīlauea's summit and Pu'u 'O'o produced infrasound for ~30 minutes-the only observed geophysical signal associated with the fissure opening. The infrasound signal from the 21 July eruption just east of Pu'u 'Ō'ō shows a clear azimuthal progression over time, indicative of fissure propagation over 12.9 hours. The total fissure propagation rate is relatively slow at 164 m/hr, although the fissure system ruptured discontinuously. Individual fissure rupture times are estimated using the acoustic data combined with visual observations.

InSAR observations of deformation associated with new episodes of volcanism at Kilauea Volcano, Hawai'i, 2007

USGS Publications Warehouse

Poland, Michael P.

2008-01-01

In June 2007, the Pu'u 'Ō'ō-Kūpaianaha eruption of Kīlauea Volcano was interrupted when magma intruded the east rift zone (ERZ), resulting in a small extrusion of lava near Makaopuhi Crater. Deformation associated with the activity was exceptionally well-documented by ASAR interferometry, which indicates deflation of the summit and uplift and extension of the ERZ. Models of co-intrusion interferograms suggest that the dike was emplaced in two distinct segments. The modeled volume of the dike greatly exceeds that of the deflation source, raising the possibility that magma from the downrift Pu'u 'Ō'ō vent (dominant extrusion site at Kīlauea since 1983) contributed to the eruption near Makaopuhi, or that the magma that fed the eruption from the summit was compressible. A month following the Makaopuhi eruption, an eruptive fissure opened on the east flank of Pu'u 'Ō'ō. Interferograms, processed within 48 hours of the event, were critical in demonstrating that the magma source feeding the eruption was shallow. The eruption probably resulted from overpressure in Pu'u 'Ō'ō's magmatic system.

Separation of actinides from lanthanides utilizing molten salt electrorefining

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grimmett, D.L.; Fusselman, S.P.; Roy, J.J.

1996-10-01

TRUMP-S (TRansUranic Management through Pyropartitioning Separation) is a pyrochemical process being developed to separate actinides form fission products in nuclear waste. A key process step involving molten salt electrorefining to separate actinides from lanthanides has been studied on a laboratory scale. Electrorefining of U, Np, Pu, Am, and lanthanide mixtures from molten cadmium at 450 C to a solid cathode utilizing a molten chloride electrolyte resulted in > 99% removal of actinides from the molten cadmium and salt phases. Removal of the last few percent of actinides is accompanied by lowered cathodic current efficiency and some lanthanide codeposition. Actinide/lanthanide separationmore » ratios on the cathode are ordered U > Np > Pu > Am and are consistent with predictions based on equilibrium potentials.« less

Results of the Excreta Bioassay Quality Control Program for April 1, 2009 through March 31, 2010

DOE Office of Scientific and Technical Information (OSTI.GOV)

Antonio, Cheryl L.

2012-07-19

A total of 58 urine samples and 10 fecal samples were submitted during the report period (April 1, 2009 through March 31, 2010) to General Engineering Laboratories, South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for Sr, 238Pu, 239Pu, 241Am, 243Am 235U, 238U, elemental uranium and fecal analyses for 241Am, 238Pu and 239Pu were tested this year as well as four tissue samples for 238Pu, 239Pu, 241Am and 241Pu. The number of QC urine samples submitted during the report period represented 1.3% of the total samplesmore » submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 33% of the analyses processed by GEL during the third year of this contract were quality control samples. GEL tested the performance of 21 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty (Table 4).« less

Statistical design and analysis of environmental studies for plutonium and other transuranics at NAEG ''safety-shot'' sites

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gilbert, R.O.; Eberhardt, L.L.; Fowler, E.B.

This paper is centered around the use of stratified random sampling for estimating the total amount (inventory) of $sup 239-240$Pu and uranium in surface soil at ten ''safety-shot'' sites on the Nevada Test Site (NTS) and Tonopah Test Range (TTR) that are currently being studied by the Nevada Applied Ecology Group (NAEG). The use of stratified random sampling has resulted in estimates of inventory at these desert study sites that have smaller standard errors than would have been the case had simple random sampling (no stratification) been used. Estimates of inventory are given for $sup 235$U, $sup 238$U, and $supmore » 239-240$Pu in soil at A Site of Area 11 on the NTS. Other results presented include average concentrations of one or more of these isotopes in soil and vegetation and in soil profile samples at depths to 25 cm. The regression relationship between soil and vegetation concentrations of $sup 235$U and $sup 238$U at adjacent sampling locations is also examined using three different models. The applicability of stratified random sampling to the estimation of concentration contours of $sup 239-240$Pu in surface soil using computer algorithms is also investigated. Estimates of such contours are obtained using several different methods. The planning of field sampling plans for estimating inventory and distribution is discussed. (auth)« less

New approaches for MOX multi-recycling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gain, T.; Bouvier, E.; Grosman, R.

Due to its low fissile content after irradiation, Pu from used MOX fuel is considered by some as not recyclable in LWR (Light Water Reactors). The point of this paper is hence to go back to those statements and provide a new analysis based on AREVA extended experience in the fields of fissile and fertile material management and optimized waste management. This is done using the current US fuel inventory as a case study. MOX Multi-recycling in LWRs is a closed cycle scenario where U and Pu management through reprocessing and recycling leads to a significant reduction of the usedmore » assemblies to be stored. The recycling of Pu in MOX fuel is moreover a way to maintain the self-protection of the Pu-bearing assemblies. With this scenario, Pu content is also reduced repetitively via a multi-recycling of MOX in LWRs. Simultaneously, {sup 238}Pu content decreases. All along this scenario, HLW (High-Level Radioactive Waste) vitrified canisters are produced and planned for deep geological disposal. Contrary to used fuel, HLW vitrified canisters do not contain proliferation materials. Moreover, the reprocessing of used fuel limits the space needed on current interim storage. With MOX multi-recycling in LWR, Pu isotopy needs to be managed carefully all along the scenario. The early introduction of a limited number of SFRs (Sodium Fast Reactors) can therefore be a real asset for the overall system. A few SFRs would be enough to improve the Pu isotopy from used LWR MOX fuel and provide a Pu-isotopy that could be mixed back with multi-recycled Pu from LWRs, hence increasing the Pu multi-recycling potential in LWRs.« less

Heptavalent Neptunium in a Gas-Phase Complex: (Np VIIO 3 +)(NO 3 –) 2

DOE PAGES

Dau, Phuong D.; Maurice, Remi; Renault, Eric; ...

2016-09-15

A central goal of chemistry is to achieve ultimate oxidation states, including in gas-phase complexes with no condensed phase perturbations. In the case of the actinide elements, the highest established oxidation states are labile Pu(VII) and somewhat more stable Np(VII). We have synthesized and characterized gas-phase AnO 3(NO 3) 2- complexes for An = U, Np, and Pu by endothermic NO 2 elimination from AnO 2(NO 3) 3-. It was previously demonstrated that the PuO 3+ core of PuO 3(NO 3) 2- has a Pu—O• radical bond such that the oxidation state is Pu(VI); it follows that in UO 3(NOmore » 3) 2- it is the stable U(VI) oxidation state. On the basis of the relatively more facile synthesis of NpO 3(NO 3) 2-, a Np(VII) oxidation state is inferred. This interpretation is substantiated by reactivity of the three complexes: NO 2 spontaneously adds to UO 3(NO 3) 2- and PuO 3(NO 3) 2- but not to NpO 3(NO 3) 2-. This unreactive character is attributed to a Np(VII)O 3+ core with three stable Np=O bonds, this in contrast to reactive U—O• and Pu—O• radical bonds. The computed structures and reaction energies for the three AnO 3(NO 3) 2- support the conclusion that the oxidation states are U(VI), Np(VII), and Pu(VI). These results establish the extreme Np(VII) oxidation state in a gas-phase complex, and demonstrate the inherently greater stability of Np(VII) versus Pu(VII).« less

Tumorigenic target cell regions in bone marrow studied by localized dosimetry of 239Pu, 241Am and 233U in the mouse femur.

PubMed

Lord, B I; Austin, A L; Ellender, M; Haines, J W; Harrison, J D

2001-06-01

To study the temporal change in microdistribution of plutonium-239, americium-241 and uranium-233 in the mouse distal femur and to compare and combine calculated radiation doses with those obtained previously for the femoral shaft. Also, to relate doses to relative risks of osteosarcoma and acute myeloid leukaemia. Computer-based image analysis of neutron-induced and alpha-track autoradiographs of sections of mouse femora was used to quantify the microdistribution of (239)Pu, (241)Am and (233)U from 1 to 448 days after intraperitoneal injection. Localized dose-rates and cumulative doses over this period were calculated for different regions of the marrow spaces in trabecular bone. The results were then combined with previous data for doses to the cortical marrow of the femoral shaft. A morphometric analysis of the distal femur was carried out. Initial deposition on endosteal surfaces and dose-rates near to the trabecular surfaces at 1 day were two to four times greater than corresponding results for cortical bone. Burial was most rapid for (233)U, about twice the rate in cortical bone. As in cortical bone, subsequent uptake into the marrow was seen for (239)Pu and (241)Am but not (233)U. Cumulative doses to 448 days for different regions of trabecular marrow were greater than corresponding values for cortical marrow for each radionuclide. Combined doses reflected the greater overall volume of cortical marrow. Cumulative radiation doses to the 10 microm thick band of marrow adjacent to all endosteal surfaces were in the ratio of approximately 7:3:1 for (239)Pu:(241)Am:(233)U. This ratio is not inconsistent with observed incidences of osteosarcoma induction by the three nuclides. Analysis of doses to different depths of marrow, however, showed that although ratios were probably not significantly different to that for a 10 microm depth, better correlations with osteosarcomagenic risk were obtained with 20-40 microm depths. For acute myeloid leukaemia, the closest relationship between relative risk and doses was obtained by considering only the central 5-10% of marrow, which gave a dose ratio of approximately 12:11:1 for (239)Pu:(241)Am:(233)U respectively.

Fundamental Chemical Kinetic And Thermodynamic Data For Purex Process Models

DOE Office of Scientific and Technical Information (OSTI.GOV)

Taylor, R.J.; Fox, O.D.; Sarsfield, M.J.

2007-07-01

To support either the continued operations of current reprocessing plants or the development of future fuel processing using hydrometallurgical processes, such as Advanced Purex or UREX type flowsheets, the accurate simulation of Purex solvent extraction is required. In recent years we have developed advanced process modeling capabilities that utilize modern software platforms such as Aspen Custom Modeler and can be run in steady state and dynamic simulations. However, such advanced models of the Purex process require a wide range of fundamental data including all relevant basic chemical kinetic and thermodynamic data for the major species present in the process. Thismore » paper will summarize some of these recent process chemistry studies that underpin our simulation, design and testing of Purex solvent extraction flowsheets. Whilst much kinetic data for actinide redox reactions in nitric acid exists in the literature, the data on reactions in the diluted TBP solvent phase is much rarer. This inhibits the accurate modelization of the Purex process particularly when species show a significant extractability in to the solvent phase or when cycling between solvent and aqueous phases occurs, for example in the reductive stripping of Pu(IV) by ferrous sulfamate in the Magnox reprocessing plant. To support current oxide reprocessing, we have investigated a range of solvent phase reactions: - U(IV)+HNO{sub 3}; - U(IV)+HNO{sub 2}; - U(IV)+HNO{sub 3} (Pu catalysis); - U(IV)+HNO{sub 3} (Tc catalysis); - U(IV)+ Np(VI); - U(IV)+Np(V); - Np(IV)+HNO{sub 3}; - Np(V)+Np(V); Rate equations have been determined for all these reactions and kinetic rate constants and activation energies are now available. Specific features of these reactions in the TBP phase include the roles of water and hydrolyzed intermediates in the reaction mechanisms. In reactions involving Np(V), cation-cation complex formation, which is much more favourable in TBP than in HNO{sub 3}, also occurs and complicates the redox chemistry. Whilst some features of the redox chemistry in TBP appear similar to the corresponding reactions in aqueous HNO{sub 3}, there are notable differences in rates, the forms of the rate equations and mechanisms. Secondly, to underpin the development of advanced single cycle flowsheets using the complexant aceto-hydroxamic acid, we have also characterised in some detail its redox chemistry and solvent extraction behaviour with both Np and Pu ions. We find that simple hydroxamic acids are remarkably rapid reducing agents for Np(VI). They also reduce Pu(VI) and cause a much slower reduction of Pu(IV) through a complex mechanism involving acid hydrolysis of the ligand. AHA is a strong hydrophilic and selective complexant for the tetravalent actinide ions as evidenced by stability constant and solvent extraction data for An(IV), M(III) and U(VI) ions. This has allowed the successful design of U/Pu+Np separation flowsheets suitable for advanced fuel cycles. (authors)« less

Study on Ultra-Long Life,Small U-Zr Metallic Fuelled Core With Burnable Poison

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kenji Tsuji; Hiromitsu Inagaki; Akira Nishikawa

2002-07-01

A conceptual design for a 50 MWe sodium cooled, U-Pu-Zr metallic fuelled, fast reactor core, which aims at a core lifetime of 30 years, has been performed [1]. As for the compensation for a large burn-up reactivity through 30 years, an axially movable reflector, which is located around the core, carries the major part of it and a burnable poison does the rest. This concept has achieved not only a long core lifetime but also a high discharged burn-up. On this study, a conceptual design for a small fast reactor loading U-Zr metallic fuelled core instead of U-Pu-Zr fuelled coremore » has been conducted, based on the original core arrangement of 4S reactor [2]. Within the range of this study including safety requirements, adopting the burnable poison would be effective to construct a core concept that achieves both a long lifetime and a high discharged burn-up. (authors)« less

Phase equilibria in the UO 2-PuO 2 system under a temperature gradient

NASA Astrophysics Data System (ADS)

Kleykamp, Heiko

2001-04-01

The phase behaviour of U 0.80Pu 0.20O 1.95 was investigated under a steady-state temperature gradient between the solidus and liquidus by a short-time power-to-melt irradiation experiment. The radial U, Pu, Am and O profiles in the fuel pin after redistribution were measured by X-ray microanalysis. During irradiation, an inner fuel melt forms which is separated from the outer solid only by one concentric liquid-solid-phase boundary. The UO 2 concentration increases to 85% and the PuO 2 concentration decreases to 15% on the solid side of the interface. Opposite gradients occur on the liquid side of the interface. The concentration discontinuity is a consequence of the necessary equality of the chemical potentials of UO 2 and PuO 2 on both sides of the phase boundary which corresponds to a 2750°C isotherm. The radial oxygen profile results in an O/(U + Pu) ratio of 2.00 at the fuel surface and 1.92 at the central void of the fuel. The redistribution is caused by the thermal diffusion of oxygen vacancies in the lattice along the temperature gradient. This process is quantified by the heat of transport Q*v which ranges between -10 kJ/mol at the central void and about -230 kJ/mol near the fuel surface.

Nature of local magma storage zones and geometry of conduit systems below balsatic eruption sites - Pu'u 'O'o, Kilauea East Rift, Hawaii, example

NASA Technical Reports Server (NTRS)

Wilson, Lionel; Head, James W., III

1988-01-01

The fluid dynamics of the well-documented eruptive episodes at Pu'u 'O'o, Kilauea are used to investigate quantitatively the size and shape of the shallow conduit system beneath the vent. The possible geometry of this region is considered. The dynamics of the eruptive episodes is used to place restrictions on the size and shape of the region and thermal calculations are used to show that the geometry is consistent with the region being the fluid residue of the partially cooled, major preepisode 1 dike. The Pu'u 'O'o example is used to illustrate some general properties of shallow magma storage zones.

Space and Time Distribution of Pu Isotopes inside The First Experimental Fuel Pin Designed for PWR and Manufactured in Indonesia

NASA Astrophysics Data System (ADS)

Suwardi; Setiawan, J.; Susilo, J.

2017-01-01

The first short fuel pin containing natural UO2 pellet in Zry4 cladding has been prepared and planned to be tested in power ramp irradiation. An irradiation test should be designed to allow an experiment can be performed safely and giving maximum results of many performance aspects of design and manufacturing. Performance analysis to the fuel specimen shows that the specimen is not match to be used for power ramp testing. Enlargement by 0.20 mm of pellet diameter has been proposed. The present work is evaluation of modified design for important aspect of isotopic Pu distribution during irradiation test, because generated Pu isotopes in natural UO2 fuel, contribute more power relative to the contribution by enriched UO2 fuel. The axial profile of neutrons flux have been chosen from both experimental measurement and model calculation. The parameters of ramp power has been obtained from statistical experiment data. A simplified and typical base-load commercial PHWR profile of LHR history has been chosen, to determine the minimum irradiation time before ramp test can be performed. The data design and Mat pro XI materials properties models have been chosen. The axial profile of neutrons flux has been accommodated by 5 slices of discrete pin. The Pu distribution of slice-4 with highest power rate has been chosen to be evaluated. The radial discretion of pellet and cladding and numerical parameter have been used the default best practice of TU. The results shows that Pu 239 increased rapidly. The maximum burn up of slice 4 at upper the median slice, it reached nearly 90% of maximum value at about 6000 h with peak of 0.8%a Pu/HM at 22000 h, which is higher than initial U 235. Each 240, 241 and 240 Pu grows slower and ends up to 0.4, 0.2 and 0.18 % respectively. This results can be used for verification of other aspect of fuel behavior in the modeling results and also can be used as guide and comparison to the future post irradiation examination for Pu isotopes distribution.

A thermodynamic approach for advanced fuels of gas-cooled reactors

NASA Astrophysics Data System (ADS)

Guéneau, C.; Chatain, S.; Gossé, S.; Rado, C.; Rapaud, O.; Lechelle, J.; Dumas, J. C.; Chatillon, C.

2005-09-01

For both high temperature reactor (HTR) and gas cooled fast reactor (GFR) systems, the high operating temperature in normal and accidental conditions necessitates the assessment of the thermodynamic data and associated phase diagrams for the complex system constituted of the fuel kernel, the inert materials and the fission products. A classical CALPHAD approach, coupling experiments and thermodynamic calculations, is proposed. Some examples of studies are presented leading with the CO and CO 2 gas formation during the chemical interaction of [UO 2± x/C] in the HTR particle, and the chemical compatibility of the couples [UN/SiC], [(U, Pu)N/SiC], [(U, Pu)N/TiN] for the GFR system. A project of constitution of a thermodynamic database for advanced fuels of gas-cooled reactors is proposed.

Gas-Phase Coordination Complexes of UVIO{2/2+}, NpVIO{2/2+}, and PuVIO{2/2+} with Dimethylformamide

NASA Astrophysics Data System (ADS)

Rutkowski, Philip X.; Rios, Daniel; Gibson, John K.; van Stipdonk, Michael J.

2011-11-01

Electrospray ionization of actinyl perchlorate solutions in H2O with 5% by volume of dimethylformamide (DMF) produced the isolatable gas-phase complexes, [AnVIO2(DMF)3(H2O)]2+ and [AnVIO2(DMF)4]2+, where An = U, Np, and Pu. Collision-induced dissociation confirmed the composition of the dipositive coordination complexes, and produced doubly- and singly-charged fragment ions. The fragmentation products reveal differences in underlying chemistries of uranyl, neptunyl, and plutonyl, including the lower stability of Np(VI) and Pu(VI) compared with U(VI).

Player-Driven Video Analysis to Enhance Reflective Soccer Practice in Talent Development

ERIC Educational Resources Information Center

Hjort, Anders; Henriksen, Kristoffer; Elbæk, Lars

2018-01-01

In the present article, we investigate the introduction of a cloud-based video analysis platform called Player Universe (PU). Video analysis is not a new performance-enhancing element in sports, but PU is innovative in how it facilitates reflective learning. Video analysis is executed in the PU platform by involving the players in the analysis…

Search for electron and gamma-ray decay of the ^238fPu fission

NASA Astrophysics Data System (ADS)

Beausang, C. W.; Gurdal, G.; Ressler, J.; Barton, C. J.; Caprio, M. A.; Casten, R. F.; Cooper, J. R.; Hecht, A. A.; Hutter, C.; Zamfir, N. V.; Hauschild, K.; Korten, W.; Mergel, E.

2002-04-01

The reaction ^9Be + ^232Th arrow ^241Pu, at beam energies of 50 and 55 MeV, was used in an attempt to populate states in the second minimum (fission isomer) of ^238Pu via the 3n evaporation channel. Prompt gamma-rays, detected using YRAST Ball and conversion electrons, detected using ICE Ball, were collected in coincidence with delayed fission events measured using elements of the Yale SCARY array of solar cell detectors. The solar cell detectors were shielded so as not to view the large prompt fission flux from the target. Instead the detectors were located so that they could detect delayed fission events, originating from the 6 ns fission isomer state in ^238Pu, which occur downstream from the target position. Data analysis is in progress and results to date will be presented. This work is partly supported by the U.S. DOE under grant numbers DE-FG02-91ER-40609, DE-FG02-88ER-40417.

Lightweight, compressible and electrically conductive polyurethane sponges coated with synergistic multiwalled carbon nanotubes and graphene for piezoresistive sensors.

PubMed

Ma, Zhonglei; Wei, Ajing; Ma, Jianzhong; Shao, Liang; Jiang, Huie; Dong, Diandian; Ji, Zhanyou; Wang, Qian; Kang, Songlei

2018-04-19

Lightweight, compressible and highly sensitive pressure/strain sensing materials are highly desirable for the development of health monitoring, wearable devices and artificial intelligence. Herein, a very simple, low-cost and solution-based approach is presented to fabricate versatile piezoresistive sensors based on conductive polyurethane (PU) sponges coated with synergistic multiwalled carbon nanotubes (MWCNTs) and graphene. These sensor materials are fabricated by convenient dip-coating layer-by-layer (LBL) electrostatic assembly followed by in situ reduction without using any complicated microfabrication processes. The resultant conductive MWCNT/RGO@PU sponges exhibit very low densities (0.027-0.064 g cm-3), outstanding compressibility (up to 75%) and high electrical conductivity benefiting from the porous PU sponges and synergistic conductive MWCNT/RGO structures. In addition, the MWCNT/RGO@PU sponges present larger relative resistance changes and superior sensing performances under external applied pressures (0-5.6 kPa) and a wide range of strains (0-75%) compared with the RGO@PU and MWCNT@PU sponges, due to the synergistic effect of multiple mechanisms: "disconnect-connect" transition of nanogaps, microcracks and fractured skeletons at low compression strain and compressive contact of the conductive skeletons at high compression strain. The electrical and piezoresistive properties of MWCNT/RGO@PU sponges are strongly associated with the dip-coating cycle, suspension concentration, and the applied pressure and strain. Fully functional applications of MWCNT/RGO@PU sponge-based piezoresistive sensors in lighting LED lamps and detecting human body movements are demonstrated, indicating their excellent potential for emerging applications such as health monitoring, wearable devices and artificial intelligence.

Volcanology Curricula Development Aided by Online Educational Resource

NASA Astrophysics Data System (ADS)

Poland, Michael P.; van der Hoeven Kraft, Katrien J.; Teasdale, Rachel

2011-03-01

Using On-Line Volcano Monitoring Data in College and University Courses: The Volcano Exploration Project: Pu`u `Ō`ō (VEPP); Hawaii Volcanoes National Park, Hawaii, 26-30 July 2010; Volcanic activity is an excellent hook for engaging college and university students in geoscience classes. An increasing number of Internet-accessible real-time and near-real time volcano monitoring data are now available and constitute an important resource for geoscience education; however, relatively few data sets are comprehensive, and many lack background information to aid in interpretation. In response to the need for organized, accessible, and well-documented volcano education resources, the U.S. Geological Survey's Hawaiian Volcano Observatory (HVO), in collaboration with NASA and the University of Hawai`i at Manoa, established the Volcanoes Exploration Project: Pu`u `Ō`ō (VEPP). The VEPP Web site (http://vepp.wr.usgs.gov) is an educational resource that provides access, in near real time, to geodetic, seismic, and geologic data from the active Pu`u `Ō`ō eruptive vent on Kilauea volcano, Hawaii, along with background and context information. A strength of the VEPP site is the common theme of the Pu`u `Ō`ō eruption, which allows the site to be revisited multiple times to demonstrate different principles and integrate many aspects of volcanology.

Volcanology curricula development aided by online educational resource

USGS Publications Warehouse

Poland, Michael P.; Van Der Hoeven, Kraft; Teasdale, R.

2011-01-01

Using On-Line Volcano Monitoring Data in College and University Courses: The Volcano Exploration Project: Pu`u `Ō`ō (VEPP); Hawaii Volcanoes National Park, Hawaii, 26–30 July 2010; Volcanic activity is an excellent hook for engaging college and university students in geoscience classes. An increasing number of Internet-accessible real-time and near–real time volcano monitoring data are now available and constitute an important resource for geoscience education; however, relatively few data sets are comprehensive, and many lack background information to aid in interpretation. In response to the need for organized, accessible, and well-documented volcano education resources, the U.S. Geological Survey's Hawaiian Volcano Observatory (HVO), in collaboration with NASA and the University of Hawai`i at Manoa, established the Volcanoes Exploration Project: Pu`u `Ō`ō (VEPP). The VEPP Web site (http://vepp.wr.usgs.gov) is an educational resource that provides access, in near real time, to geodetic, seismic, and geologic data from the active Pu`u `Ō`ō eruptive vent on Kilauea volcano, Hawaii, along with background and context information. A strength of the VEPP site is the common theme of the Pu`u `Ō`ō eruption, which allows the site to be revisited multiple times to demonstrate different principles and integrate many aspects of volcanology.

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

NASA Astrophysics Data System (ADS)

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

2010-12-01

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

Multispectral thermal infrared mapping of sulfur dioxide plumes: A case study from the East Rift Zone of Kilauea Volcano, Hawaii

USGS Publications Warehouse

Realmuto, V.J.; Sutton, A.J.; Elias, T.

1997-01-01

The synoptic perspective and rapid mode of data acquisition provided by remote sensing are well suited for the study of volcanic SO2 plumes. In this paper we describe a plume-mapping procedure that is based on image data acquired with NASA's airborne thermal infrared multispectral scanner (TIMS) and apply the procedure to TIMS data collected over the East Rift Zone of Kilauea Volcano, Hawaii, on September 30, 1988. These image data covered the Pu'u 'O'o and Kupaianaha vents and a skylight in the lava tube that was draining the Kupaianaha lava pond. Our estimate of the SO2 emission rate from Pu'u 'O'o (17 - 20 kg s-1) is roughly twice the average of estimates derived from correlation spectrometer (COSPEC) measurements collected 10 days prior to the TIMS overflight (10 kg s-1). The agreement between the TIMS and COSPEC results improves when we compare SO2 burden estimates, which are relatively independent of wind speed. We demonstrate the feasibility of mapping Pu'u 'O'o - scale SO2 plumes from space in anticipation of the 1998 launch of the advanced spaceborne thermal emission and reflectance radiometer (ASTER). Copyright 1997 by the American Geophysical Union.

Prospects for improved understanding of isotopic reactor antineutrino fluxes

NASA Astrophysics Data System (ADS)

Gebre, Y.; Littlejohn, B. R.; Surukuchi, P. T.

2018-01-01

Predictions of antineutrino fluxes produced by fission isotopes in a nuclear reactor have recently received increased scrutiny due to observed differences in predicted and measured inverse beta decay (IBD) yields, referred to as the "reactor antineutrino flux anomaly." In this paper, global fits are applied to existing IBD yield measurements to produce constraints on antineutrino production by individual plutonium and uranium fission isotopes. We find that fits including measurements from highly U 235 -enriched cores and fits including Daya Bay's new fuel evolution result produce discrepant best-fit IBD yields for U 235 and Pu 239 . This discrepancy can be alleviated in a global analysis of all data sets through simultaneous fitting of Pu 239 , U 235 , and U 238 yields. The measured IBD yield of U 238 in this analysis is (7.02 ±1.65 )×10-43 cm2/fission , nearly two standard deviations below existing predictions. Future hypothetical IBD yield measurements by short-baseline reactor experiments are examined to determine their possible impact on the global understanding of isotopic IBD yields. It is found that future improved short-baseline IBD yield measurements at both high-enriched and low-enriched cores can significantly improve constraints for U 235 , U 238 , and Pu 239 , providing comparable or superior precision to existing conversion- and summation-based antineutrino flux predictions. Systematic and experimental requirements for these future measurements are also investigated.

A fast semi-quantitative method for Plutonium determination in an alpine firn/ice core

NASA Astrophysics Data System (ADS)

Gabrieli, J.; Cozzi, G.; Vallelonga, P.; Schwikowski, M.; Sigl, M.; Boutron, C.; Barbante, C.

2009-04-01

Plutonium is present in the environment as a consequence of atmospheric nuclear tests carried out in the 1960s, nuclear weapons production and releases by the nuclear industry over the past 50 years. Plutonium, unlike uranium, is essentially anthropogenic and it was first produced and isolated in 1940 by deuteron bombardment of uranium in the cyclotron of Berkeley University. It exists in five main isotopes, 238Pu, 239Pu, 240Pu, 241Pu, 242Pu, derived from civilian and military sources (weapons production and detonation, nuclear reactors, nuclear accidents). In the environment, 239Pu is the most abundant isotope. Approximately 6 tons of 239Pu have been released into the environment as a result of 541 atmospheric weapon tests Nuclear Pu fallout has been studied in various environmental archives, such as sediments, soil and herbarium grass. Mid-latitude ice cores have been studied as well, on Mont Blanc, the Western Alps and on Belukha Glacier, Siberian Altai. We present a Pu record obtained by analyzing 52 discrete samples of an alpine firn/ice core from Colle Gnifetti (M. Rosa, 4450 m a.s.l.), dating from 1945 to 1991. The239Pu signal was recorded directly, without preliminary cleaning or preconcentration steps, using an ICP-SFMS (Thermo Element2) equipped with a desolvation system (APEX). 238UH+ interferences were negligible for U concentrations lower than 50 ppt as verified both in spiked fresh snow and pre-1940 ice samples. The shape of 239Pu profile reflects the three main periods of atmospheric nuclear weapons testing: the earliest peak starts in 1954/55 to 1958 and includes the first testing period which reached a maximum in 1958. Despite a temporary halt in testing in 1959/60, the Pu concentration decreased only by half with respect to the 1958 peak. In 1961/62 Pu concentrations rapidly increased reaching a maximum in 1963, which was about 40% more intense than the 1958 peak. After the sign of the "Limited Test Ban Treaty" between USA and URSS in 1964, Pu deposition decreased very sharply reaching a minimum in 1967. The third period (1967-1975) is characterized by irregular Pu profiles with smaller peaks (about 20-30% compared to the 1964 peak) which could be due to French and Chinese tests. Comparison with the Pu profiles obtained from the Col du Dome and Belukha ice cores by AMS (Accelerator Mass Spectrometry) shows very good agreement. Considering the semi-quantitative method and the analytical uncertainty, the results are also quantitatively comparable. However, the Pu concentrations at Colle Gnifetti are normally 2-3 times greater than in Col du Dome. This could be explained by different air mass transport or, more likely, different accumulation rates at each site.

Hydrologic Resources Management Program and Underground Test Area Project FY 2006 Progress Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Culham, H W; Eaton, G F; Genetti, V

2008-04-08

This report describes FY 2006 technical studies conducted by the Chemical Biology and Nuclear Science Division (CBND) at Lawrence Livermore National Laboratory (LLNL) in support of the Hydrologic Resources Management Program (HRMP) and the Underground Test Area Project (UGTA). These programs are administered by the U.S. Department of Energy, National Nuclear Security Administration, Nevada Site Office (NNSA/NSO) through the Defense Programs and Environmental Restoration Divisions, respectively. HRMP-sponsored work is directed toward the responsible management of the natural resources at the Nevada Test Site (NTS), enabling its continued use as a staging area for strategic operations in support of national security.more » UGTA-funded work emphasizes the development of an integrated set of groundwater flow and contaminant transport models to predict the extent of radionuclide migration from underground nuclear testing areas at the NTS. The report is organized on a topical basis and contains four chapters that highlight technical work products produced by CBND. However, it is important to recognize that most of this work involves collaborative partnerships with the other HRMP and UGTA contract organizations. These groups include the Energy and Environment Directorate at LLNL (LLNL-E&E), Los Alamos National Laboratory (LANL), the Desert Research Institute (DRI), the U.S. Geological Survey (USGS), Stoller-Navarro Joint Venture (SNJV), and National Security Technologies (NSTec). Chapter 1 is a summary of FY 2006 sampling efforts at near-field 'hot' wells at the NTS, and presents new chemical and isotopic data for groundwater samples from four near-field wells. These include PM-2 and U-20n PS 1DDh (CHESHIRE), UE-7ns (BOURBON), and U-19v PS No.1ds (ALMENDRO). Chapter 2 is a summary of the results of chemical and isotopic measurements of groundwater samples from three UGTA environmental monitoring wells. These wells are: ER-12-4 and U12S located in Area 12 on Rainier Mesa and USGS HGH No.2 WW2 located in Yucca Flat. In addition, three springs were sampled White Rock Spring and Captain Jack Spring in Area 12 on Rainier Mesa and Topopah Spring in Area 29. Chapter 3 is a compilation of existing noble gas data that has been reviewed and edited to remove inconsistencies in presentation of total vs. single isotope noble gas values reported in the previous HRMP and UGTA progress reports. Chapter 4 is a summary of the results of batch sorption and desorption experiments performed to determine the distribution coefficients (Kd) of Pu(IV), Np(V), U(VI), Cs and Sr to zeolitized tuff (tuff confining unit, TCU) and carbonate (lower carbonate aquifer, LCA) rocks in synthetic NTS groundwater Chapter 5 is a summary of the results of a series of flow-cell experiments performed to examine Np(V) and Pu(V) sorption to and desorption from goethite. Np and Pu desorption occur at a faster rate and to a greater extent than previously reported. In addition, oxidation changes occurred with the Pu whereby the surface-sorbed Pu(IV) was reoxidized to aqueous Pu(V) during desorption.« less

Extinct 244Pu in ancient zircons.

PubMed

Turner, Grenville; Harrison, T Mark; Holland, Greg; Mojzsis, Stephen J; Gilmour, Jamie

2004-10-01

We have found evidence, in the form of fissiogenic xenon isotopes, for in situ decay of 244Pu in individual 4.1- to 4.2-billion-year-old zircons from the Jack Hills region of Western Australia. Because of its short half-life, 82 million years, 244Pu was extinct within 600 million years of Earth's formation. Detrital zircons are the only known relics to have survived from this period, and a study of their Pu geochemistry will allow us to date ancient metamorphic events and determine the terrestrial Pu/U ratio for comparison with the solar ratio.

The chemical state of defective uranium-plutonium oxide fuel pins irradiated in sodium cooled reactors

NASA Astrophysics Data System (ADS)

Kleykamp, H.

1997-09-01

Steady-state irradiation experiments were conducted in the sodium loop of the Siloe reactor on artificially failed mixed oxide pins that had been pre-irradiated in fast reactors up to 11.5% burnup. The formation of the predominant reaction product Na 3(U,Pu)O 4 starts on the fuel surface and is terminated when a lower O/(U + Pu) threshold of the fuel is attained. The axial extent of the reaction product depends on the size of the initial cladding defect. The occurrence of secondary cracks is possible. Na(U,Pu)O 3 forms at higher fuel temperatures. The existence of Na 3U 1- xPu xO 4 is shown in pre-irradiated blanket pins after artificial defect formation. Caesium in the oxocompounds is reduced to the metallic state and is dissolved in the coolant. Evidence of a very low chemical potential of oxygen in defective fuel pins is sustained by the occurrence of actinide-platinum metal phases formed by coupled reduction of hypostoichiometric fuel with ɛ-(Mo,Tc,Ru,Rh,Pd) precipitates. Continued operation of defective pins is not hazardous by easy precautions.

Evaluation of different methods for immobilization of Candida antarctica lipase B (CalB lipase) in polyurethane foam and its application in the production of geranyl propionate.

PubMed

Nicoletti, Gabrieli; Cipolatti, Eliane P; Valério, Alexsandra; Carbonera, NatáliaThaisa Gamba; Soares, Nicole Spillere; Theilacker, Eron; Ninow, Jorge L; de Oliveira, Débora

2015-09-01

With the aim of studying the best method for the interaction of polyurethane (PU) foam and Candida antarctica lipase B, different methods of CalB immobilization were studied: adsorption (PU-ADS), bond (using polyethyleneimine) (PU-PEI), ionic adsorption by PEI with cross-linking with glutaraldehyde (PU-PEI-GA) and entrapment (PU). The characterization of immobilized enzyme derivatives was performed by apparent density and Fourier transform infrared spectroscopy. The free enzyme and enzyme preparations were evaluated at different pH values and temperatures. The highest enzyme activity was obtained using the PU method (5.52 U/g). The methods that stood out to compare the stabilities and kinetic parameters were the PU and PU-ADS. Conversions of 83.5 and 95.9 % for PU and PU-ADS derivatives were obtained, in 24 h reaction, using citronella oil and propionic acid as substrates.

Supercritical fluid extraction and separation of uranium from other actinides.

PubMed

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

2014-06-15

The feasibility of separating U from nitric acid solutions of mixed actinides using tri-n-butylphosphate (TBP)-modified supercritical fluid carbon dioxide (sc-CO2) was investigated. The actinides U, Np, Pu, and Am were extracted into sc-CO2 modified with TBP from a range of nitric acid concentrations, in the absence of, or in the presence of, a number of traditional reducing and/or complexing agents to demonstrate the separation of these metals from U under sc-CO2 conditions. The separation of U from Pu using sc-CO2 was successful at nitric acid concentrations of less than 3M in the presence of acetohydroxamic acid (AHA) or oxalic acid (OA) to mitigate Pu extraction, and the separation of U from Np was successful at nitric acid concentrations of less than 1M in the presence of AHA, OA, or sodium nitrite to mitigate Np extraction. Americium was not well extracted under any condition studied. Copyright © 2014 Elsevier B.V. All rights reserved.

ORNL Resolved Resonance Covariance Generation for ENDF/B-VII.1

DOE Office of Scientific and Technical Information (OSTI.GOV)

Leal, Luiz C.; Guber, Klaus H.; Wiarda, Dorothea

2012-12-01

Resonance-parameter covariance matrix (RPCM) evaluations in the resolved resonance regionwere done at the Oak Ridge National Laboratory (ORNL) for the chromium isotopes, titanium isotopes, 19F, 58Ni, 60Ni, 35Cl, 37Cl, 39K, 41K, 55Mn, 233U, 235U, 238U, and 239Pu using the computer code SAMMY. The retroactive approach of the code SAMMY was used to generate the RPCMs for 233U. For 235U, the approach used for covariance generation was similar to the retroactive approach with the distinction that real experimental data were used as opposed to data generated from the resonance parameters. RPCMs for 238U and 239Pu were generated together with the resonancemore » parameter evaluations. The RPCMs were then converted in the ENDF format using the FILE32 representation. Alternatively, for computer storage reasons, the FILE32 was converted in the FILE33 cross section covariance matrix (CSCM). Both representations were processed using the computer code PUFF-IV. This paper describes the procedures used to generate the RPCM and CSCM in the resonance region for ENDF/B-VII.1. The impact of data uncertainty in nuclear reactor benchmark calculations is also presented.« less

Evidence from Xenon isotopes for limited mixing between MORB sources and plume sources since 4.45 Ga

NASA Astrophysics Data System (ADS)

Mukhopadhyay, S.

2011-12-01

Xenon isotopes provide unique insights into the sources of volatile material for planet Earth, the degassing of the mantle, and the chemical evolution of the mantle [1-4]. 129Xe is produced from 129I, which has a half-life of 16 Myrs, and 131-136Xe are produced from 244Pu, which has a half-life of 80 Myrs. To a smaller extent, 131-136Xe are also produced from 238U fission. Thus, ratios of Pu-derived to U-derived fission xenon and 129I-derived to Pu-derived fission xenon constrain the rate and degree of outgassing of a mantle reservoir. Here, I report on the Pu-derived to U-derived fission xenon and Pu/I ratio of the Iceland plume. I then compare the plume observations with the gas rich popping rock from the North Mid Atlantic Ridge that samples the upper mantle [4]. Through step crushing of multiple aliquots of a basalt glass from Iceland, 51 high-precision He, Ne, Ar, and Xe isotopic compositions were generated. Combined He, Ne, and Xe measurements provide unequivocal evidence that the Iceland plume has a lower 129Xe/130Xe ratio than MORBs because it evolved with a I/Xe ratio distinct from the MORB source and not because of recycled atmosphere (which has low 129Xe/130Xe) in the plume source. Since 129I became extinct 80 Myrs after solar system formation, limited mixing between plume and MORB source is a stringent requirement since 4.45 Ga. Of the 51 different isotopic analyses, 42 data points were distinct from the atmospheric 129Xe/130Xe composition at two standard deviations. These 42 data points were utilized to calculate the ratio of Pu- to U-derived fission xenon. The starting composition of terrestrial Xe is a matter of debate. However, for reasonable starting compositions of air, non-radiogenic atmosphere, solar wind, and U-Xe [5-7], the Iceland plume ,on average, has approximately a factor of two higher Pu-derived xenon than the MORB source. These data thus, provide unequivocal evidence that the Iceland plume is less degassed than the MORB source and that the differences must have existed early on because Pu becomes extinct after ~ 400 Myrs. Thus, the Xe isotopic data suggests that differences between plume and MORB sources are the result of different mantle processing rates and not related to the preferential recycling of atmospheric gases into the plume source. Furthermore, if the plumes are derived from the large low shear wave velocity (LLSVPs) provinces at the base of the lower mantle [8], then our results require that LLSVPs are not made of solely recycled material. Rather, primitive material must constitute some fraction of the LLSVPs, and LLSVPs are ancient, having persisted through most of Earth's history. [1] Holland and Ballentine, Nature, 2006. [2] Yokochi and Marty, EPSL, 2004. [3] Coltice et al., Chem Geol., 2009. [4] Moriera et al., Science, 1998. [5] Caffee et al., Science, 1998. [6] Kunz et al., Science 1998. [7] Pepin and Porcelli, EPSL, 2006. [8] Torsvik et al., Nature, 2010.

Study of hot thermally fissile nuclei using relativistic mean field theory

NASA Astrophysics Data System (ADS)

Quddus, Abdul; Naik, K. C.; Patra, S. K.

2018-07-01

We have studied the properties of hot 234,236U and 240Pu nuclei in the framework of relativistic mean field formalism. The recently developed FSUGarnet and IOPB-I parameter sets are implemented for the first time to deform nuclei at finite temperature. The results are compared with the well known NL3 set. The said isotopes are structurally important because of the thermally fissile nature of 233,235U and 239Pu as these nuclei (234,236U and 240Pu) are formed after the absorption of a thermal neutron, which undergoes fission. Here, we have evaluated the nuclear properties, such as shell correction energy, neutron-skin thickness, quadrupole and hexadecapole deformation parameters and asymmetry energy coefficient for these nuclei as a function of temperature.

Future research program on prompt γ-ray emission in nuclear fission

NASA Astrophysics Data System (ADS)

Oberstedt, S.; Billnert, R.; Hambsch, F.-J.; Lebois, M.; Oberstedt, A.; Wilson, J. N.

2015-12-01

In recent years the measurement of prompt fission γ-ray spectra (PFGS) has gained renewed interest, after about forty years since the first comprehensive studies of the reactions 235U(n th , f), 239Pu(n th ,f) and 252Cf(sf). The renaissance was initiated by requests for new values especially for γ-ray multiplicity and average total energy release per fission in neutron-induced fission of 235U and 239Pu. Both isotopes are considered the most important ones with respect to the modeling of innovative cores required for the Generation-IV reactors, the majority working with fast neutrons. During the last 5 years we have conducted a systematic study of spectral data for thermal-neutron-induced fission on 235U and 241Pu as well as for the spontaneous fission of 252Cf with unprecedented accuracy. From the new data we conclude that those reactions do not considerably contribute to the observed heat excess and suspect other reactions playing a significant role. Possible contributions may originate from fast-neutron-induced reactions on 238U, which is largely present in the fuel, or from γ-induced fission from neutron capture in the construction material. A first experiment campaign on prompt γ-ray emission from fast-neutron-induced fission on 235,238U was successfully performed in order to test our assumptions. In the following we attempt to summarize, what has been done in the field to date, and to motivate future measurement campaigns exploiting dedicated neutron and photon beams as well as upcoming highly efficient detector assemblies.

Bromine monoxide emissions from Kilauea volcano - Hawai`i

NASA Astrophysics Data System (ADS)

Salerno, G. G.; Oppenheimer, C.; Tsanev, V. I.; Sutton, A. J.; Elias, T.

2009-12-01

Since the first detection of bromine monoxide (BrO) in volcanic plumes, there has been considerable interest in the atmospheric synthesis and impact of reactive halogens in volcanic plumes. We report here the first observations of BrO in the volcanic plume emitted from the summit of Kilauea volcano. We present data collected in 2007, 2008 and 2009 at Pu`u`O`o and Halema`uma`u crater by ground-based Differential Optical Absorption Spectroscopy (DOAS). In 2007, we did not detect any bromine compounds either from the summit or from the Pu`u`O`o plume. However, in 2008 and 2009, we found a good correlation between BrO and SO2 (SO2/BrO molar ratios of ~2000 and ~400) in the plume emitted by the new vent opened at Halema`uma`u crater in March 2008. We discuss the observed variations in BrO production and SO2/BrO ratios over time and contrasting the volcano summit and the east rift zone emissions (with respect to the two-stage degassing long recognized at Kilauea). Factors accounting for the variability include plume age and eruptive style. The presence of BrO in the plume from the new vent in Halema`uma`u crater might depend either on the high temperature from near-surface magma or vent geometry, combined with strong ultraviolet radiation promoting the ”bromine explosion”. Our BrO results significantly extend the global catalogue of volcanic reactive halogen degassing including, for the first time, data representing a hot-spot setting.

Oak ridge national laboratory automated clean chemistry for bulk analysis of environmental swipe samples

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bostick, Debra A.; Hexel, Cole R.; Ticknor, Brian W.

2016-11-01

To shorten the lengthy and costly manual chemical purification procedures, sample preparation methods for mass spectrometry are being automated using commercial-off-the-shelf (COTS) equipment. This addresses a serious need in the nuclear safeguards community to debottleneck the separation of U and Pu in environmental samples—currently performed by overburdened chemists—with a method that allows unattended, overnight operation. In collaboration with Elemental Scientific Inc., the prepFAST-MC2 was designed based on current COTS equipment that was modified for U/Pu separations utilizing Eichrom™ TEVA and UTEVA resins. Initial verification of individual columns yielded small elution volumes with consistent elution profiles and good recovery. Combined columnmore » calibration demonstrated ample separation without crosscontamination of the eluent. Automated packing and unpacking of the built-in columns initially showed >15% deviation in resin loading by weight, which can lead to inconsistent separations. Optimization of the packing and unpacking methods led to a reduction in the variability of the packed resin to less than 5% daily. The reproducibility of the automated system was tested with samples containing 30 ng U and 15 pg Pu, which were separated in a series with alternating reagent blanks. These experiments showed very good washout of both the resin and the sample from the columns as evidenced by low blank values. Analysis of the major and minor isotope ratios for U and Pu provided values well within data quality limits for the International Atomic Energy Agency. Additionally, system process blanks spiked with 233U and 244Pu tracers were separated using the automated system after it was moved outside of a clean room and yielded levels equivalent to clean room blanks, confirming that the system can produce high quality results without the need for expensive clean room infrastructure. Comparison of the amount of personnel time necessary for successful manual vs. automated chemical separations showed a significant decrease in hands-on time from 9.8 hours to 35 minutes for seven samples, respectively. This documented time savings and reduced labor translates to a significant cost savings per sample. Overall, the system will enable faster sample reporting times at reduced costs by limiting personnel hours dedicated to the chemical separation.« less

Pyrochlore-rich titanate ceramics for the immobilization of plutonium: redox effects on phase equilibria in cerium- and thorium- substituted analogs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ryerson, F J; Ebbinghaus, B

2000-05-25

Three compositions representing plutonium-free analogs of a proposed Ca-Ti-Gd-Hf-U-PU oxide ceramic for the immobilization of plutonium were equilibrated at 1 atm, 1350 C over a range of oxygen fugacities between air and that equivalent to the iron-wuestite buffer. The cerium analog replaces Pu on a mole-per-mole basic with Ce; the thorium analog replaces Pu with Th. A third material has 10 wt% Al{sub 2}O{sub 3} added to the cerium analog to encourage the formation of a Hf-analog of, CaHfTi{sub 2}O{sub 7}, zirconolite, which is referred to as hafnolite. The predominant phase produced in each formulation under all conditions is pyrochlore,more » A{sub 2}T{sub 2}O{sub 7}, where the T site is filled by Ti, and Ca, the lanthanides, Hf, U and Pu are accommodated on the A-site. Other lanthanide and uranium-bearing phases encountered include brannerite (UTi{sub 2}O{sub 6}), hafnolite (CaHfTi{sub 2}O{sub 7}), perovskite (CaTiO{sub 3}) and a calcium-lanthanide aluminotitanate with nominal stoichiometry (Ca,Ln)Ti{sub 2}Al{sub 9}O{sub 19}, where Ln is a lanthanide. The phase compositions show progressive shifts with decreasing oxygen fugacity. All of the phases observed have previously been identified in titanate-based high-level radioactive waste ceramics and demonstrate the flexibility of these ceramics to variations in processing parameters. The main variation is an increase in the uranium concentrations of pyrochlore and brannerite which must be accommodated by variations in modal abundance. Pyrochlore compositions are consistent with existing spectroscopic data suggesting that uranium is predominantly pentavalent in samples synthesized in air. A simple model based on ideal stoichiometry suggests the U{sup +4}/{Sigma}U varies linearly with log fO{sub 2} and that all of the uranium is quadravalent at the iron-wuestite buffer.« less

Sm-Nd-Pu timepieces in the Angra dos Reis meteorite

NASA Technical Reports Server (NTRS)

Lugmair, G. W.; Marti, K.

1977-01-01

Isotope ratios and age estimations are presented for the ultramafic pyroxenite Angra dos Reis meteorite. A pyroxene-phosphate internal isochron age of 4.55 plus or minus 0.04 eons was obtained, in agreement with reported Pb-Pb ages. It is suggested that Sm-146 decay led to an increase in the ratio of Nd-142 to Nd-144 in pyroxene, which is greater than the ratio of the Nd isotopes in phosphates. The effect of Pu-244 on the fission xenon components in pyroxene and phosphate is examined. The ratios of Pu-244 to Nd, U-238, and Th-232 are compared for pyroxene and phosphate separates. The exposure age of the meteorite, as obtained by the Kr-81 to Kr-83 method, was found to be 55.5 plus or minus 1.2 million years.

Advancing Understanding of the +4 Metal Extractant Thenoyltrifluoroacetonate (TTA-); Synthesis and Structure of MIVTTA4 (MIV = Zr, Hf, Ce, Th, U, Np, Pu) and MIII(TTA)4- (MIII = Ce, Nd, Sm, Yb).

PubMed

Cary, Samantha K; Livshits, Maksim; Cross, Justin N; Ferrier, Maryline G; Mocko, Veronika; Stein, Benjamin W; Kozimor, Stosh A; Scott, Brian L; Rack, Jeffrey J

2018-04-02

Thenoyltrifluoroacetone (HTTA)-based extractions represent popular methods for separating microscopic amounts of transuranic actinides (i.e., Np and Pu) from macroscopic actinide matrixes (e.g. bulk uranium). It is well-established that this procedure enables +4 actinides to be selectively removed from +3, + 5, and +6 f-elements. However, even highly skilled and well-trained researchers find this process complicated and (at times) unpredictable. It is difficult to improve the HTTA extraction-or find alternatives-because little is understood about why this separation works. Even the identities of the extracted species are unknown. In addressing this knowledge gap, we report here advances in fundamental understanding of the HTTA-based extraction. This effort included comparatively evaluating HTTA complexation with +4 and +3 metals (M IV = Zr, Hf, Ce, Th, U, Np, and Pu vs M III = Ce, Nd, Sm, and Yb). We observed +4 metals formed neutral complexes of the general formula M IV (TTA) 4 . Meanwhile, +3 metals formed anionic M III (TTA) 4 - species. Characterization of these M(TTA) 4 x- ( x = 0, 1) compounds by UV-vis-NIR, IR, 1 H and 19 F NMR, single-crystal X-ray diffraction, and X-ray absorption spectroscopy (both near-edge and extended fine structure) was critical for determining that Np IV (TTA) 4 and Pu IV (TTA) 4 were the primary species extracted by HTTA. Furthermore, this information lays the foundation to begin developing and understanding of why the HTTA extraction works so well. The data suggest that the solubility differences between M IV (TTA) 4 and M III (TTA) 4 - are likely a major contributor to the selectivity of HTTA extractions for +4 cations over +3 metals. Moreover, these results will enable future studies focused on explaining HTTA extractions preference for +4 cations, which increases from Np IV to Pu IV , Hf IV , and Zr IV .

Determination of plutonium and its isotopic ratio in marine sediment samples using quadrupole ICP-MS with the shield torch system under normal plasma conditions.

PubMed

Zheng, Jian; Yamada, Masatoshi; Wang, Zhongliang; Aono, Tatsuo; Kusakabe, Masashi

2004-06-01

An analytical method for determining (239)Pu and (240)Pu in marine sediment samples, which uses quadrupole ICP-MS, was developed in this work. A simple anion-exchange chromatography system was employed for the separation and purification of Pu from the sample matrix. A sufficient decontamination factor of 1.4 x 10(4) for U, which interferes with the determination of (239)Pu, was achieved. High sensitivity Pu determination was obtained, which led to an extremely low concentration detection limit of approximately 8 fg/ml (0.019 mBq/ml for (239)Pu; 0.071 mBq/ml for (240)Pu) in a sample solution, or an absolute detection limit of 42 fg in a 5 ml sample solution, by using the shield torch technique. Analytical results for the determination of the (239+240)Pu and the (240)Pu/(239)Pu ratio in IAEA 368 (ocean sediment) reference material indicated that the accuracy of the method was satisfactory. The method developed was successfully applied to a study of Pu behavior in the sediments from Sagami Bay, Japan. The observed high (240)Pu/(239)Pu ratio in the sediment core indicated that there was additional Pu input derived from close-in fallout in addition to the global fallout.

Age determination of single plutonium particles after chemical separation

NASA Astrophysics Data System (ADS)

Shinonaga, T.; Donohue, D.; Ciurapinski, A.; Klose, D.

2009-01-01

Age determination of single plutonium particles was demonstrated using five particles of the standard reference material, NBS 947 (Plutonium Isotopic Standard. National Bureau of Standards, Washington, D.C. 20234, August 19, 1982, currently distributed as NBL CRM-137) and the radioactive decay of 241Pu into 241Am. The elemental ratio of Am/Pu in Pu particles found on a carbon planchet was measured by wavelength dispersive X-ray spectrometry (WDX) coupled to a scanning electron microscope (SEM). After the WDX measurement, each plutonium particle, with an average size of a few μm, was picked up and relocated to a silicon wafer inside the SEM chamber using a micromanipulator. The silicon wafer was then transferred to a quartz tube for dissolution in an acid solution prior to chemical separation. After the Pu was chemically separated from Am and U, the isotopic ratios of Pu ( 240Pu/ 239Pu, 241Pu/ 239Pu and 242Pu/ 239Pu) were measured with a thermal ionization mass spectrometer (TIMS) for the calculation of Pu age. The age of particles determined in this study was in good agreement with the expected age (35.9 a) of NBS 947 within the measurement uncertainty.

Lava fountain heights at Pu'u 'O'o, Kilauea, Hawaii - Indicators of amount and variations of exsolved magma volatiles

NASA Technical Reports Server (NTRS)

Head, James W., III; Wilson, Lionel

1987-01-01

Factors most important in determining fountain height in Hawaiian-type basaltic eruptions were assessed on the basis of theoretical calculations and observations at Pu'u 'O'o vent, east rift zone of Kilauea, Hawaii. It is shown that fountain height is very sensitive to changes in exsolved gas content (and, thus, can be used to estimate variability in exsolved gas content) and relatively insensitive to large variations in volume flux. Volume flux was found to be the most important parameter determining the equilibrium vent diameter. The results of calculations also indicate that there was a general increase in magma gas content over the first 20 episodes of the Pu'u 'O'o eruption and that gas depletion took place in the conduit beneath the vent during repose periods.

Electroanalytical measurements of binary-analyte mixtures in molten LiCl-KCl eutectic: Uranium(III)- and Magnesium(II)-Chloride

NASA Astrophysics Data System (ADS)

Rappleye, Devin; Newton, Matthew L.; Zhang, Chao; Simpson, Michael F.

2017-04-01

The electrochemical behavior of MgCl2 in molten LiCl-KCl eutectic was investigated to evaluate its suitability as a surrogate for PuCl3 in studies related to the eletrorefining of used nuclear fuel. The reduction of Mg2+ was found to be electrochemically reversible up to 300 mV s-1 at 773 K. The diffusion coefficient for Mg2+ was calculated to be 1.74 and 2.17 × 10-5 cm2 s-1 with and without U3+ present, respectively, at 773 K using cyclic voltammetry (CV). Upon comparison to literature data, the diffusion coefficient of Mg2+ differs by only 8.8% (with U3+ present) from that of Pu3+ and the difference in peak potentials was only 79 mV. Binary-analyte mixtures of UCl3 and MgCl2 in eutectic LiCl-KCl were further investigated using CV, normal pulse voltammetry (NPV), chronoamperometry (CA) and open-circuit potential (OCP) measurements for the purpose of comparing each technique's accuracy in measuring U3+ and Mg2+ concentrations. Of all the techniques tested, NPV resulted in the lowest error which was, on average, 11.4% and 9.81% for U3+ and Mg2+, respectively.

Measurement and simulation of a Compton suppression system for safeguards application

NASA Astrophysics Data System (ADS)

Lee, Seung Kyu; Seo, Hee; Won, Byung-Hee; Lee, Chaehun; Shin, Hee-Sung; Na, Sang-Ho; Song, Dae-Yong; Kim, Ho-Dong; Park, Geun-Il; Park, Se-Hwan

2015-11-01

Plutonium (Pu) contents in spent nuclear fuels, recovered uranium (U) or uranium/transuranium (U/TRU) products must be measured in order to secure the safeguardability of a pyroprocessing facility. Self-induced X-Ray fluorescence (XRF) and gamma-ray spectroscopy are useful techniques for determining Pu-to-U ratios and Pu isotope ratios of spent fuel. Photon measurements of spent nuclear fuel by using high-resolution spectrometers such as high-purity germanium (HPGe) detectors show a large continuum background in the low-energy region, which is due in large part to Compton scattering of energetic gamma rays. This paper proposes a Compton suppression system for reducing of the Compton continuum background. In the present study, the system was configured by using an HPGe main detector and a BGO (bismuth germanate: Bi4Ge3O12) guard detector. The system performances for gamma-ray measurement and XRF were evaluated by means of Monte Carlo simulations and measurements of the radiation source. The Monte Carlo N-Particle eXtended (MCNPX) simulations were performed using the same geometry as for the experiments, and considered, for exact results, the production of secondary electrons and photons. As a performance test of the Compton suppression system, the peak-to-Compton ratio, which is a figure of merit to evaluate the gamma-ray detection, was enhanced by a factor of three or more when the Compton suppression system was used.

Trace element geochemistry of volcanic gases and particles from 1983--1984 eruptive episodes of Kilauea volcano

DOE Office of Scientific and Technical Information (OSTI.GOV)

Crowe, B.M.; Finnegan, D.L.; Zoller, W.H.

1987-12-10

Compositional data have been obtained for volcanic gases and particles collected from fume emitted at the Pu'u O'o vent on the east rift zone of Kilauea volcano. The samples were collected by pumping fume through a filter pack system consisting of a front stage particulate filter followed by four base-treated filters (/sup 7/LiOH). Particles and condensed phases are trapped on the particulate filter, and acidic gases are collected on the treated filters. The filters are analyzed for 30 elements by instrumental neutron activation analysis. Fume samples were collected from the Pu'u O'o vent for two eruptive episodes: (1) 7 daysmore » after episode 11 (cooling vent samples) and (2) the stage of episode 13 (active vent samples).« less

Rapid separation and purification of uranium and plutonium from dilute-matrix samples

DOE PAGES

Armstrong, Christopher R.; Ticknor, Brian W.; Hall, Gregory; ...

2014-03-11

This work presents a streamlined separation and purification approach for trace uranium and plutonium from dilute (carrier-free) matrices. The method, effective for nanogram quantities of U and femtogram to picogram quantities of Pu, is ideally suited for environmental swipe samples that contain a small amount of collected bulk material. As such, it may be applicable for processing swipe samples such as those collected in IAEA inspection activities as well as swipes that are loaded with unknown analytes, such as those implemented in interlaboratory round-robin or proficiency tests. Additionally, the simplified actinide separation could find use in internal laboratory monitoring ofmore » clean room conditions prior to or following more extensive chemical processing. We describe key modifications to conventional techniques that result in a relatively rapid, cost-effective, and efficient U and Pu separation process. We demonstrate the efficacy of implementing anion exchange chromatography in a single column approach. We also show that hydrobromic acid is an effective substitute in lieu of hydroiodoic acid for eluting Pu. Lastly, we show that nitric acid is an effective digestion agent in lieu of perchloric acid and/or hydrofluoric acid. A step by step procedure of this process is detailed.« less

Volatile molecule PuO 3 observed from subliming plutonium dioxide

NASA Astrophysics Data System (ADS)

Ronchi, C.; Capone, F.; Colle, J. Y.; Hiernaut, J. P.

2000-06-01

Mass spectrometric measurements of effusing vapours over PuO 2 and (U, Pu)O 2 indicate the presence of volatile PuO 3 (g) molecules. The formation of plutonium trioxide vapour is due to a chemical process involving oxygen adsorbed during oxidation of the sample. Although in the examined samples, the fraction of trioxide effusing in vacuo was of the order of 0.02 ppm of the plutonium content, under steady-state oxidation conditions it has been shown that the process can have a relevant effect on the sublimation rate of the dioxide.

FLUORINE PROCESS FOR SEPARATION OF MATERIALS

DOEpatents

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

1958-05-01

A process is described for separating plutoniunn from neutron-irradiated uranium, which consists of reacting the irradiated uranium mass with HF to form the tetrafluorides of U, Pu, and Np, and then reacting this mixture of tetrafluorides with fiuorine at temperature between 140 and 315 d C. This causes volatile hexafluorides of U and Np to form while at the temperature employed the Pu tetrafluoride is unaffected and remains as a residue.

Instrumentation effects on U and Pu CBNM standards spectra quality measured on a 500 mm3 CdZnTe and a 2×2 inch LaBr3 detectors

NASA Astrophysics Data System (ADS)

Meleshenkovskii, I.; Borella, A.; Van der Meer, K.; Bruggeman, M.; Pauly, N.; Labeau, P. E.; Schillebeeckx, P.

2018-01-01

Nowadays, there is interest in developing gamma-ray measuring devices based on the room temperature operated medium resolution detectors such as semiconductor detectors of the CdZnTe type and scintillators of the LaBr3 type. This is true also for safeguards applications and the International Atomic Energy Agency (IAEA) has launched a project devoted to the assessment of medium resolution gamma-ray spectroscopy for the verification of the isotopic composition of U and Pu bearing samples. This project is carried out within the Non-Destructive Assay Working Group of the European Safeguards Research and Development Association (ESARDA). In this study we analyze medium resolution spectra of U and Pu standards with the aim to develop an isotopic composition determination algorithm, particularly suited for these types of detectors. We show how the peak shape of a CdZnTe detector is influenced by the instrumentation parameters. The experimental setup consisted of a 500 mm3 CdZnTe detector, a 2×2 inch LaBr3 detector, two types of measurement instrumentation - an analogue one and a digital one, and a set of certified samples - a 207Bi point source and U and Pu CBNM standards. The results of our measurements indicate that the lowest contribution to the peak asymmetry and thus the smallest impact on the resolution of the 500 mm3 CdZnTe detector was achieved with the digital MCA. Analysis of acquired spectra allowed to reject poor quality measurement runs and produce summed spectra files with the least impact of instrumentation instabilities. This work is preliminary to further studies concerning the development of an isotopic composition determination algorithm particularly suited for CZT and LaBr3 detectors for safeguards applications.

Comparative Photoemission Study of Actinide (Am, Pu, Np and U) Metals, Nitrides, and Hydrides

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gouder, Thomas; Seibert, Alice; Rebizant, Jean

2007-07-01

Core-level and valence-band spectra of Pu and the other early actinide compounds show remarkable systematics, which can be understood in the framework of final state screening. We compare the early actinide (U, Np, Pu and Am) metals, nitrides and hydrides and a few other specific compounds (PuSe, PuS, PuCx, PuSix) prepared as thin films by sputter deposition. In choosing these systems, we combine inherent 5f band narrowing, due to 5f orbital contraction throughout the actinide series, with variations of the chemical environment in the compounds. Goal of this work was to learn more on the electronic structure of the earlymore » actinide systems and to achieve the correct interpretation of their photoemission spectra. The highly correlated nature of the 5f states in systems, which are on the verge to localization, makes this a challenging task, because of the peculiar interplay between ground state DOS and final-state effects. Their influence can be estimated by doing systematic studies on systems with different (5f) bandwidths. We conclude on the basis of such systematic experiments that final-state effects due to strong e-e correlations in narrow 5f-band systems lead to multiplet like structures, analogous to those observed in the case of systems with localized electron states. Such observations in essentially band-like 5f-systems was first surprising, but the astonishing similarity of photoemission spectra of very different chemical systems (e.g. PuSe, Pu{sub 2}C{sub 3}..) points to a common origin, relating them to atomic features rather than material dependent density of states (DOS) features. (authors)« less

Hyperfine field, electric field gradient, quadrupole coupling constant and magnetic properties of challenging actinide digallide

NASA Astrophysics Data System (ADS)

Khan, Sajid; Yazdani-Kachoei, M.; Jalali-Asadabadi, S.; Ahmad, Iftikhar

2017-12-01

In this paper, we explore the structural and magnetic properties as well as electric field gradient (EFG), hyperfine field (HFF) and quadrupole coupling constant in actinide digallide AcGa2 (Ac = U, Np, Pu) using LDA, GGA, LDA+U, GGA+U and hybrid functional with Wu-Cohen Generalized Gradient approximation HF-WC. Relativistic effects of the electrons are considered by including spin-orbit coupling. The comparison of the calculated structural parameters and magnetic properties with the available experimental results confirms the consistency and hence effectiveness of our theoretical tools. The calculated magnetic moments demonstrate that UGa2 and NpGa2 are ferromagnetic while PuGa2 is antiferromagnetic in nature. The EFG of AcGa2 is reported for the first time. The HFF, EFG and quadrupole coupling constant in AcGa2 (Ac = U, Np, Pu) are mainly originated from f-f and p-p contributions of Ac atom and p-p contribution of Ga atom.

Renewability and sustainability aspects of nuclear energy

NASA Astrophysics Data System (ADS)

Şahin, Sümer

2014-09-01

Renewability and sustainability aspects of nuclear energy have been presented on the basis of two different technologies: (1) Conventional nuclear technology; CANDU reactors. (2) Emerging nuclear technology; fusion/fission (hybrid) reactors. Reactor grade (RG) plutonium, 233U fuels and heavy water moderator have given a good combination with respect to neutron economy so that mixed fuel made of (ThO2/RG-PuO2) or (ThC/RG-PuC) has lead to very high burn up grades. Five different mixed fuel have been selected for CANDU reactors composed of 4 % RG-PuO2 + 96 % ThO2; 6 % RG-PuO2 + 94 % ThO2; 10 % RG-PuO2 + 90 % ThO2; 20 % RG-PuO2 + 80 % ThO2; 30 % RG-PuO2 + 70 % ThO2, uniformly taken in each fuel rod in a fuel channel. Corresponding operation lifetimes have been found as ˜ 0.65, 1.1, 1.9, 3.5, and 4.8 years and with burn ups of ˜ 30 000, 60 000, 100 000, 200 000 and 290 000 MW.d/ton, respectively. Increase of RG-PuO2 fraction in radial direction for the purpose of power flattening in the CANDU fuel bundle has driven the burn up grade to 580 000 MW.d/ton level. A laser fusion driver power of 500 MWth has been investigated to burn the minor actinides (MA) out of the nuclear waste of LWRs. MA have been homogenously dispersed as carbide fuel in form of TRISO particles with volume fractions of 0, 2, 3, 4 and 5 % in the Flibe coolant zone in the blanket surrounding the fusion chamber. Tritium breeding for a continuous operation of the fusion reactor is calculated as TBR = 1.134, 1.286, 1.387, 1.52 and 1.67, respectively. Fission reactions in the MA fuel under high energetic fusion neutrons have lead to the multiplication of the fusion energy by a factor of M = 3.3, 4.6, 6.15 and 8.1 with 2, 3, 4 and 5 % TRISO volume fraction at start up, respectively. Alternatively with thorium, the same fusion driver would produce ˜160 kg 233U per year in addition to fission energy production in situ, multiplying the fusion energy by a factor of ˜1.3.

AFS-2 FLOWSHEET MODIFICATIONS TO ADDRESS THE INGROWTH OF PU(VI) DURING METAL DISSOLUTION

DOE Office of Scientific and Technical Information (OSTI.GOV)

Crapse, K.; Rudisill, T.; O'Rourke, P.

2014-07-02

In support of the Alternate Feed Stock Two (AFS-2) PuO{sub 2} production campaign, Savannah River National Laboratory (SRNL) conducted a series of experiments concluding that dissolving Pu metal at 95°C using a 6–10 M HNO{sub 3} solution containing 0.05–0.2 M KF and 0–2 g/L B could reduce the oxidation of Pu(IV) to Pu(VI) as compared to dissolving Pu metal under the same conditions but at or near the boiling temperature. This flowsheet was demonstrated by conducting Pu metal dissolutions at 95°C to ensure that PuO{sub 2} solids were not formed during the dissolution. These dissolution parameters can be used formore » dissolving both Aqueous Polishing (AP) and MOX Process (MP) specification materials. Preceding the studies reported herein, two batches of Pu metal were dissolved in the H-Canyon 6.1D dissolver to prepare feed solution for the AFS-2 PuO{sub 2} production campaign. While in storage, UV-visible spectra obtained from an at-line spectrophotometer indicated the presence of Pu(VI). Analysis of the solutions also showed the presence of Fe, Ni, and Cr. Oxidation of Pu(IV) produced during metal dissolution to Pu(VI) is a concern for anion exchange purification. Anion exchange requires Pu in the +4 oxidation state for formation of the anionic plutonium(IV) hexanitrato complex which absorbs onto the resin. The presence of Pu(VI) in the anion feed solution would require a valence adjustment step to prevent losses. In addition, the presence of Cr(VI) would result in absorption of chromate ion onto the resin and could limit the purification of Pu from Cr which may challenge the purity specification of the final PuO{sub 2} product. Initial experiments were performed to quantify the rate of oxidation of Pu(IV) to Pu(VI) (presumed to be facilitated by Cr(VI)) as functions of the HNO{sub 3} concentration and temperature in simulated dissolution solutions containing Cr, Fe, and Ni. In these simulated Pu dissolutions studies, lowering the temperature from near boiling to 95 °C reduced the oxidation rate of Pu(IV) to Pu(VI). For 8.1 M HNO{sub 3} simulated dissolution solutions, at near boiling conditions >35% Pu(VI) was present in 50 h while at 95 °C <10% Pu(VI) was present at 50 h. At near boiling temperatures, eliminating the presence of Cr and varying the HNO{sub 3} concentration in the range of 7–8.5 M had little effect on the rate of conversion of Pu(IV) to Pu(VI). HNO{sub 3} oxidation of Pu(IV) to Pu(VI) in a pure solution has been reported previously. Based on simulated dissolution experiments, this study concluded that dissolving Pu metal at 95°C using a 6 to 10 M HNO{sub 3} solution 0.05–0.2 M KF and 0–2 g/L B could reduce the rate of oxidation of Pu(IV) to Pu(VI) as compared to near boiling conditions. To demonstrate this flowsheet, two small-scale experiments were performed dissolving Pu metal up to 6.75 g/L. No Pu-containing residues were observed in the solutions after cooling. Using Pu metal dissolution rates measured during the experiments and a correlation developed by Holcomb, the time required to completely dissolve a batch of Pu metal in an H-Canyon dissolver using this flowsheet was estimated to require nearly 5 days (120 h). This value is reasonably consistent with an estimate based on the Batch 2 and 3 dissolution times in the 6.1D dissolver and Pu metal dissolution rates measured in this study and by Rudisill et al. Data from the present and previous studies show that the Pu metal dissolution rate decreases by a factor of approximately two when the temperature decreased from boiling (112 to 116°C) to 95°C. Therefore, the time required to dissolve a batch of Pu metal in an H-Canyon dissolver at 95°C would likely double (from 36 to 54 h) and require 72 to 108 h depending on the surface area of the Pu metal. Based on the experimental studies, a Pu metal dissolution flowsheet utilizing 6–10 M HNO{sub 3} containing 0.05–0.2 M KF (with 0–2 g/L B) at 95°C is recommended to reduce the oxidation of Pu(IV) to Pu(VI) as compared to near boiling conditions. The time required to completely dissolve a batch of Pu metal will increase, however, by approximately a factor of two as compared to initial dissolutions at near boiling (assuming the KF concentration is maintained at nominally 0.1 M). By lowering the temperature to 95°C under otherwise the same operating parameters as previous dissolutions, the Pu(VI) concentration should not exceed 15% after a 120 h heating cycle. Increasing the HNO{sub 3} concentration and lowering Pu concentration are expected to further limit the amount of Pu(VI) formed.« less

A rapid and accurate method for the determination of plutonium in food using magnetic sector ICP-MS with an ultra-sonic nebuliser and ion chromatography.

PubMed

Evans, P; Elahi, S; Lee, K; Fairman, B

2003-02-01

In the event of a nuclear incident it is essential that analytical information on the distribution and level of contamination is available. An ICP-MS method is described which can provide data on plutonium contamination in food within 3 h of sample receipt without compromising detection limits or accuracy relative to traditional counting methods. The method can also provide simultaneous determinations of americium and neptunium. Samples were prepared by HNO3 closed-vessel microwave digestion, evaporated to dryness and diluted into a mobile phase comprising 1.5 M HNO3 and 0.1 mM 2,6-pyridinedicarboxylic acid. A commercially available polystyrene-divinylbenzene ion chromatography column provides on-line separation of 239Pu and 238U reducing the impact of the 238U1H interference. Oxidation of the sample using H2O2 ensures all Pu is in the Pu(+4) state. The oxidation also displaces Np away from the solvent front by changing the oxidation state from Np(+3) to Np(+4) and produces the insoluble Am(+4) ion. Simultaneous Pu, Am and Np analyses therefore require omission of the oxidation stage and some loss of Pu data quality. Analyses were performed using a magnetic sector ICP-MS (Finnigan MAT Element). The sample is introduced to the plasma via an ultrasonic nebuliser-desolvation unit (Cetac USN 6000AT+). This combination achieves an instrumental sensitivity of 238U > 2 x 10(7) cps/ppb and removes hydrogen from the sample gas, which also inhibits the formation of 238U1H. The net effect of the improved sample introduction conditions is to achieve detection levels for Pu of 0.020 pg g(-1) (4.6 x 10(-2) Bq kg(-1)) which is significantly below 1/10th of the most stringent EU (European Union) legislation, currently 0.436 pg g(-1) (1 Bq kg(-1)) set for baby food. The new method was evaluated with a range of biological samples ranging from cabbage to milk and meat. Recovery of Pu agrees with published values (100% +/- 20%).

Neutron-Induced Fission Measurements at the Dance and Lsds Facilities at Lanl

NASA Astrophysics Data System (ADS)

Jandel, M.; Bredeweg, T. A.; Bond, E. M.; Chadwick, M. B.; Couture, A.; O'Donnell, J. M.; Fowler, M. M.; Haight, R. C.; Hayes-Sterbenz, A. C.; Rundberg, R. S.; Rusev, G. Y.; Ullmann, J. L.; Vieira, D. J.; Wilhelmy, J. B.; Wu, C. Y.; Becker, J. A.; Alexander, C. W.; Belier, G.

2014-09-01

New results from neutron-induced fission measurements performed at the Detector for Advanced Neutron Capture Experiments (DANCE) and Lead Slowing Down Spectrometer (LSDS) are presented. New correlated data on promptfission γ-ray (PFG) distributions were measured using the DANCE array for resonant neutron-induced fission of 233U, 235U and 239Pu. The deduced properties of PFG emission are presented using a simple parametrization. An accurate knowledge of fission γ-ray spectra enables us to analyze the isomeric states of 236U created after neutron capture on 235U. We briefly discuss these new results. Finally, we review details and preliminary results of the challenging 237U(n,f) cross section measurement at the LSDS facility.

Iodine-xenon studies of Allende inclusions - Eggs and the Pink Angel

NASA Technical Reports Server (NTRS)

Swindle, T. D.; Caffee, M. W.; Hohenberg, C. M.

1988-01-01

The I-Xe systems of six Allende inclusions (five Eggs and the Pink Angel) appear to have been altered by nonnebular secondary processes. Evidence for this includes temperature-ordered variations in the initial I isotopic composition within several objects (with older apparent I-Xe ages associated with higher extraction temperatures) and the absence of primitive I-Xe ages. The span of apparent ages seen in Allende objects (10 Myr or more) is probably too long to reflect any nebular process, so at least some alteration probably occurred ont the parent body. The range in initial (Pu-244)/(U-238) ratios for the Eggs (0.003-0.014) includes the current best estimates of the bulk solar system value (0.004-0.007). For Egg 3, the Pu/U ratio varies by a factor of two between extractions, probably the result of fractionation of Pu from U among different phases.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Swindle, T.D.; Caffee, M.W.; Hohenberg, C.M.

The iodine-xenon systems of six Allende inclusions (five Eggs and the Pink Angel) appear to have been altered by non-nebular secondary processes. Evidence for this includes temperature-ordered variations in the initial I isotopic composition within several objects (with older apparent I-Xe ages associated with higher extraction temperatures) and the absence of primitive I-Xe ages. The span of apparent ages seen in Allende objects (10 Ma or more) is probably too long to reflect any nebular process, so at least some alteration probably occurred on the parent body. The range in initial {sup 244}Pu/{sup 238}U ratios for the Eggs (3-14 {times}more » 10{sup minus 3}) includes the current best estimates of the bulk solar system value (4-7 {times} 10{sup minus 3}). For Egg 3, the Pu/U ratio varies by a factor of two between extractions, probably the result of fractionation of Pu from U among different phases.« less

U-238 fission and Pu-239 production in subcritical assembly

NASA Astrophysics Data System (ADS)

Grab, Magdalena; Wojciechowski, Andrzej

2018-04-01

The project touches upon an issue of U-238 fission reactions and Pu-239 production reactions in subcritical assembly. The experiment took place in November 2014 at the Dzhelepov Laboratory of Nuclear Problems (JINR, Dubna) using PHASOTRON.Data of this experiment were analyzed in Laboratory of Information Technologies (LIT). Four MCNPX models were considered for simulation: Bertini/Dresnen, Bertini/Abla, INCL4/Drensnen, INCL4/Abla. The main goal of the project was to compare the experimental data and simulation results. We obtain a good agreement of experimental data and computation results especially for detectors placed besides the assembly axis. In addition, the U-238 fission reactions are more probable to be observed in the region of a higher particle energy spectrum, located closer to the assembly axis and the particle beam as well and vice versa Pu-239 production reactions were dominant in the peripheral region of geometry.

Gas analyses from the Pu'u O'o eruption in 1985, Kilauea volcano, Hawaii

USGS Publications Warehouse

Greenland, L.P.

1986-01-01

Volcanic gas samples were collected from July to November 1985 from a lava pond in the main eruptive conduit of Pu'u O'o from a 2-week-long fissure eruption and from a minor flank eruption of Pu'u O'o. The molecular composition of these gases is consistent with thermodynamic equilibrium at a temperature slightly less than measured lava temperatures. Comparison of these samples with previous gas samples shows that the composition of volatiles in the magma has remained constant over the 3-year course of this episodic east rift eruption of Kilauea volcano. The uniformly carbon depleted nature of these gases is consistent with previous suggestions that all east rift eruptive magmas degas during prior storage in the shallow summit reservoir of Kilauea. Minor compositional variations within these gas collections are attributed to the kinetics of the magma degassing process. ?? 1986 Springer-Verlag.

Tritium concentrations in the active Pu'u O'o crater, Kilauea volcano, Hawaii: implications for cold fusion in the Earth's interior

NASA Astrophysics Data System (ADS)

Quick, J. E.; Hinkley, T. K.; Reimer, G. M.; Hedge, C. E.

1991-11-01

The assertion that deuterium-deuterium fusion may occur at low temperature suggests a potential new source of geothermal heat. If a cold-fusion-like process occurs within the Earth, then a test for its existence would be a search for anomalous tritium in volcanic emissions. The Pu'u O'o crater is the first point at which large amounts of water are degassed from the magma that feeds the Kilauea system. The magma is probably not contaminated by meteoric-source ground water prior to degassing at Pu'u O'o, although mixing of meteoric and magmatic H 2O occurs within the crater. Tritium contents of samples from within the crater are lower than in samples taken simultaneously from the nearby upwind crater rim. These results provide no evidence in support of a cold-fusion-like process in the Earth's interior.

Tritium concentrations in the active Pu'u O'o crater, Kilauea volcano, Hawaii: implications for cold fusion in the Earth's interior

USGS Publications Warehouse

Quick, J.E.; Hinkley, T.K.; Reimer, G.M.; Hedge, C.E.

1991-01-01

The assertion that deuterium-deuterium fusion may occur at low temperature suggests a potential new source of geothermal heat. If a cold-fusion-like process occurs within the Earth, then a test for its existence would be a search for anomalous tritium in volcanic emissions. The Pu'u O'o crater is the first point at which large amounts of water are degassed from the magma that feeds the Kilauea system. The magma is probably not contaminated by meteoric-source ground water prior to degassing at Pu'u O'o, although mixing of meteoric and magmatic H2O occurs within the crater. Tritium contents of samples from within the crater are lower than in samples taken simultaneously from the nearby upwind crater rim. These results provide no evidence in support of a cold-fusion-like process in the Earth's interior. ?? 1991.

Induction of osteosarcoma and acute myeloid leukaemia in CBA/H mice by the alpha-emitting nuclides, uranium-233, plutonium-239 and amercium-241.

PubMed

Ellender, M; Harrison, J D; Pottinger, H; Thomas, J M

2001-01-01

To compare tumour induction in CBA/H mice, principally osteosarcoma and acute myeloid leukaemia, resulting from exposure to the alpha-emitting nuclides, uranium-233, plutonium-239 and americium-241, and to relate differences between the three nuclides to the pattern of dose delivery within tissues. Each nuclide was administered intraperitoneally in citrate solution to three groups of adult male CBA/H mice at levels of activity which gave estimated life-time average skeletal doses of about 0.25-0.3 Gy, 0.5-1 Gy and 1-2 Gy. Animals were carefully monitored and sacrificed as soon as they showed signs of ill health; tumours were identified by standard histopathological techniques. Statistical modelling by Cox regression showed that, considering all three nuclides together, there was a highly significant increase in risk of death from osteosarcoma or myeloid leukaemia with increasing dose rate. For osteosarcoma, the effect was significantly greater for 239Pu than 241Am, while separate analysis for 233U showed no significant increase with increasing dose rate. For example, the increase in relative risk of death from osteosarcoma for an increase in life-time average dose rate to bone of 1 mGyd(-1) was 4.2 (2.7-6.5) for 239Pu, 2.3 (1.4-3.4) for 241Am and 1.1 (0.4-3.1) for 233U. For myeloid leukaemia, there was no significant difference between 239Pu and 241Am in the effect of dose rate. The increase in relative risk from myeloid leukaemia for an increase in average dose rate of 1 mGyd(-1) was 1.8 (1.1-2.8) for 239Pu, 2.0 (1.4-2.9) for 241Am and 1.5 (0.8-2.7) for 233U. Significant increases in renal and hepatic carcinomas were also recorded in animals exposed to 233U and 241Am, respectively. Studies of the distribution of the nuclides within the skeleton, published separately, have shown differences in their retention in individual bones and within bone. The proportions of decays occurring near to endosteal bone surfaces and throughout bone marrow were in the order: 239Pu> 241Am>233U. For osteosarcoma, the relative effectiveness of the nuclides in terms of average bone dose, in the order 239Pu>241Am>233U, is consistent with the proportion of dose delivered near to endosteal surfaces. For myeloid leukaemia, the greater effectiveness of 239Pu and 241Am than 233U is consistent with their accumulation in marrow.

Impact of fission neutron energies on reactor antineutrino spectra

NASA Astrophysics Data System (ADS)

Littlejohn, B. R.; Conant, A.; Dwyer, D. A.; Erickson, A.; Gustafson, I.; Hermanek, K.

2018-04-01

Recent measurements of reactor-produced antineutrino fluxes and energy spectra are inconsistent with models based on measured thermal fission beta spectra. In this paper, we examine the dependence of antineutrino production on fission neutron energy. In particular, the variation of fission product yields with neutron energy has been considered as a possible source of the discrepancies between antineutrino observations and models. In simulations of low-enriched and highly-enriched reactor core designs, we find a substantial fraction of fissions (from 5% to more than 40%) are caused by nonthermal neutrons. Using tabulated evaluations of nuclear fission and decay, we estimate the variation in antineutrino emission by the prominent fission parents U 235 , Pu 239 , and Pu 241 versus neutron energy. The differences in fission neutron energy are found to produce less than 1% variation in detected antineutrino rate per fission of U 235 , Pu 239 , and Pu 241 . Corresponding variations in the antineutrino spectrum are found to be less than 10% below 7 MeV antineutrino energy, smaller than current model uncertainties. We conclude that insufficient modeling of fission neutron energy is unlikely to be the cause of the various reactor anomalies. Our results also suggest that comparisons of antineutrino measurements at low-enriched and highly-enriched reactors can safely neglect the differences in the distributions of their fission neutron energies.

The prospect of uranium nitride (UN) and mixed nitride fuel (UN-PuN) for pressurized water reactor

NASA Astrophysics Data System (ADS)

Syarifah, Ratna Dewi; Suud, Zaki

2015-09-01

Design study of small Pressurized Water Reactors (PWRs) core loaded with uranium nitride fuel (UN) and mixed nitride fuel (UN-PuN), Pa-231 as burnable poison, and Americium has been performed. Pa-231 known as actinide material, have large capture cross section and can be converted into fissile material that can be utilized to reduce excess reactivity. Americium is one of minor actinides with long half life. The objective of adding americium is to decrease nuclear spent fuel in the world. The neutronic analysis results show that mixed nitride fuel have k-inf greater than uranium nitride fuel. It is caused by the addition of Pu-239 in mixed nitride fuel. In fuel fraction analysis, for uranium nitride fuel, the optimum volume fractions are 45% fuel fraction, 10% cladding and 45% moderator. In case of UN-PuN fuel, the optimum volume fractions are 30% fuel fraction, 10% cladding and 60% coolant/ moderator. The addition of Pa-231 as burnable poison for UN fuel, enrichment U-235 5%, with Pa-231 1.6% has k-inf more than one and excess reactivity of 14.45%. And for mixed nitride fuel, the lowest value of reactivity swing is when enrichment (U-235+Pu) 8% with Pa-231 0.4%, the excess reactivity value 13,76%. The fuel pin analyze for the addition of Americium, the excess reactivity value is lower than before, because Americium absorb the neutron. For UN fuel, enrichment U-235 8%, Pa-231 1.6% and Am 0.5%, the excess reactivity is 4.86%. And for mixed nitride fuel, when enrichment (U-235+Pu) 13%, Pa-231 0.4% and Am 0.1%, the excess reactivity is 11.94%. For core configuration, it is better to use heterogeneous than homogeneous core configuration, because the radial power distribution is better.

The interaction of molecular hydrogen with α-radiolytic oxidants on a (U,Pu)O2 surface

NASA Astrophysics Data System (ADS)

Bauhn, Lovisa; Hansson, Niklas; Ekberg, Christian; Fors, Patrik; Delville, Rémi; Spahiu, Kastriot

2018-07-01

In order to assess the impact of α-radiolysis of water on the oxidative dissolution of spent fuel, an un-irradiated, annealed MOX fuel pellet with high content of Pu (∼24 wt%), and a specific α-activity of 4.96 GBq/gMOX, was leached in carbonate-containing solutions of low ionic strength. The high Pu content in the pellet stabilizes the (U,Pu)O2(s) matrix towards oxidative dissolution, whereas the α-decays emitted from the surface are expected to produce ∼3.6 × 10-7 mol H2O2/day, contributing to the oxidative dissolution of the pellet. Two sets of leaching tests were conducted under different redox conditions: Ar gas atmosphere and deuterium gas atmosphere. A relatively slow increase of the U and Pu concentrations was observed in the Ar case, with U concentrations increasing from 1·10-6 M after 1 h to ∼7 × 10-5 M after 58 days. Leaching under an atmosphere starting at 1 MPa deuterium gas was undertaken in order to evaluate any effect of dissolved hydrogen on the radiolytic dissolution of the pellet, as well as to investigate any potential recombination of the α-radiolytic products with dissolved deuterium. For the latter purpose, isotopic analysis of the D/H content was carried out on solution samples taken during the leaching. Despite the continuous production of radiolytic oxidants, the concentrations of U and Pu remained quite constant at the level of ∼3 × 10-8 M during the first 30 days, i.e. as long as the deuterium pressure remained higher than 0.8 MPa. These data rule out any oxidative dissolution of the pellet during the first month. The un-irradiated MOX fuel does not contain metallic ε-particles, hence it is mainly the interaction of radiolytic oxidants and dissolved deuterium with the surface of the mixed actinide oxide that causes the neutralization of the oxidants. This conclusion is supported by the steadily increasing levels of HDO measured in the leachate samples.

Safeguards in Pyroprocessing: an Integrated Model Development and Measurement Data Analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Jinsuo

Pyroprocessing is an electrochemical method based on the molten salt electrolyte, mainly the LiCl-KCl eutectic molten salt, to recycle the used nuclear fuel. For a conceptual design of commercial pyroprocessing facility, tons of special nuclear materials, namely U and Pu, may be involved, which could be used for non-peaceful purposes if they are diverted. Effective safeguards approaches have to be developed prior to the development and construction of a pyroprocessing facility. Present research focused on two main objectives, namely calculating the properties of nuclear species in LiCl-KCl molten salt and developing integrated model to safeguard a pyroprocessing facility. Understanding themore » characteristics of special nuclear materials in LiCl-KCl eutectic salt is extremely important to understand their behaviors in an electrorefiner. The model development for the separation processes in the pyroprocessing, including electrorefining, actinide drawdown, and rare earth drawdown benefits the understanding of material transport and separation performance of these processes under various conditions. The output signals, such as potential, current, and species concentration contribute to the material balance closure and provide safeguards signatures to detect the scenarios of diversion. U and Pu are the two main elements concerned in this study due to our interest in safeguards.« less

Cooperation on Improved Isotopic Identification and Analysis Software for Portable, Electrically Cooled High-Resolution Gamma Spectrometry Systems Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dreyer, Jonathan G.; Wang, Tzu-Fang; Vo, Duc T.

Under a 2006 agreement between the Department of Energy (DOE) of the United States of America and the Institut de Radioprotection et de Sûreté Nucléaire (IRSN) of France, the National Nuclear Security Administration (NNSA) within DOE and IRSN initiated a collaboration to improve isotopic identification and analysis of nuclear material [i.e., plutonium (Pu) and uranium (U)]. The specific aim of the collaborative project was to develop new versions of two types of isotopic identification and analysis software: (1) the fixed-energy response-function analysis for multiple energies (FRAM) codes and (2) multi-group analysis (MGA) codes. The project is entitled Action Sheet 4more » – Cooperation on Improved Isotopic Identification and Analysis Software for Portable, Electrically Cooled, High-Resolution Gamma Spectrometry Systems (Action Sheet 4). FRAM and MGA/U235HI are software codes used to analyze isotopic ratios of U and Pu. FRAM is an application that uses parameter sets for the analysis of U or Pu. MGA and U235HI are two separate applications that analyze Pu or U, respectively. They have traditionally been used by safeguards practitioners to analyze gamma spectra acquired with high-resolution gamma spectrometry (HRGS) systems that are cooled by liquid nitrogen. However, it was discovered that these analysis programs were not as accurate when used on spectra acquired with a newer generation of more portable, electrically cooled HRGS (ECHRGS) systems. In response to this need, DOE/NNSA and IRSN collaborated to update the FRAM and U235HI codes to improve their performance with newer ECHRGS systems. Lawrence Livermore National Laboratory (LLNL) and Los Alamos National Laboratory (LANL) performed this work for DOE/NNSA.« less

Results of The Excreta Bioassay Quality Control Program For April 1, 2010 Through March 31, 2011

DOE Office of Scientific and Technical Information (OSTI.GOV)

Antonio, Cheryl L.

2012-07-19

A total of 76 urine samples and 10 spiked fecal samples were submitted during the report period (April 1, 2010 through March 31, 2011) to GEL Laboratories, LLC in South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for 14C, Sr, for 238Pu, 239Pu, 241Am, 243Am, 235U, 238U, 238U-mass and fecal analyses for 241Am, 238Pu and 239Pu were tested this year. The number of QC urine samples submitted during the report period represented 1.1% of the total samples submitted. In addition to the samples provided by IDP,more » GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 31% of the analyses processed by GEL during the first year of contract 112512 were quality control samples. GEL tested the performance of 23 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty except the slightly elevated relative bias for 243,244Cm (Table 4).« less

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Goldstein, Steven J; Oldham, Warren J; Murrell, Michael T

2010-12-07

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

Quantitative Fissile Assay In Used Fuel Using LSDS System

NASA Astrophysics Data System (ADS)

Lee, YongDeok; Jeon, Ju Young; Park, Chang-Je

2017-09-01

A quantitative assay of isotopic fissile materials (U235, Pu239, Pu241) was done at Korea Atomic Energy Research Institute (KAERI), using lead slowing down spectrometer (LSDS). The optimum design of LSDS was performed based on economics, easy maintenance and assay effectiveness. LSDS system consists of spectrometer, neutron source, detection and control. LSDS system induces fissile fission and fast neutrons are collected at fission chamber. The detected signal has a direct relation to the mass of existing fissile isotopes. Many current commercial assay technologies have a limitation in direct application on isotopic fissile assay of spent fuel, except chemical analysis. In the designed system, the fissile assay model was setup and the correction factor for self-shield was obtained. The isotopic fissile content assay was performed by changing the content of Pu239. Based on the fuel rod, the isotopic content was consistent with 2% uncertainty for Pu239. By applying the covering (neutron absorber), the effective shielding was obtained and the activation was calculated on the target. From the assay evaluation, LSDS technique is very powerful and direct to analyze the isotopic fissile content. LSDS is applicable for nuclear fuel cycle and spent fuel management for safety and economics. Additionally, an accurate fissile content will contribute to the international transparency and credibility on spent fuel.

Decay of Plutonium isotopes via spontaneous and heavy-ion induced fission paths

NASA Astrophysics Data System (ADS)

Sharma, Kanishka; Sawhney, Gudveen; Sharma, Manoj K.; Gupta, Raj K.

2018-04-01

Based on the collective clusterization approach, we have extended our earlier study on α-decay, exotic cluster-decay, and heavy particle radioactivity, to the phenomenon of spontaneous fission (SF) in the ground-state (g.s.) decays of even mass 234-246Pu parents. The calculations for the SF half-lives of these Pu-isotopes have been made within the framework of preformed cluster model (PCM), both for spherical as well as β2-deformed choices of shapes, and a comparison is made with the relevant available experimental data, which prefer spherical shapes. The importance of the orientation degree of freedom (hot compact or cold elongated configurations) is also explored. Next, in order to look for the exclusive role of heavy-ion induced fission, the dynamics of 6He + 238U reaction forming 244Pu* is studied over the center of mass energy range of E c . m . = 15.0- 28.8MeV, using the dynamical cluster-decay model (DCM), an extension of the PCM with temperature T- and angular momentum ℓ-effects included. The β2-deformed fragments of 244Pu* in the mass range A2 = 106- 113 (plus their complementary heavy fragments), corresponding to asymmetric fission peaks, are found contributing towards the fission cross-section. Finally, the potential energy surfaces and barrier modification effects are presented for the relative comparison of spontaneous and the heavy-ion induced fission processes. Both are found to behave similar with respect to the probable emission of fragments and hence point out to the shell closure property of the decay fragments.

Vesicle microtexture analysis and eruption dynamics of selected high fountaining episodes at Pu`u `Ō`ō, Kīlauea volcano, Hawai`i between 1985-1986.

NASA Astrophysics Data System (ADS)

Holt, S. J.; Carey, R.; Houghton, B. F.; Orr, T. R.; McPhie, J.

2015-12-01

The early phases of the ongoing eruption of Pu`u `Ō`ō in the East Rift Zone (ERZ) of Kīlauea on Hawai`i provide a unique opportunity to study the vesicle microtexture of tephra from five high (≥200m) Hawaiian fountaining events, from a single vent, over a prolonged period of time. The high Hawaiian fountains erupted at Pu`u `Ō`ō varied in height from 200 m up to a maximum of 467 m, during which the shallow conduit at Pu`u `Ō`ō remained stable. We conducted microtextural analysis of pyroclasts from five high (264 to 391 m) Hawaiian fountaining episodes at Kīlauea, Episodes 32, 37, 40, 44 and 45, erupted from the Pu`u `Ō`ō vent between 1985 and 1986 in order to constrain the parameters that lead to large variations in fountain height of Hawaiian fountains at Pu`u `Ō`ō. Our results show that pyroclasts from a single episode can vary greatly in texture (from bubbly to foamy) and have vesicle volume densities (Nmv) that vary by an order of magnitude. This range in vesicle texture and population is due to extensive growth and coalescence of vesicles within the eruption jet post-fragmentation, resulting in the observed vesicle texture not being wholly indicative of the syn-fragmentation vesicle population. Only four pyroclasts were found to have textures that are interpreted to be indicative of the vesicle population at the moment of fragmentation, all of which have bubbly texture, high density, high Nmv, and low vesicle-to-melt ratio (VG/VL). Due to the paucity of pyroclasts representative of syn-eruption vesiculation processes, comparison of shallow conduit dynamics across episodes can only be qualitative observations, which suggest the ascending melt is thermally and mechanically heterogeneous on a small scale during Hawaiian-style fountaining. This highlights the importance for detailed micro-scale qualitative textural observations on pyroclasts with end-member densities, as well as modal densities, when carrying out vesicle microtexture analysis. This will ensure that a sufficient number of pyroclasts with textures representative of the syn-fragmentation vesicle population are identified, in order to carry out quantitative comparisons across episodes.

SO2 from episode 48A eruption, Hawaii: Sulfur dioxide emissions from the episode 48A East Rift Zone eruption of Kilauea volcano, Hawaii

USGS Publications Warehouse

Andres, R.J.; Kyle, P.R.; Stokes, J.B.; Rose, William I.

1989-01-01

An SO2 flux of 1170??400 (1??) tonnes per day was measured with a correlation spectrometer (COSPEC) in October and November 1986 from the continuous, nonfountaining, basaltic East Rift Zone eruption (episode 48A) of Kilauea volcano. This flux is 5-27 times less than those of highfountaining episodes, 3-5 times greater than those of contemporaneous summit emissions or interphase Pu'u O'o emissions, and 1.3-2 times the emissions from Pu'u O'o alone during 48A. Calculations based on the SO2 emission rate resulted in a magma supply rate of 0.44 million m3 per day and a 0.042 wt% sulfur loss from the magma upon eruption. Both of these calculated parameters agree with determinations made previously by other methods. ?? 1989 Springer-Verlag.

HOW OLD IS IT? - 241PU/241AM NUCLEAR FORENSIC CHRONOLOGY REFERENCE MATERIALS

PubMed Central

Fitzgerald, Ryan; Inn, Kenneth G.W.; Horgan, Christopher

2018-01-01

One material attribute for nuclear forensics is material age. 241Pu is almost always present in uranium- and plutonium-based nuclear weapons, which pose the greatest threat to our security. The in-growth of 241Am due to the decay of 241Pu provides an excellent chronometer of the material. A well-characterized 241Pu/241Am standard is needed to validate measurement capability, as a basis for between-laboratory comparability, and as material for verifying laboratory performance. This effort verifies the certification of a 38 year old 241Pu Standard Reference Material (SRM4340) through alpha-gamma anticoincidence counting, and also establishes the separation date to two weeks of the documented date. PMID:29720779

A xenograft model reveals that PU.1 functions as a tumor suppressor for multiple myeloma in vivo

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nishimura, Nao; Endo, Shinya; Ueno, Shikiko

We previously demonstrated that PU.1 expression is down-regulated in the majority of myeloma cell lines and primary myeloma cells from patients. We introduced the tet-off system into the human myeloma cell lines U266 and KMS12PE that conditionally express PU.1 and demonstrated that PU.1 induces cell cycle arrest and apoptosis in myeloma cells in vitro. Here, we established a mouse xenograft model of myeloma using these cell lines to analyze the effects of PU.1 on the phenotype of myeloma cells in vivo. When doxycycline was added to the drinking water of mice engrafted with these myeloma cells, all mice had continuous growth ofmore » subcutaneous tumors and could not survived more than 65 days. In contrast, mice that were not exposed to doxycycline did not develop subcutaneous tumors and survived for at least 100 days. We next generated mice engrafted with subcutaneous tumors 5–10 mm in diameter that were induced by exposure to doxycycline. Half of the mice stopped taking doxycycline-containing water, whereas the other half kept taking the water. Although the tumors in the mice taking doxycycline continued to grow, tumor growth in the mice not taking doxycycline was significantly suppressed. The myeloma cells in the tumors of the mice not taking doxycycline expressed PU.1 and TRAIL and many of such cells were apoptotic. Moreover, the expression of a cell proliferation marker Ki67 was significantly decreased in tumors from the mice not taking doxycycline, compared with that of tumors from the mice continuously taking doxycycline. The present data strongly suggest that PU.1 functions as a tumor suppressor of myeloma cells in vivo. - Highlights: • PU.1 suppresses xenograft myeloma cell growth and prolongs survival periods of mice. • PU.1 induces TRAIL expression and apoptosis in myeloma cells in vivo. • PU.1 suppresses Ki67 expression in myeloma cells in vivo. • Up-regulation of PU.1 is a promising strategy for generating anti-myeloma agents.« less

Sources of the transuranic elements plutonium and neptunium in arctic marine sediments.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cooper, L. W.; Kelley, J. M.; Bond, L. A.

2000-01-01

We report here thermal ionization mass spectrometry measurements of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, {sup 242}Pu, and {sup 237}Np isolated from oceanic, estuarine, and riverine sediments from the Arctic Ocean Basin. {sup 238}Pu/{sup 239+240}Pu activity ratios are also reported for alpha spectrometric analyses undertaken on a subset of these samples. Our results indicate that the Pu in sediments on the Alaskan shelf and slope, as well as that in the deep basins (Amerasian and Eurasian) of the Arctic Ocean, has its origin in stratospheric and tropospheric fallout. Sediments from the Ob and Yenisei Rivers show isotopic Pu signatures thatmore » are distinctly different from those of northern-hemisphere stratospheric fallout and indicate the presence of weapons-grade Pu originating from nuclear fuel reprocessing wastes generated at Russian facilities within these river catchments. Consequently, sediments of the Eurasian Arctic Ocean, particularly those in the Barents and Kara Seas, probably contain a mixture of Pu from stratospheric fallout, tropospheric fallout, and fuel-reprocessing wastes of riverine origin. In particular, the {sup 241}Pu/{sup 239}Pu ratios observed in these sediments are inconsistent with significant contributions of Pu to the arctic sediments studied from western European reprocessing facilities, principally Sellafield in the UK. Several other potential sources of Pu to arctic sediments can also be excluded as significant based upon the transuranic isotope ratios presented.« less

Synergism between polyurethane and polydopamine in the synthesis of Ni-Fe alloy monoliths.

PubMed

Naresh Kumar, Thangavel; Sivabalan, Santhana; Chandrasekaran, Naveen; Phani, Kanala Lakshminarasimha

2015-02-04

Herein, we report the first synthesis of a light-weight macroporous 3-D alloy monolith of Ni-Fe/C using synergism between polydopamine (pDA) and polyurethane (pU); in situ formed polyurethane (pU) enables efficient mixing of pDA (carbon source) and Ni-FeOx resulting in Ni-Fe alloy monoliths at a temperature as low as ∼600 °C. The monolithic Ni-Fe/C exhibits enhanced oxygen evolution activity.

Use of boiled hexamethylenetetramine and urea to increase the porosity of cerium dioxide microspheres formed in the internal gelation process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hunt, R. D.; Collins, J. L.; Cowell, B. S.

Cerium dioxide (CeO 2) is a commonly used simulant for plutonium dioxide and for plutonium (Pu) in a mixed uranium (U) and Pu oxide [(U, Pu)O 2] in nuclear fuel development. This effort developed CeO 2 microspheres with different porosities and diameters for use in a crush-strength study. The internal gelation technique has produced CeO 2 microspheres with limited initial porosity. When an equal molar solution of urea and hexamethylenetetramine (HMTA) is gently boiling for 1 hr and used in the gelation process, the crystallite size and porosity of mixed U and thorium oxide microspheres and the (U, Pu)O 2more » microspheres increased significantly. In this study with cerium, the combination of ammonium cerium nitrate and 1-h boiled HMTA-urea failed to produce a stable feed broth. However, when the 1-h heated HMTA-urea was combined with unheated HMTA-urea in 1 to 3 volume ratio or the boiling time of the HMTA-urea was reduced to 15-20 min, a stable solution of HMTA, urea, and Ce was formed at 273 K. This new Ce solution produced CeO 2 microspheres with much higher initial porosities. Intermediate porosities were possible when the heated HMTA/urea was aged prior to use.« less

Use of boiled hexamethylenetetramine and urea to increase the porosity of cerium dioxide microspheres formed in the internal gelation process

DOE PAGES

Hunt, R. D.; Collins, J. L.; Cowell, B. S.

2017-05-13

Cerium dioxide (CeO 2) is a commonly used simulant for plutonium dioxide and for plutonium (Pu) in a mixed uranium (U) and Pu oxide [(U, Pu)O 2] in nuclear fuel development. This effort developed CeO 2 microspheres with different porosities and diameters for use in a crush-strength study. The internal gelation technique has produced CeO 2 microspheres with limited initial porosity. When an equal molar solution of urea and hexamethylenetetramine (HMTA) is gently boiling for 1 hr and used in the gelation process, the crystallite size and porosity of mixed U and thorium oxide microspheres and the (U, Pu)O 2more » microspheres increased significantly. In this study with cerium, the combination of ammonium cerium nitrate and 1-h boiled HMTA-urea failed to produce a stable feed broth. However, when the 1-h heated HMTA-urea was combined with unheated HMTA-urea in 1 to 3 volume ratio or the boiling time of the HMTA-urea was reduced to 15-20 min, a stable solution of HMTA, urea, and Ce was formed at 273 K. This new Ce solution produced CeO 2 microspheres with much higher initial porosities. Intermediate porosities were possible when the heated HMTA/urea was aged prior to use.« less

Fission fragment yields and total kinetic energy release in neutron-induced fission of235,238U,and239Pu

NASA Astrophysics Data System (ADS)

Tovesson, F.; Duke, D.; Geppert-Kleinrath, V.; Manning, B.; Mayorov, D.; Mosby, S.; Schmitt, K.

2018-03-01

Different aspects of the nuclear fission process have been studied at Los Alamos Neutron Science Center (LANSCE) using various instruments and experimental techniques. Properties of the fragments emitted in fission have been investigated using Frisch-grid ionization chambers, a Time Projection Chamber (TPC), and the SPIDER instrument which employs the 2v-2E method. These instruments and experimental techniques have been used to determine fission product mass yields, the energy dependent total kinetic energy (TKE) release, and anisotropy in neutron-induced fission of U-235, U-238 and Pu-239.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Syarifah, Ratna Dewi, E-mail: syarifah.physics@gmail.com; Suud, Zaki, E-mail: szaki@fi.itb.ac.id

Design study of small Pressurized Water Reactors (PWRs) core loaded with uranium nitride fuel (UN) and mixed nitride fuel (UN-PuN), Pa-231 as burnable poison, and Americium has been performed. Pa-231 known as actinide material, have large capture cross section and can be converted into fissile material that can be utilized to reduce excess reactivity. Americium is one of minor actinides with long half life. The objective of adding americium is to decrease nuclear spent fuel in the world. The neutronic analysis results show that mixed nitride fuel have k-inf greater than uranium nitride fuel. It is caused by the additionmore » of Pu-239 in mixed nitride fuel. In fuel fraction analysis, for uranium nitride fuel, the optimum volume fractions are 45% fuel fraction, 10% cladding and 45% moderator. In case of UN-PuN fuel, the optimum volume fractions are 30% fuel fraction, 10% cladding and 60% coolant/ moderator. The addition of Pa-231 as burnable poison for UN fuel, enrichment U-235 5%, with Pa-231 1.6% has k-inf more than one and excess reactivity of 14.45%. And for mixed nitride fuel, the lowest value of reactivity swing is when enrichment (U-235+Pu) 8% with Pa-231 0.4%, the excess reactivity value 13,76%. The fuel pin analyze for the addition of Americium, the excess reactivity value is lower than before, because Americium absorb the neutron. For UN fuel, enrichment U-235 8%, Pa-231 1.6% and Am 0.5%, the excess reactivity is 4.86%. And for mixed nitride fuel, when enrichment (U-235+Pu) 13%, Pa-231 0.4% and Am 0.1%, the excess reactivity is 11.94%. For core configuration, it is better to use heterogeneous than homogeneous core configuration, because the radial power distribution is better.« less

Selected Images of the Pu'u 'O'o-Kupaianaha Eruption, 1983-1997

USGS Publications Warehouse

Takahashi, Taeko Jane; Heliker, Christina C.; Diggles, Michael F.

2003-01-01

The 100 images in this CD?ROM have been selected from the collections of the Hawaiian Volcano Observatory as enduring favorites of the staff, researchers, media, designers, and the public over time. They represent photographs of a variety of geological phenomena and eruptive events, chosen for their content, quality of exposure, and aesthetic appeal. The number was kept to 100 to maintain the high resolution desirable. Since 1997, digital imagery has been the predominant mode of photographically documenting the eruption. Many of these photos, from 1998 to the present, are viewable on the website: http://hvo.wr.usgs.gov/kilauea/update/archive/ Episode numbers are given as E-numbers in parentheses before each caption that pertains to the Pu`u `O`o?Kupaianaha eruption; details of the episodes are given in table 1. Hawaiian words and place names are listed below to facilitate searching. All images included in this collection are owned by the U.S. Geological Survey, Hawaiian Volcano Observatory, and are in the public domain. Therefore, no permission or fee is required for their use. Please include photo credit for the photographer and the U.S. Geological Survey. We assume no responsibility for the modification of these images.

GGA + U studies of the early actinide mononitrides and dinitrides

NASA Astrophysics Data System (ADS)

Obodo, K. O.; Chetty, N.

2013-11-01

We present a detailed comparative study of the electronic and mechanical properties of the early actinide mononitrides and dinitrides within the framework of the Perdew-Burke-Ernzerhof generalized gradient approximation (GGA [PBE]) and GGA + U implementations of density functional theory with the inclusion of spin-orbit coupling. The dependence of selected observables of these materials on the effective U-parameter is investigated in detail. The properties include the lattice constant, bulk modulus, charge density distribution, hybridization of the atomic orbitals, energy of formation and the lattice dynamics. The inclusion of the Hubbard U parameter results in a proper description of the 5f electrons, and is subsequently used in the determination of the structural and electronic properties of these compounds. The mononitrides and dinitrides of the early actinides are metallic except for UN2, which is a semiconductor. These actinide nitrides are non-magnetic with the exception of UN, NpN, PuN, NpN2 and PuN2 that are magnetic systems with orbital-dependent magnetic moments oriented in the z-axis. We observed that ThN2 is elastically unstable to isotropic pressure. We discovered that UN2 is thermodynamically unstable, but may be stabilized by N vacancy formation.

Energy dependence of fission product yields from 235U, 238U, and 239Pu with monoenergetic neutrons between thermal and 14.8 MeV

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gooden, Matthew; Arnold, Charles; Bhike, Megha

Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements has been performed. The energy dependence of a number of cumulative fission product yields (FPY) have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of fission counting using specially designed dual-fission chambers and γ-ray counting. Each dual-fission chamber is a back-to-back ionization chamber encasing an activation target in the center with thin deposits of the same target isotope in each chamber. This method allows for the direct measurementmore » of the total number of fissions in the activation target with no reference to the fission cross-section, thus reducing uncertainties. γ-ray counting of the activation target was performed on well-shielded HPGe detectors over a period of two months post irradiation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 3.6, 4.6, 5.5, 7.5, 8.9 and 14.8 MeV. Preliminary results from thermal irradiations at the MIT research reactor will also be presented and compared to present data and evaluations.« less

Energy dependence of fission product yields from 235U, 238U, and 239Pu with monoenergetic neutrons between thermal and 14.8 MeV

DOE PAGES

Gooden, Matthew; Arnold, Charles; Bhike, Megha; ...

2017-09-13

Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements has been performed. The energy dependence of a number of cumulative fission product yields (FPY) have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of fission counting using specially designed dual-fission chambers and γ-ray counting. Each dual-fission chamber is a back-to-back ionization chamber encasing an activation target in the center with thin deposits of the same target isotope in each chamber. This method allows for the direct measurementmore » of the total number of fissions in the activation target with no reference to the fission cross-section, thus reducing uncertainties. γ-ray counting of the activation target was performed on well-shielded HPGe detectors over a period of two months post irradiation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 3.6, 4.6, 5.5, 7.5, 8.9 and 14.8 MeV. Preliminary results from thermal irradiations at the MIT research reactor will also be presented and compared to present data and evaluations.« less

Closed DTU fuel cycle with Np recycle and waste transmutation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Beller, D.E.; Sailor, W.C.; Venneri, F.

1999-09-01

A nuclear energy scenario for the 21st century that included a denatured thorium-uranium-oxide (DTU) fuel cycle and new light water reactors (LWRs) supported by accelerator-driven transmutation of waste (ATW) systems was previously described. This coupled system with the closed DTU fuel cycle provides several improvements beyond conventional LWR (CLWR) (once-through, UO{sub 2} fuel) nuclear technology: increased proliferation resistance, reduced waste, and efficient use of natural resources. However, like CLWR fuel cycles, the spent fuel in the first one-third core discharged after startup contains higher-quality Pu than the equilibrium fuel cycle. To eliminate this high-grade Pu, Np is separated and recycledmore » with Th and U--rather than with higher actinides [(HA) including Pu]. The presence of Np in the LWR feed greatly increases the production of {sup 238}Pu so that a few kilograms of Pu generated enough alpha-decay heat that the separated Pu is highly resistant to proliferation. This alternate process also simplifies the pyrochemical separation of fuel elements (Th and U) from HAs. To examine the advantages of this concept, the authors modeled a US deployment scenario for nuclear energy that includes DTU-LWRs plus ATW`s to burn the actinides produced by these LWRs and to close the back-end of the DTU fuel cycle.« less

Volcanology curricula development aided by online educational resource

USGS Publications Warehouse

Poland, Michael P.; van der Hoeven Kraft, Katrien J.; Teasdale, Rachel

2011-01-01

Volcanic activity is an excellent hook for engaging college and university students in geoscience classes. An increasing number of Internet-accessible real-time and near–real time volcano monitoring data are now available and constitute an important resource for geoscience education; however, relatively few data sets are comprehensive, and many lack background information to aid in interpretation. In response to the need for organized, accessible, and well-documented volcano education resources, the U.S. Geological Survey's Hawaiian Volcano Observatory (HVO), in collaboration with NASA and the University of Hawai`i at Manoa, established the Volcanoes Exploration Project: Pu`u `Ō`ō (VEPP). The VEPP Web site (http://vepp.wr.usgs.gov) is an educational resource that provides access, in near real time, to geodetic, seismic, and geologic data from the active Pu`u `Ō`ō eruptive vent on Kilauea volcano, Hawaii, along with background and context information. A strength of the VEPP site is the common theme of the Pu`u `Ō`ō eruption, which allows the site to be revisited multiple times to demonstrate different principles and integrate many aspects of volcanology.

Further evaluations of the toxicity of irradiated advanced heavy water reactor fuels.

PubMed

Edwards, Geoffrey W R; Priest, Nicholas D

2014-11-01

The neutron economy and online refueling capability of heavy water moderated reactors enable them to use many different fuel types, such as low enriched uranium, plutonium mixed with uranium, or plutonium and/or U mixed with thorium, in addition to their traditional natural uranium fuel. However, the toxicity and radiological protection methods for fuels other than natural uranium are not well established. A previous paper by the current authors compared the composition and toxicity of irradiated natural uranium to that of three potential advanced heavy water fuels not containing plutonium, and this work uses the same method to compare irradiated natural uranium to three other fuels that do contain plutonium in their initial composition. All three of the new fuels are assumed to incorporate plutonium isotopes characteristic of those that would be recovered from light water reactor fuel via reprocessing. The first fuel investigated is a homogeneous thorium-plutonium fuel designed for a once-through fuel cycle without reprocessing. The second fuel is a heterogeneous thorium-plutonium-U bundle, with graded enrichments of U in different parts of a single fuel assembly. This fuel is assumed to be part of a recycling scenario in which U from previously irradiated fuel is recovered. The third fuel is one in which plutonium and Am are mixed with natural uranium. Each of these fuels, because of the presence of plutonium in the initial composition, is determined to be considerably more radiotoxic than is standard natural uranium. Canadian nuclear safety regulations require that techniques be available for the measurement of 1 mSv of committed effective dose after exposure to irradiated fuel. For natural uranium fuel, the isotope Pu is a significant contributor to the committed effective dose after exposure, and thermal ionization mass spectrometry is sensitive enough that the amount of Pu excreted in urine is sufficient to estimate internal doses, from all isotopes, as low as 1 mSv. In addition, if this method is extended so that Pu is also measured, then the combined amount of Pu and Pu is sufficiently high in the thorium-plutonium fuel that a committed effective dose of 1 mSv would be measurable. However, the fraction of Pu and Pu in the other two fuels is sufficiently low that a 1 mSv dose would remain below the detection limit using this technique. Thus new methods, such as fecal measurements of Pu (or other alpha emitters), will be required to measure exposure to these new fuels.

Prompt fissionγ-ray characteristics from neutron-induced fission on 239Pu and the time-dependence of prompt-γray emission

NASA Astrophysics Data System (ADS)

Gatera, Angélique; Göök, Alf; Hambsch, Franz-Josef; Moens, André; Oberstedt, Andreas; Oberstedt, Stephan; Sibbens, Goedele; Vanleeuw, David; Vidali, Marzio

2018-03-01

Recent years have seen an increased interest in prompt fission γ-ray (PFG) measurements motivated by a high priority request of the OECD/NEA for high precision data, mainly for the nuclear fuel isotopes 235U and 239Pu. Our group has conducted a PFG measurement campaign using state-of-the-art lanthanum halide detectors for all the main actinides to a precision better than 3%. The experiments were performed in a coincidence setup between a fission trigger and γ-ray detectors. The time-of-flight technique was used to discriminate photons, traveling at the speed of light, and prompt fission neutrons. For a full rejection of all neutrons below 20 MeV, the PFG time window should not be wider than a few nanoseconds. This window includes most PFG, provided that no isomeric states were populated during the de-excitation process. When isomeric states are populated, PFGs can still be emitted up to 1 yus after the instant of fission or later. To study these γ-rays, the detector response to neutrons had to be determined and a correction had to be applied to the γ-ray spectra. The latest results for PFG characteristics from the reaction 239Pu(nth,f) will be presented, together with an analysis of PFGs emitted up to 200 ns after fission in the spontaneous fission of 252Cf as well as for thermal-neutron induced fission on 235U and 239Pu. The results are compared with calculations in the framework of the Hauser-Feshbach Monte Carlo code CGMF and FIFRELIN.

Radionuclide transfer to reptiles.

PubMed

Wood, Michael D; Beresford, Nicholas A; Semenov, Dmitry V; Yankovich, Tamara L; Copplestone, David

2010-11-01

Reptiles are an important, and often protected, component of many ecosystems but have rarely been fully considered within ecological risk assessments (ERA) due to a paucity of data on contaminant uptake and effects. This paper presents a meta-analysis of literature-derived environmental media (soil and water) to whole-body concentration ratios (CRs) for predicting the transfer of 35 elements (Am, As, B, Ba, Ca, Cd, Ce, Cm, Co, Cr, Cs, Cu, Fe, Hg, K, La, Mg, Mn, Mo, Na, Ni, Pb, Po, Pu, Ra, Rb, Sb, Se, Sr, Th, U, V, Y, Zn, Zr) to reptiles in freshwater ecosystems and 15 elements (Am, C, Cs, Cu, K, Mn, Ni, Pb, Po, Pu, Sr, Tc, Th, U, Zn) to reptiles in terrestrial ecosystems. These reptile CRs are compared with CRs for other vertebrate groups. Tissue distribution data are also presented along with data on the fractional mass of bone, kidney, liver and muscle in reptiles. Although the data were originally collected for use in radiation dose assessments, many of the CR data presented in this paper will also be useful for chemical ERA and for the assessments of dietary transfer in humans for whom reptiles constitute an important component of the diet, such as in Australian aboriginal communities.

Release of plutonium isotopes into the environment from the Fukushima Daiichi Nuclear Power Plant accident: what is known and what needs to be known.

PubMed

Zheng, Jian; Tagami, Keiko; Uchida, Shigeo

2013-09-03

The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has caused serious contamination in the environment. The release of Pu isotopes renewed considerable public concern because they present a large risk for internal radiation exposure. In this Critical Review, we summarize and analyze published studies related to the release of Pu from the FDNPP accident based on environmental sample analyses and the ORIGEN model simulations. Our analysis emphasizes the environmental distribution of released Pu isotopes, information on Pu isotopic composition for source identification of Pu releases in the FDNPP-damaged reactors or spent fuel pools, and estimation of the amounts of Pu isotopes released from the FDNPP accident. Our analysis indicates that a trace amount of Pu isotopes (∼2 × 10(-5)% of core inventory) was released into the environment from the damaged reactors but not from the spent fuel pools located in the reactor buildings. Regarding the possible Pu contamination in the marine environment, limited studies suggest that no extra Pu input from the FDNPP accident could be detected in the western North Pacific 30 km off the Fukushima coast. Finally, we identified knowledge gaps remained on the release of Pu into the environment and recommended issues for future studies.

Simulation of Fast Neutronics in an Accelerator-Driven Sub-Critical Core

NASA Astrophysics Data System (ADS)

Gwyn Rosaire, C.; Sattarov, Akhdiyor; McIntyre, Peter; Tsvetkov, Pavel

2011-10-01

Accelerator-driven subcritical fission in a molten salt core (ADSMS) is being developed as a technology for green nuclear power. ADSMS burns its fertile fuel to completion, it cannot melt down, and it destroys long-lived minor actinides. The ADSMS core consists of a vessel filled with a molten salt eutectic of UCl3 and NaCl. The fast neutronics of ADSMS makes possible two unique benefits: isobreeding, a steady-state equilibrium in which ^238U is bred to ^239Pu and the ^239Pu fissions, and destruction of minor actinides, in which fission of the intermediary nuclides dominates of breeding. Results of simulations of the fast neutronics in the ADSMS core will be presented.

Advancing Understanding of the +4 Metal Extractant Thenoyltrifluoroacetonate (TTA –); Synthesis and Structure of M IVTTA 4 (M IV = Zr, Hf, Ce, Th, U, Np, Pu) and M III(TTA) 4 – (M III = Ce, Nd, Sm, Yb)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cary, Samantha K.; Livshits, Maksim; Cross, Justin N.

Thenoyltrifluoroacetone (HTTA)-based extractions represent popular methods for separating microscopic amounts of transuranic actinides (i.e., Np and Pu) from macroscopic actinide matrixes (e.g. bulk uranium). It is well-established that this procedure enables +4 actinides to be selectively removed from +3, + 5, and +6 f-elements. However, even highly skilled and well-trained researchers find this process complicated and (at times) unpredictable. It is difficult to improve the HTTA extraction—or find alternatives—because little is understood about why this separation works. Even the identities of the extracted species are unknown. In addressing this knowledge gap, we report in this paper advances in fundamental understandingmore » of the HTTA-based extraction. This effort included comparatively evaluating HTTA complexation with +4 and +3 metals (M IV = Zr, Hf, Ce, Th, U, Np, and Pu vs M III = Ce, Nd, Sm, and Yb). We observed +4 metals formed neutral complexes of the general formula M IV(TTA) 4. Meanwhile, +3 metals formed anionic M III(TTA) 4 – species. Characterization of these M(TTA) 4 x– (x = 0, 1) compounds by UV–vis–NIR, IR, 1H and 19F NMR, single-crystal X-ray diffraction, and X-ray absorption spectroscopy (both near-edge and extended fine structure) was critical for determining that Np IV(TTA) 4 and Pu IV(TTA) 4 were the primary species extracted by HTTA. Furthermore, this information lays the foundation to begin developing and understanding of why the HTTA extraction works so well. The data suggest that the solubility differences between M IV(TTA) 4 and M III(TTA) 4 – are likely a major contributor to the selectivity of HTTA extractions for +4 cations over +3 metals. Finally and moreover, these results will enable future studies focused on explaining HTTA extractions preference for +4 cations, which increases from Np IV to Pu IV, Hf IV, and Zr IV.« less

Advancing Understanding of the +4 Metal Extractant Thenoyltrifluoroacetonate (TTA –); Synthesis and Structure of M IVTTA 4 (M IV = Zr, Hf, Ce, Th, U, Np, Pu) and M III(TTA) 4 – (M III = Ce, Nd, Sm, Yb)

DOE PAGES

Cary, Samantha K.; Livshits, Maksim; Cross, Justin N.; ...

2018-03-21

Thenoyltrifluoroacetone (HTTA)-based extractions represent popular methods for separating microscopic amounts of transuranic actinides (i.e., Np and Pu) from macroscopic actinide matrixes (e.g. bulk uranium). It is well-established that this procedure enables +4 actinides to be selectively removed from +3, + 5, and +6 f-elements. However, even highly skilled and well-trained researchers find this process complicated and (at times) unpredictable. It is difficult to improve the HTTA extraction—or find alternatives—because little is understood about why this separation works. Even the identities of the extracted species are unknown. In addressing this knowledge gap, we report in this paper advances in fundamental understandingmore » of the HTTA-based extraction. This effort included comparatively evaluating HTTA complexation with +4 and +3 metals (M IV = Zr, Hf, Ce, Th, U, Np, and Pu vs M III = Ce, Nd, Sm, and Yb). We observed +4 metals formed neutral complexes of the general formula M IV(TTA) 4. Meanwhile, +3 metals formed anionic M III(TTA) 4 – species. Characterization of these M(TTA) 4 x– (x = 0, 1) compounds by UV–vis–NIR, IR, 1H and 19F NMR, single-crystal X-ray diffraction, and X-ray absorption spectroscopy (both near-edge and extended fine structure) was critical for determining that Np IV(TTA) 4 and Pu IV(TTA) 4 were the primary species extracted by HTTA. Furthermore, this information lays the foundation to begin developing and understanding of why the HTTA extraction works so well. The data suggest that the solubility differences between M IV(TTA) 4 and M III(TTA) 4 – are likely a major contributor to the selectivity of HTTA extractions for +4 cations over +3 metals. Finally and moreover, these results will enable future studies focused on explaining HTTA extractions preference for +4 cations, which increases from Np IV to Pu IV, Hf IV, and Zr IV.« less

Repeated deflation-inflation events at Kilauea Volcano, Hawai'i: What's up (and down) with that?

NASA Astrophysics Data System (ADS)

Poland, M. P.; Miklius, A.; Lundgren, P.; Sutton, A. J.

2011-12-01

Cyclic deflation-inflation ("DI") events are a common occurrence at Kilauea Volcano. Most DI events begin with deflation at the summit that generally lasts 12-72 hours and accumulate ~1-5 microradians of tilt as measured on the rim of Kilauea caldera, followed by inflation that is initially rapid but wanes as the net deformation approaches pre-event levels over the course of 12-48 hours. In rare cases, the initial deflation is followed by large-magnitude (~20 microradians) inflation over a few hours followed by hours to days of deflation to pre-event levels. Such DID events have only been recorded during 2000-2004. DI events are also manifested at the Pu'u 'O'o eruptive vent on Kilauea's east rift zone, about 15 km from the summit, and lag summit deformation by about 1-2 hours. For DI events with relatively large-magnitudes (i.e., several microradians) and long-durations (i.e., several days), deformation is manifested along the east rift zone between Pu'u 'O'o and the summit, and eruptive activity at Pu'u 'O'o is impacted with long periods of deflation and inflation associated with eruptive pauses and surges, respectively. During a period of increased magma transport between the summit and Pu'u 'O'o in 2005-2007, DI events recorded at the summit were not detected at Pu'u 'O'o. Since the March 2008 start of Kilauea's ongoing summit eruption, the number of DI events per year has increased from about 5-10 to about 50-60. The level of the summit lava column (continuously visible since early 2010), has generally tracked DI deformation. Surface deformation associated with DI events is measured by tilt, GPS, and InSAR. At the summit, preliminary source models suggest a depth of 1-2 km and a sill-like geometry beneath the center of the caldera, with volume loss and subsequent recovery on the order of tens of thousands of cubic meters with each DI cycle. The localized nature of the DI signal at Pu'u 'O'o argues for a shallow source that is probably less than 1 km deep. At least two mechanisms are consistent with the occurrence of DI events at Kilauea. First, blockage and subsequent clearing of the transport pathway that feeds the shallow summit magma system and conduit to Pu'u 'O'o could cause the observed deformation. A second possibility is that DI events represent convective overturns caused by replacement of degassed magma with gas-rich magma. Such a model is consistent with the increased number of DI events following the onset of Kilauea's summit eruption, when summit gas emissions increased by a factor of about 5, but there have been no changes in degassing rates during periods of frequent (i.e., daily) or rare (i.e., monthly) DI events during 2008-2011. The source of DI events therefore remains a target of continued study.

The need for precise and well-documented experimental data on prompt fission neutron spectra from neutron-induced fission of 239Pu

DOE PAGES

Neudecker, Denise; Taddeucci, Terry Nicholas; Haight, Robert Cameron; ...

2016-01-06

The spectrum of neutrons emitted promptly after 239Pu(n,f)—a so-called prompt fission neutron spectrum (PFNS)—is a quantity of high interest, for instance, for reactor physics and global security. However, there are only few experimental data sets available that are suitable for evaluations. In addition, some of those data sets differ by more than their 1-σ uncertainty boundaries. We present the results of MCNP studies indicating that these differences are partly caused by underestimated multiple scattering contributions, over-corrected background, and inconsistent deconvolution methods. A detailed uncertainty quantification for suitable experimental data was undertaken including these effects, and test-evaluations were performed with themore » improved uncertainty information. The test-evaluations illustrate that the inadequately estimated effects and detailed uncertainty quantification have an impact on the evaluated PFNS and associated uncertainties as well as the neutron multiplicity of selected critical assemblies. A summary of data and documentation needs to improve the quality of the experimental database is provided based on the results of simulations and test-evaluations. Furthermore, given the possibly substantial distortion of the PFNS by multiple scattering and background effects, special care should be taken to reduce these effects in future measurements, e.g., by measuring the 239Pu PFNS as a ratio to either the 235U or 252Cf PFNS.« less

Estimation of the formation rates of polyatomic species of heavy metals in plutonium analyses using a multicollector ICP-MS with a desolvating nebulizer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mitroshkov, Alexandre V.; Olsen, Khris B.; Thomas, Linda M.

2015-01-01

The analyses of IAEA and environmental samples for Plutonium isotopic content are conducted normally at very low concentrations of Pu–usually in the range of part per trillion level and even more often at the parts per quadrillion level. To analyze such low concentrations, the interferences in the analytical solution must be reduced as much as possible. Polyatomic interferences (PIs), formed by the heavy metals (HMs) from Hf to Bi are known to create the problems for Pu isotopic analyses, because even the relatively high resolution of a modern multicollector ICP-MS is not enough to separate Pu isotopes from this PIsmore » in most of the cases. Desolvating nebulizers (DSN) (e.g. APEX and AridusII) reduce significantly the formation of PIs compare to the use of wet plasma. The purpose of this work was to investigate the rate of formation of PIs, produced by HMs, when high resolution MC ICP-MS with desolvating nebulizer was used for Pu isotopic analyses and to estimate the influence of the metals present in the sample on the results of analyses. The NU Plasma HR Multicollector and AridusII desolvating nebulizer were used in this investigation. This investigation was done for all Pu isotopes normally analyzed by ICP-MS, including ²⁴⁴Pu, with the exception of ²³⁸Pu, which most of the time can’t be analyzed by ICP-MS, because of the overwhelming presence of ²³⁸U in the solutions. The PI formation rates were determined and reported for all 12 HMs from Hf to Bi. Selected IAEA samples were scanned for the presence of HMs and the influence of HMs on the results of Pu isotopic analyses was evaluated. It was found that the implemented separation procedure provides sufficient separation of HM from Pu, although the effect of PIs on the measurement of low level isotopes like ²⁴¹Pu and ²⁴²Pu in some cases can still be observed.« less

Renewability and sustainability aspects of nuclear energy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Şahin, Sümer, E-mail: ssahin@atilim.edit.tr

Renewability and sustainability aspects of nuclear energy have been presented on the basis of two different technologies: (1) Conventional nuclear technology; CANDU reactors. (2) Emerging nuclear technology; fusion/fission (hybrid) reactors. Reactor grade (RG) plutonium, {sup 233}U fuels and heavy water moderator have given a good combination with respect to neutron economy so that mixed fuel made of (ThO{sub 2}/RG‐PuO{sub 2}) or (ThC/RG-PuC) has lead to very high burn up grades. Five different mixed fuel have been selected for CANDU reactors composed of 4 % RG‐PuO{sub 2} + 96 % ThO{sub 2}; 6 % RG‐PuO{sub 2} + 94 % ThO{sub 2};more » 10 % RG‐PuO{sub 2} + 90 % ThO{sub 2}; 20 % RG‐PuO{sub 2} + 80 % ThO{sub 2}; 30 % RG‐PuO{sub 2} + 70 % ThO{sub 2}, uniformly taken in each fuel rod in a fuel channel. Corresponding operation lifetimes have been found as ∼ 0.65, 1.1, 1.9, 3.5, and 4.8 years and with burn ups of ∼ 30 000, 60 000, 100 000, 200 000 and 290 000 MW.d/ton, respectively. Increase of RG‐PuO{sub 2} fraction in radial direction for the purpose of power flattening in the CANDU fuel bundle has driven the burn up grade to 580 000 MW.d/ton level. A laser fusion driver power of 500 MW{sub th} has been investigated to burn the minor actinides (MA) out of the nuclear waste of LWRs. MA have been homogenously dispersed as carbide fuel in form of TRISO particles with volume fractions of 0, 2, 3, 4 and 5 % in the Flibe coolant zone in the blanket surrounding the fusion chamber. Tritium breeding for a continuous operation of the fusion reactor is calculated as TBR = 1.134, 1.286, 1.387, 1.52 and 1.67, respectively. Fission reactions in the MA fuel under high energetic fusion neutrons have lead to the multiplication of the fusion energy by a factor of M = 3.3, 4.6, 6.15 and 8.1 with 2, 3, 4 and 5 % TRISO volume fraction at start up, respectively. Alternatively with thorium, the same fusion driver would produce ∼160 kg {sup 233}U per year in addition to fission energy production in situ, multiplying the fusion energy by a factor of ∼1.3.« less

INNOVATIVE TECHNOLOGY VERIFICATION REPORT "FIELD MEASUREMENT TECHNOLOGIES FOR TOTAL PETROLEUM HYDROCARBONS IN SOIL" WILKS ENTERPRISE, INC. INFRACAL TOG/TPH ANALYZER

EPA Science Inventory

The hifracal' TOG/TPH Analyzer developed by Wilks Enterprise, Inc. (Wilks), was demonstrated under the U.S. Environmental Protection Agency Superfund Innovative Technology Evaluation Program in June 2000 at the Navy Base Ventura County site in Port Hueneme, California. The pu...

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reilly, Sean Douglas; Smith, Paul Herrick; Jarvinen, Gordon D.

Understanding the water solubility of plutonium and uranium compounds and residues at TA-55 is necessary to provide a technical basis for appropriate criticality safety, safety basis and accountability controls. Individual compound solubility was determined using published solubility data and solution thermodynamic modeling. Residue solubility was estimated using a combination of published technical reports and process knowledge of constituent compounds. The scope of materials considered includes all compounds and residues at TA-55 as of March 2016 that contain Pu-239 or U-235 where any single item in the facility has more than 500 g of nuclear material. This analysis indicates that themore » following materials are not appreciably soluble in water: plutonium dioxide (IDC=C21), plutonium phosphate (IDC=C66), plutonium tetrafluoride (IDC=C80), plutonium filter residue (IDC=R26), plutonium hydroxide precipitate (IDC=R41), plutonium DOR salt (IDC=R42), plutonium incinerator ash (IDC=R47), uranium carbide (IDC=C13), uranium dioxide (IDC=C21), U 3O 8 (IDC=C88), and uranium filter residue (IDC=R26). This analysis also indicates that the following materials are soluble in water: plutonium chloride (IDC=C19) and uranium nitrate (IDC=C52). Equilibrium calculations suggest that PuOCl is water soluble under certain conditions, but some plutonium processing reports indicate that it is insoluble when present in electrorefining residues (R65). Plutonium molten salt extraction residues (IDC=R83) contain significant quantities of PuCl 3, and are expected to be soluble in water. The solubility of the following plutonium residues is indeterminate due to conflicting reports, insufficient process knowledge or process-dependent composition: calcium salt (IDC=R09), electrorefining salt (IDC=R65), salt (IDC=R71), silica (IDC=R73) and sweepings/screenings (IDC=R78). Solution thermodynamic modeling also indicates that fire suppression water buffered with a commercially-available phosphate buffer would significantly reduce the solubility of PuCl 3 by the precipitation of PuPO 4.« less

Creation of a sharp compositional interface in the Pu`u `O`o shallow magma reservoir, Kilauea volcano, Hawai`i

NASA Astrophysics Data System (ADS)

Mittelstaedt, E.; Garcia, M. O.

2006-12-01

Lavas from the early episodes of the Pu`u `O`O eruption (1983-85) of Kilauea Volcano on the island of Hawai'i display rapid compositional variation over short periods for some episodes, especially from the well sampled episode 30 with ~2 wt% MgO variation in <4 hours. Little chemical variation is observed within the episode 30 lavas before or after this abrupt change suggesting a sharp compositional interface within the Pu`u `O`o dike-like shallow reservoir. The change in lava composition throughout the eruption is due to changes in cooling within the dike-like shallow reservoir of Pu`u `O`o. Potential explanations for a sharp interface, such as a reservoir of changing width and changing country rock thermal properties, are evaluated using a simple thermal model of a dike-like body with spatially variable thermal conductivity. The model that best reproduces the compositional data involves a change in thermal conductivity from 2.7 to 11 W m-1 C-1. which is consistent with deep drill hole data in the east rift zone. The change in thermal conductivity may indicate that fluid flow in the east rift zone is restricted at depth possibly by increasing numbers of dikes acting as acuacludes or decreasing pore space due to formation of secondary minerals. Results suggest that country rock thermal gradients can strongly influence magma chemistry in shallow reservoirs.

[Noninvasive estimation of human tissue respiration with wavelet-analysis of oxygen saturation and blood flow oscillations in microvessels].

PubMed

Krupatkin, A I

2012-01-01

Laser Doppler flowmetry, laser spectrophotometry of oxygen saturation and fluorescence determination of NAD-H/FAD ratio were carried out at 30 humans in the upper extremity skin zones with and without arteriole-venule anastomoses (AVA). For the first time it was shown that wavelet-analysis of oxygen saturation and microvascular blood flow oscillations was an effective approach to noninvasive estimation of skin oxygen extraction (OE) and oxygen consumption rate (OC). OE = (SaO2--SvO2)/SaO2, where SaO2 (%) and SvO2(%) are the oxygen saturation of arterial and venular blood, correspondingly. If the ratio between amplitudes of cardiac rhythm (Ac, p.u.) and respiratory rhythm (Ar, p.u.) Ac/Ar < or = 1, SvO2 = SO2. In the case of Ac/Ar >1, SvO2 = SO2/(Ac/Ar). OC = Mnutr x (SaO2-SvO2) in p.u. x %O2, where Mnutr--value of nutritive perfusion (p.u.). Mnutr = M/SI, where SI--shunting index of blood flow in microvessels. The values of perfusion, OE and OC were higher in the skin with AVA than in the skin without AVA. The values of perfusion and oxygen saturation were more variable in the skin with AVA. The greatest significance for tissue metabolism have the oxygen diffused from the smallest arterioles and capillaries. The contribution increased to tissue metabolism of total perfusion and of oxygen diffused from arterioles in the conditions of tissue ischemia.

Tank 241-U-103, grab samples 3U-99-1, 3u-99-2 and 3U-99-3

DOE Office of Scientific and Technical Information (OSTI.GOV)

STEEN, F.H.

This document is the final report for tank 241-U-103 grab samples. Three grab samples were collected from riser 13 on March 12, 1999 and received by the 222-S laboratory on March 15, 1999. Analyses were performed in accordance with the Compatibility Grab Sampling and Analysis Plan for Fiscal year 1999 (TSAP) and the Data Quality Objectives for Tank Farms Waste Compatibility Program (DQO). The analytical results are presented in the data summary report. None of the subsamples submitted for differential scanning calorimetry (DSC), total organic carbon (TOC) and plutonium 239 (Pu239) analyses exceeded the notification limits as stated in TSAP.

Multidimensional team-based intervention using musical cues to reduce odds of facility-acquired pressure ulcers in long-term care: a paired randomized intervention study.

PubMed

Yap, Tracey L; Kennerly, Susan M; Simmons, Mark R; Buncher, Charles R; Miller, Elaine; Kim, Jay; Yap, Winston Y

2013-09-01

To test the effectiveness of a pressure ulcer (PU) prevention intervention featuring musical cues to remind all long-term care (LTC) staff (nursing and ancillary) to help every resident move or reposition every 2 hours. Twelve-month paired-facility two-arm (with one-arm crossover) randomized intervention trial. Ten midwestern U.S. LTC facilities. Four treatment facilities received intervention during Months 1 to 12, four comparison facilities received intervention during Months 7 to 12, and two pseudo-control facilities received no intervention. LTC facility residents (N = 1,928). All facility staff received in-person education, video, and handouts, and visiting family members received informational pamphlets on PU prevention and an intervention featuring musical cues. Nurse-led multidisciplinary staff teams presented the cues as prompts for staff and family to reposition residents or remind them to move. Musical selections (with and without lyrics) customized to facility preferences were played daily over the facility intercom or public address system every 2 hours for the 12-hour daytime period. Primary outcome measure was the frequency of new facility-acquired PUs divided by the total number of facility Minimum Data Set (MDS) resident assessments conducted during the study period. Odds of a new PU were lower in intervention facilities (P = .08) for MDS 2.0 assessments and were significantly lower (P = .05) for MDS 3.0. Mean odds ratios suggested intervention facility residents were 45% less likely than comparison facility residents to develop a new PU. Customized musical cues that prompt multidisciplinary staff teams to encourage or enable movement of all residents hold promise for reducing facility-acquired PUs in LTC settings. © 2013, Copyright the Authors Journal compilation © 2013, The American Geriatrics Society.

Radiotoxicity Characterization of Multi-Recycled Thorium Fuel - 12394

DOE Office of Scientific and Technical Information (OSTI.GOV)

Franceschini, F.; Wenner, M.; Fiorina, C.

2012-07-01

As described in companion papers, Westinghouse is proposing the implementation of a thorium based fuel cycle to burn the transuranic (TRU) contained in the used nuclear fuel. The potential of thorium as a TRU burner is described in another paper presented at this conference. This paper analyzes the long-term impact of thorium on the front-end and backend of the fuel cycle. This is accomplished by an assessment of the isotopic make-up of Th in a closed cycle and its impact on representative metrics, such as radiotoxicity, decay heat and gamma heat. The behavior in both thermal and fast neutron energymore » ranges has been investigated. Irradiation in a Th fuel PWR has been assumed as representative of the thermal range, while a Th fuel fast reactor (FR) has been employed to characterize the behavior in the high-energy range. A comparison with a U-fuel closed-cycle FR has been undertaken in an attempt of a more comprehensive evaluation of each cycle's long-term potential. As the Th fuel undergoes multiple cycles of irradiation, the isotopic composition of the recycled fuel changes. Minor Th isotopes are produced; U-232 and Pa-231 build up; the U vector gradually shifts towards increasing amounts of U-234, U-235 etc., eventually leading to the production of non negligible amounts of TRU isotopes, especially Pu-238. The impact of the recycled fuel isotopic makeup on the in-core behavior is mild, and for some aspects beneficial, i.e. the reactivity swing during irradiation is reduced as the fertile characteristics of the fuel increase. On the other hand, the front and the back-end of the fuel cycle are negatively affected due to the presence of Th-228 and U-232 and the build-up of higher actinides (Pu-238 etc.). The presence of U-232 can also be seen as advantageous as it represents an obstacle to potential proliferators. Notwithstanding the increase in the short-term radiotoxicity and decay heat in the multi-recycled fuel, the Th closed cycle has some potentially substantial advantages compared to the U cycle, such as the smaller actinide radiotoxicity and decay heat for up to 25,000 years after irradiation. In order for these benefits to materialize, the capability to reprocess and remotely manufacture industrial amounts of recycled fuel appears to be the key. Westinghouse is proposing the implementation of a thorium based fuel cycle to burn the TRU contained in the current UNF. The general approach and the potential of thorium as TRU burner is described in other papers presented at this conference. The focus of this paper is to analyze the long-term potential of thorium, once the legacy TRU has been exhausted and the thorium reactor system will become self-sufficient. Therefore, a comparison of Th closed cycle, in fast and thermal neutron energy ranges, vs. U closed cycle, in the fast energy range, has been undertaken. The results presented focus on selected backend and front-end metrics: isotopic actinide composition and potential implications on ingested radiotoxicity, decay heat and gamma heat. The evaluation confirms potential substantial improvements in the backend of the fuel cycle by transitioning to a thorium closed cycle. These benefits are the result of a much lower TRU content, in particular Pu-241, Am-241 and Pu-240, characterizing the Th vs. U actinide inventories, and the ensuing process waste to be disposed. On the other hand, the larger gamma activity of Th recycled fuel, consisting predominantly of hard gammas from U-232's decay products, is a significant challenge for fuel handling, transportation and manufacturing but can be claimed as beneficial for the proliferation resistance of the fuel. It is worth remembering that in our perspective the Th closed cycle and the U closed cycle will follow a transmutation phase which will likely take place over several decades and dictate the technologies required. These will likely include remote fuel manufacturing, regardless of the specific system adopted for the transmutation, which could then be inherited for the ensuing closed cycles. Finally, specific data related to the fuel manufacturing and separation technologies and their performance in the prospected industrial scale deployment, are key for further quantification of the potential merits of the options explored. Further studies in this direction should be warranted before making definitive conclusion. (authors)« less

Plutonium-uranium mixed oxide characterization by coupling micro-X-ray diffraction and absorption investigations

NASA Astrophysics Data System (ADS)

Degueldre, C.; Martin, M.; Kuri, G.; Grolimund, D.; Borca, C.

2011-09-01

Plutonium-uranium mixed oxide (MOX) fuels are currently used in nuclear reactors. The potential differences of metal redox state and microstructural developments of the matrix before and after irradiation are commonly analysed by electron probe microanalysis. In this work the structure and next-neighbor atomic environments of Pu and U oxide features within unirradiated homogeneous MOX and irradiated (60 MW d kg -1) MOX samples was analysed by micro-X-ray fluorescence (μ-XRF), micro-X-ray diffraction (μ-XRD) and micro-X-ray absorption fine structure (μ-XAFS) spectroscopy. The grain properties, chemical bonding, valences and stoichiometry of Pu and U are determined from the experimental data gained for the unirradiated as well as for irradiated fuel material examined in the center of the fuel as well as in its peripheral zone (rim). The formation of sub-grains is observed as well as their development from the center to the rim (polygonization). In the irradiated sample Pu remains tetravalent (>95%) and no (<5%) Pu(V) or Pu(VI) can be detected while the fuel could undergo slight oxidation in the rim zone. Any slight potential plutonium oxidation is buffered by the uranium dioxide matrix while locally fuel cladding interaction could also affect the redox of the fuel.

MA transmutation performance in the optimized MYRRHA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Malambu, E.; Van den Eynde, G.; Fernandez, R.

MYRRHA (multi-purpose hybrid research reactor for high-tech applications) is a multipurpose research facility currently being developed at SCK-CEN. It will be able to work in both critical and subcritical modes and, cooled by lead-bismuth eutectic. In this paper the minor actinides (MA) transmutation capabilities of MYRRHA are investigated. (Pu + Am, U) MOX fuel and (Np + Am + Cm, Pu) Inert Matrix Fuel test samples have been loaded in the central channel of the MYRRHA critical core and have been irradiated during five cycles, each one consisting of 90 days of operation at 100 MWth and 30 days ofmore » shutdown. The reactivity worth of the test fuel assembly was about 1.1 dollar. A wide range of burn-up level has been achieved, extending from 42 to 110 MWd/kg HM, the samples with lower MA-to-Pu ratios reaching the highest burn-up. This study has highlighted the importance of the initial MA content, expressed in terms of MA/Pu ratio, on the transmutation rate of MA elements. For (Pu + Am, U) MOX fuel samples, a net build-up of MA is observed when the initial content of MA is very low (here, 1.77 wt% MA/Pu) while a net decrease in MA is observed in the sample with an initial content of 5 wt%. This suggests the existence of some 'equilibrium' initial MA content value beyond which a net transmutation is achievable.« less

Differential die-away analysis system response modeling and detector design

NASA Astrophysics Data System (ADS)

Jordan, K. A.; Gozani, T.; Vujic, J.

2008-05-01

Differential die-away-analysis (DDAA) is a sensitive technique to detect presence of fissile materials such as 235U and 239Pu. DDAA uses a high-energy (14 MeV) pulsed neutron generator to interrogate a shipping container. The signature is a fast neutron signal hundreds of microseconds after the cessation of the neutron pulse. This fast neutron signal has decay time identical to the thermal neutron diffusion decay time of the inspected cargo. The theoretical aspects of a cargo inspection system based on the differential die-away technique are explored. A detailed mathematical model of the system is developed, and experimental results validating this model are presented.

STATUS REPORT: EVIDENCE BASED ADVANCES IN ...

EPA Pesticide Factsheets

This report summarizes the status of specific inhalation dosimetry procedures for gases as outlined in U.S. EPA’s 1994 Methods for Derivation of Inhalation Reference Concentrations and Applications of Inhalation Dosimetry (U.S. EPA 1994) and reviews recent scientific advances in gas dosimetry related to these procedures. These procedures are used predominately for interspecies extrapolation, typically from laboratory animal inhalation exposures to humans. The specific procedures addressed in this report are those used for the tracheobronchial (TB) and pulmonary (PU) regions of the respiratory tract and the procedure used for the systemic or extrarespiratory (ER) region. In addition, this report presents, reviews and discusses information and data on inhalation dosimetry in children and the adequacy of the procedures in the RfC Methods with regard to children. For the purposes of this report the scientific literature was searched from 1985 (about 10 years prior to the issuance of RfC Methods) to April 30, 2011. The studies identified in this update addressing overall concepts and approaches for portal-of-entry gas dosimetry in the TB and PU regions of the airways support the principles and procedures in RfC Methods. In some cases these studies suggest and provide examples of further refinement within the existing dosimetry modeling framework of the RfC Methods through development and application of mass transfer coefficients as regional measures of gas up

Chemical thermodynamic representations of and

DOE Office of Scientific and Technical Information (OSTI.GOV)

Besmann, T.M.; Lindemer, T.B.

1984-01-01

All available oxygen potential-temperature-composition data for the calcium fluorite-structure phase were retrieved from the literature and utilized in the development of a binary solid solution representation of the phase. The data and phase relations are found to be best described by a solution of (Pu/sub 4/3/O/sub 2/) and (PuO/sub 2/) with a temperature dependent interaction energy. The fluorite-structure is assumed to be represented by a combination of the binaries and , and thus treated as a solution of (Pu/sub 4/3/O/sub 2/), (PuO/sub 2/), (UO/sub 2/), and either (U/sub 2/O/sub 4/./sub 5/) or (U/sub 3/O/sub 7/). The resulting equations wellmore » reproduce the large amount of oxygen potential-temperature-composition data for the mixed oxide system, all of which were also retrieved from the literature. These models are the first that appear to display the appropriate oxygen potential-temperature-composition and phase relation behavior over the entire range of existence for the phases. 39 refs., 10 figs., 3 tabs.« less

Static electric dipole polarizabilities of tri- and tetravalent U, Np, and Pu ions.

PubMed

Parmar, Payal; Peterson, Kirk A; Clark, Aurora E

2013-11-21

High-quality static electric dipole polarizabilities have been determined for the ground states of the hard-sphere cations of U, Np, and Pu in the III and IV oxidation states. The polarizabilities have been calculated using the numerical finite field technique in a four-component relativistic framework. Methods including Fock-space coupled cluster (FSCC) and Kramers-restricted configuration interaction (KRCI) have been performed in order to account for electron correlation effects. Comparisons between polarizabilities calculated using Dirac-Hartree-Fock (DHF), FSCC, and KRCI methods have been made using both triple- and quadruple-ζ basis sets for U(4+). In addition to the ground state, this study also reports the polarizability data for the first two excited states of U(3+/4+), Np(3+/4+), and Pu(3+/4+) ions at different levels of theory. The values reported in this work are the most accurate to date calculations for the dipole polarizabilities of the hard-sphere tri- and tetravalent actinide ions and may serve as reference values, aiding in the calculation of various electronic and response properties (for example, intermolecular forces, optical properties, etc.) relevant to the nuclear fuel cycle and material science applications.

Study on reduction and back extraction of Pu(IV) by urea derivatives in nitric acid conditions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ye, G.A.; Xiao, S.T.; Yan, T.H.

2013-07-01

The reduction kinetics of Pu(IV) by hydroxyl-semicarbazide (HSC), hydroxyurea (HU) and di-hydroxyurea (DHU) in nitric acid solutions were investigated separately with adequate kinetic equations. In addition, counter-current cascade experiments were conducted for Pu split from U in nitric acid media using three kinds of reductant, respectively. The results show that urea derivatives as a kind of novel salt-free reductant can reduce Pu(IV) to Pu(III) rapidly in the nitric acid solutions. The stripping experimental results showed that Pu(IV) in the organic phase can be stripped rapidly to the aqueous phase by the urea derivatives, and the separation factors of plutonium /uraniummore » can reach more than 10{sup 4}. This indicates that urea derivatives is a kind of promising salt-free agent for uranium/plutonium separation. In addition, the complexing effect of HSC with Np(IV) was revealed, and Np(IV) can be back-extracted by HSC with a separation factor of about 20.« less

Short Lived Fission Product Yield Measurements in 235U, 238U and 239Pu

NASA Astrophysics Data System (ADS)

Silano, Jack; Tonchev, Anton; Tornow, Werner; Krishichayan, Fnu; Finch, Sean; Gooden, Matthew; Wilhelmy, Jerry

2017-09-01

Yields of short lived fission products (FPYs) with half lives of a few minutes to an hour contain a wealth of information about the fission process. Knowledge of short lived FPYs would contribute to existing data on longer lived FPY mass and charge distributions. Of particular interest are the relative yields between the ground states and isomeric states of FPYs since these isomeric ratios can be used to determine the angular momentum of the fragments. Over the past five years, a LLNL-TUNL-LANL collaboration has made precision measurements of FPYs from quasi-monoenergetic neutron induced fission of 235U, 238U and 239Pu. These efforts focused on longer lived FPYs, using a well characterized dual fission chamber and several days of neutron beam exposure. For the first time, this established technique will be applied to measuring short lived FPYs, with half lives of minutes to less than an hour. A feasibility study will be performed using irradiation times of < 1 hour, improving the sensitivity to short lived FPYs by limiting the buildup of long lived isotopes. Results from this exploratory study will be presented, and the implications for isomeric ratio measurements will be discussed. This work was performed under the auspices of US DOE by LLNL under Contract DE-AC52-07NA27344.

Neutron-Induced Fission Cross Sections of 240Pu, 243Am, and natW in the Energy Range 1-200 MeV

NASA Astrophysics Data System (ADS)

Laptev, A. B.; Donets, A. Yu.; Dushin, V. N.; Fomichev, A. V.; Fomichev, A. A.; Haight, R. C.; Shcherbakov, O. A.; Soloviev, S. M.; Tuboltsev, Yu. V.; Vorobyev, A. S.

2005-05-01

A long-range research program devoted to measurements of neutron-induced fission cross-sections of actinides and stable isotopes is under way at the GNEIS facility. By now the new series of experiments for measurements of fission cross-section ratios relative to 235U has been completed for 240Pu, 243Am, and natW in a wide energy range of incident neutrons from 1 MeV to 200 MeV in the frame of the ISTC Project ♯1971. The measurements were performed using the multiplate ionization chamber and time-of-flight techniques. The results obtained in this measurement are presented in comparison with the other data.

Size-resolved chemistry of aerosols produced by Halema'uma'u eruption 2008-2009, Kilauea Volcano, Hawai'i

NASA Astrophysics Data System (ADS)

Ilyinskaya, E.; Martin, R.; Edmonds, M.; Sutton, A. J.; Elias, T.; Werner, C. A.

2009-12-01

A dense quiescent plume has been emitted continuously from the 2008 eruptive vent in Halema'uma'u crater since March 2008. Aerosol particles were sampled near-source in the young plume (<30 s old) in May 2008 and April 2009, and at 10 km downwind (April 2009 only). We also sampled the plume from Pu'u O'o vent both near-source and 8-10 km downwind (2007 to 2009). Sampling was performed using filter packs and a cascade impactor that collects and segregates PM10 (particle matter <10 μm) into 14 size fractions. The collected PM was analysed for SO42-, F-, Cl-, Na+, K+, Ca2+ and Mg2+. Our results show a distinctive peak of sulphate abundance at ~0.3-0.5 μm in the 2008 and 2009 summit samples. The total SO42- mass concentration collected in each sampling run correlates well with that of metals but poorly with Cl- and F-. Downwind measurements of PM from Halema'uma'u and Pu'u O'o show SO42- in the same narrow size bin (0.3-0.5 μm) with concentrations similar to, or higher than at source. It is noteworthy that the particles appear not to have grown when the plume has drifted 5-10 km downwind. However, a 1 μm size mode of SO42- seen at Pu'u O'o crater rim (not seen at Halema'uma'u) is absent from the downwind plume. This result leads us to believe that the particles grow rapidly after emission but get scavenged efficiently once they reach a certain size (>0.5 μm). The formation of aerosol measured downwind is dominated by oxidation of SO2 to SO42- in the plume. The ratio of Cl-/SO42- is higher downwind than at the source in both Halema'uma'u and Pu'u O'o plumes, and increases further during rainfall; we propose that the Cl--bearing aerosol is formed by dissolution of HCl gas into water droplets in the plume.

Use of anthropogenic radioisotopes to estimate rates of soil redistribution by wind II: The potential for future use of 239+240Pu

NASA Astrophysics Data System (ADS)

Van Pelt, R. Scott; Ketterer, Michael E.

2013-06-01

In the previous paper, the use of soilborne 137Cs from atmospheric fallout to estimate rates of soil redistribution, particularly by wind, was reviewed. This method relies on the assumption that the source of 137Cs in the soil profile is from atmospheric fallout following the period of atmospheric weapons testing so that the temporal and, to a certain extent, the spatial patterns of 137Cs deposition are known. One of the major limitations occurs when local or regional sources of 137Cs contamination mask the pulse from global fallout, making temporal estimates of redistribution difficult or impossible. Like 137Cs, Pu exhibits strong affinity for binding to soil particle surfaces, and therefore, re-distribution of Pu inventory indicates inferred soil re-distribution. Compared to 137Cs, 239Pu and 240Pu offer several important advantages: (a) the two major Pu isotopes have much longer half-lives than 137Cs and (b) the ratio 240Pu/239Pu is used to examine whether the Pu is from stratospheric fallout. In this paper, we review the literature concerning Pu in soil and of current attempts to use this tracer to estimate rates of soil redistribution. We also present preliminary, unpublished data from a pilot study designed to test whether or not 239+240Pu can be used to estimate rates of soil redistribution by wind. Based on similarities of profile distribution and relative inventories between 137Cs measurements and 239+240Pu measurements of split samples from a series of fields with documented wind erosion histories, we conclude that 239+240Pu may well be the anthropogenic radioisotope of choice for future soil redistribution investigations.

A Volcano Exploration Project Pu`u `O`o (VEPP) Exercise: Is Kilauea in Volcanic Unrest? (Invited)

NASA Astrophysics Data System (ADS)

Schwartz, S. Y.

2010-12-01

Volcanic activity captures the interest and imagination of students at all stages in their education. Analysis of real data collected on active volcanoes can further serve to engage students in higher-level inquiry into the complicated physical processes associated with volcanic eruptions. This exercise takes advantage of both student fascination with volcanoes and the recognized benefits of incorporating real, internet-accessible data to achieve its goals of enabling students to: 1) navigate a scientific website; 2) describe the physical events that produce volcano monitoring data; 3) identify patterns in geophysical time-series and distinguish anomalies preceding and synchronous with eruptive events; 4) compare and contrast geophysical time series and 5) integrate diverse data sets to assess the eruptive state of Kilauea volcano. All data come from the VEPP website (vepp.wr.usgs.gov) which provides background information on the historic activity and volcano monitoring methods as well as near-real time volcano monitoring data from the Pu`u `O`o eruptive vent on Kilauea Volcano. This exercise, designed for geology majors, has students initially work individually to acquire basic skills with volcano monitoring data interpretation and then together in a jigsaw activity to unravel the events leading up to and culminating in the July 2007 volcanic episode. Based on patterns established prior to the July 2007 event, students examine real-time volcano monitoring data to evaluate the present activity level of Kilauea volcano. This exercise will be used for the first time in an upper division Geologic Hazards class in fall 2010 and lessons learned including an exercise assessment will be presented.

CHEMICAL DIFFERENCES BETWEEN SLUDGE SOLIDS AT THE F AND H AREA TANK FARMS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reboul, S.

2012-08-29

The primary source of waste solids received into the F Area Tank Farm (FTF) was from PUREX processing performed to recover uranium and plutonium from irradiated depleted uranium targets. In contrast, two primary sources of waste solids were received into the H Area Tank Farm (HTF): a) waste from PUREX processing; and b) waste from H-modified (HM) processing performed to recover uranium and neptunium from burned enriched uranium fuel. Due to the differences between the irradiated depleted uranium targets and the burned enriched uranium fuel, the average compositions of the F and H Area wastes are markedly different from onemore » another. Both F and H Area wastes contain significant amounts of iron and aluminum compounds. However, because the iron content of PUREX waste is higher than that of HM waste, and the aluminum content of PUREX waste is lower than that of HM waste, the iron to aluminum ratios of typical FTF waste solids are appreciably higher than those of typical HTF waste solids. Other constituents present at significantly higher concentrations in the typical FTF waste solids include uranium, nickel, ruthenium, zinc, silver, cobalt and copper. In contrast, constituents present at significantly higher concentrations in the typical HTF waste solids include mercury, thorium, oxalate, and radionuclides U-233, U-234, U-235, U-236, Pu-238, Pu-242, Cm-244, and Cm-245. Because of the higher concentrations of Pu-238 in HTF, the long-term concentrations of Th-230 and Ra-226 (from Pu-238 decay) will also be higher in HTF. The uranium and plutonium distributions of the average FTF waste were found to be consistent with depleted uranium and weapons grade plutonium, respectively (U-235 comprised 0.3 wt% of the FTF uranium, and Pu-240 comprised 6 wt% of the FTF plutonium). In contrast, at HTF, U-235 comprised 5 wt% of the uranium, and Pu-240 comprised 17 wt% of the plutonium, consistent with enriched uranium and high burn-up plutonium. X-ray diffraction analyses of various FTF and HTF samples indicated that the primary crystalline compounds of iron in sludge solids are Fe{sub 2}O{sub 3}, Fe{sub 3}O{sub 4}, and FeO(OH), and the primary crystalline compounds of aluminum are Al(OH){sub 3} and AlO(OH). Also identified were carbonate compounds of calcium, magnesium, and sodium; a nitrated sodium aluminosilicate; and various uranium compounds. Consistent with expectations, oxalate compounds were identified in solids associated with oxalic acid cleaning operations. The most likely oxidation states and chemical forms of technetium are assessed in the context of solubility, since technetium-99 is a key risk driver from an environmental fate and transport perspective. The primary oxidation state of technetium in SRS sludge solids is expected to be Tc(IV). In salt waste, the primary oxidation state is expected to be Tc(VII). The primary form of technetium in sludge is expected to be a hydrated technetium dioxide, TcO{sub 2} {center_dot} xH{sub 2}O, which is relatively insoluble and likely co-precipitated with iron. In salt waste solutions, the primary form of technetium is expected to be the very soluble pertechnetate anion, TcO{sub 4}{sup -}. The relative differences between the F and H Tank Farm waste provide a basis for anticipating differences that will occur as constituents of FTF and HTF waste residue enter the environment over the long-term future. If a constituent is significantly more dominant in one of the Tank Farms, its long-term environmental contribution will likely be commensurately higher, assuming the environmental transport conditions of the two Tank Farms share some commonality. It is in this vein that the information cited in this document is provided - for use during the generation, assessment, and validation of Performance Assessment modeling results.« less

PuLSE: Quality control and quantification of peptide sequences explored by phage display libraries.

PubMed

Shave, Steven; Mann, Stefan; Koszela, Joanna; Kerr, Alastair; Auer, Manfred

2018-01-01

The design of highly diverse phage display libraries is based on assumption that DNA bases are incorporated at similar rates within the randomized sequence. As library complexity increases and expected copy numbers of unique sequences decrease, the exploration of library space becomes sparser and the presence of truly random sequences becomes critical. We present the program PuLSE (Phage Library Sequence Evaluation) as a tool for assessing randomness and therefore diversity of phage display libraries. PuLSE runs on a collection of sequence reads in the fastq file format and generates tables profiling the library in terms of unique DNA sequence counts and positions, translated peptide sequences, and normalized 'expected' occurrences from base to residue codon frequencies. The output allows at-a-glance quantitative quality control of a phage library in terms of sequence coverage both at the DNA base and translated protein residue level, which has been missing from toolsets and literature. The open source program PuLSE is available in two formats, a C++ source code package for compilation and integration into existing bioinformatics pipelines and precompiled binaries for ease of use.

TrkB Activators for the Treatment of Traumatic Vision Loss

DTIC Science & Technology

2017-06-01

em ( do i: 10 .1 08 9/ ne u. 20 17 .5 10...Im m un e Sy st em ( do i: 10 .1 08 9/ ne u. 20 17 .5 10 4) T hi s ar tic le h as b ee n pe er -r ev ie w ed a nd a cc ep te d fo r pu bl ic...Sy st em ( do i: 10 .1 08 9/ ne u. 20 17 .5 10 4) T hi s ar tic le h as b ee n pe er -r ev ie w ed a nd a cc ep te d fo r pu bl ic at io

Development of a Self-Consistent Model of Plutonium Sorption: Quantification of Sorption Enthalpy and Ligand-Promoted Dissolution

DOE Office of Scientific and Technical Information (OSTI.GOV)

Powell, Brian; Kaplan, Daniel I; Arai, Yuji

2016-12-29

This university lead SBR project is a collaboration lead by Dr. Brian Powell (Clemson University) with co-principal investigators Dan Kaplan (Savannah River National Laboratory), Yuji Arai (presently at the University of Illinois), Udo Becker (U of Michigan) and Rod Ewing (presently at Stanford University). Hypothesis: The underlying hypothesis of this work is that strong interactions of plutonium with mineral surfaces are due to formation of inner sphere complexes with a limited number of high-energy surface sites, which results in sorption hysteresis where Pu(IV) is the predominant sorbed oxidation state. The energetic favorability of the Pu(IV) surface complex is strongly influencedmore » by positive sorption entropies, which are mechanistically driven by displacement of solvating water molecules from the actinide and mineral surface during sorption. Objectives: The overarching objective of this work is to examine Pu(IV) and Pu(V) sorption to pure metal (oxyhydr)oxide minerals and sediments using variable temperature batch sorption, X-ray absorption spectroscopy, electron microscopy, and quantum-mechanical and empirical-potential calculations. The data will be compiled into a self-consistent surface complexation model. The novelty of this effort lies largely in the manner the information from these measurements and calculations will be combined into a model that will be used to evaluate the thermodynamics of plutonium sorption reactions as well as predict sorption of plutonium to sediments from DOE sites using a component additivity approach.« less

The Use of Isotope Dilution Alpha Spectrometry and Liquid Scintillation Counting to Determine Radionuclides in Environmental Samples (abstract)

NASA Astrophysics Data System (ADS)

Bylyku, Elida

2009-04-01

In Albania in recent years it has been of increasing interest to determine various pollutants in the environment and their possible effects on human health. The radiochemical procedure used to identify Pu, Am, U, Th, and Sr radioisotopes in soil, sediment, water, coal, and milk samples is described. The analysis is carried out in the presence of respective tracer solutions and combines the procedure for Pu analysis based on anion exchange, the selective method for Sr isolation based on extraction chromatography using Sr-Spec resin, and the application of the TRU-Spec column for separation of Am fraction. An acid digestion method has been applied for the decomposition of samples. The radiochemical procedure involves the separation of Pu from Th, Am, and Sr by anion exchange, followed by the preconcentration of Am and Sr by coprecipitation with calcium oxalate. Am is separated from Sr by extraction chromatography. Uranium is separated from the bulk elements by liquid-liquid extraction using UTEVA® resin. Thin sources for alpha spectrometric measurements are prepared by microprecipitation with NdF3. Two International Atomic Energy Agency reference materials were analyzed in parallel with the samples.

Prompt Fission Neutron Multiplicities for 241Pu using Surrogate Reactions

NASA Astrophysics Data System (ADS)

Akindele, Oluwatomi; Burke, Jason; Casperson, Robert; Hughes, Richard; Norman, Eric; Saastamoinen, Antti; Wang, Barbara

2017-09-01

The prompt fission neutron multiplicity for 241Pu was measured at the Texas A&M University Cyclotron using the NeutronSTARS array. Due to the short half-life (14.3 yrs) of 241Pu, inelastic scattering on 242Pu with 55 MeV alpha particles was used as a surrogate. The average neutron multiplicity (ν), and the neutron multiplicity distribution for equivalent neutron energies up to 20 MeV are discussed and reported. This work was performed under the auspices of the U.S. DOE by LLNL under contract DE-AC52-07NA27344, and supported by the DOE NNSA under Award Number DE-NA0000979, and through the Nuclear Science and Security Consortium under Award Number DE-NA-0003180.

Rates of Earth degassing

NASA Technical Reports Server (NTRS)

Onions, R. K.

1994-01-01

The degassing of the Earth during accretion is constrained by Pu-U-I-Xe systematics. Degassing was much more efficient during the first 100-200 Ma than subsequently, and it was more complete for Xe than for the lighter gases. More than 90 percent of the degassed Xe escaped from the atmosphere during this period. The combination of fractional degassing of melts and rare gas escape from the atmosphere is able to explain the deficit of terrestrial Xe as a simple consequence of this early degassing history. By the time Xe was quantitatively retained in the atmosphere, the abundances of Kr and the lighter gases in the Earth's interior were similar to or higher than the present-day atmospheric abundances. Subsequent transfer of these lighter rare gases into the atmosphere requires a high rate of post-accretion degassing and melt production. Considerations of Pu-U-Xe systematics suggest that relatively rapid post-accretion degassing was continued to ca. 4.1-4.2 Ga. The present-day degassing history of the Earth is investigated through consideration of rare gas isotope abundances. Although the Earth is a highly degassed body, depleted in rare gases by many orders of magnitude relative to their solar abundances, it is at the present-day losing primordial rare gases which were trapped at the time of accretion.

ANALYSIS AND EXAMINATION OF MOX FUEL FROM NONPROLIFERATION PROGRAMS

DOE Office of Scientific and Technical Information (OSTI.GOV)

McCoy, Kevin; Machut, Dr McLean; Morris, Robert Noel

The U.S. Department of Energy has decided to dispose of a portion of the nation s surplus plutonium by reconstituting it into mixed oxide (MOX) fuel and irradiating it in commercial power reactors. Four lead assemblies were manufactured and irradiated to a maximum fuel rod burnup of 47.3 MWd/kg heavy metal. This was the first commercial irradiation of MOX fuel with a 240Pu/239Pu ratio of less than 0.10. Five fuel rods with varying burnups and plutonium contents were selected from one of the assemblies and shipped to Oak Ridge National Laboratory for hot cell examination. The performance of the rodsmore » was analyzed with AREVA s next-generation GALILEO code. The results of the analysis confirmed that the fuel rods had performed safely and predictably, and that GALILEO is applicable to MOX fuel with a low 240Pu/239Pu ratio as well as to standard MOX. The results are presented and compared to the GALILEO database. In addition, the fuel cladding was tested to confirm that traces of gallium in the fuel pellets had not affected the mechanical properties of the cladding. The irradiated cladding was found to remain ductile at both room temperature and 350 C for both the axial and circumferential directions.« less

Evaluation of possible physical-chemical processes that might lead to separations of actinides in ORNL waste tanks

DOE Office of Scientific and Technical Information (OSTI.GOV)

Del Cul, G.D.; Toth, L.M.; Bond, W.D.

The concern that there might be some physical-chemical process which would lead to a separation of the poisoning actinides ({sup 232}Th, {sup 238}U) from the fissionable ones ({sup 239}Pu, {sup 235}U) in waste storage tanks at Oak Ridge National Laboratory has led to a paper study of potential separations processes involving these elements. At the relatively high pH values (>8), the actinides are normally present as precipitated hydroxides. Mechanisms that might then selectively dissolve and reprecipitate the actinides through thermal processes or additions of reagents were addressed. Although redox reactions, pH changes, and complexation reactions were all considered, only themore » last type was regarded as having any significant probability. Furthermore, only carbonate accumulation, through continual unmonitored air sparging of the tank contents, could credibly account for gross transport and separation of the actinide components. From the large amount of equilibrium data in the literature, concentration differences in Th, U, and Pu due to carbonate complexation as a function of pH have been presented to demonstrate this phenomenon. While the carbonate effect does represent a potential separations process, control of long-term air sparging and solution pH, accompanied by routine determinations of soluble carbonate concentration, should ensure that this separations process does not occur.« less

CORRELATIONS OF EFFECTIVE TEMPERATURES FOR NEUTRON SPECTRA EMITTED IN U$sup 235$ AND Pu$sup 239$ FISSION BY FAST AND SLOW NEUTRONS (in Russian)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smirenkin, G.M.

1959-12-01

The method of threshold indicators was used for determining the magnitude of dT/sub ef//dE/sub n/. The fission neutrons were produced by fast and slow neutron bombardment. tron bombardment was accomplished in a paraffin block. Hollow metallic U/sup 235/ (90% enriched) and Pu/sup 239/ specimens with 50 mm outside diameters and 10 mm thick contained the threshold activator Ag/sup 107/(n,2n)Ag/sup 106m/. Measurements were made of the neutron flux above the threshold (9.5 Mev) of the Ag/sup 107/(n,2n)Ag/sup 106m/ reaction and the number of fission in the sphere (N/sub gamma /). The final data showed that for U/sup 235/ dT/sub ef//dE/sub n/more » = 0.008 plus or minus 0.004 and for Pu/sup 239/ dT/ sub ef/ /dE/sub n/ = tron fission distributions explain part of the error of the measurement. (R.V.J.)« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

The methods cover: C in solutions, F (electrode), elements by atomic emission spectrometry, inorganic anions by ion chromatography, Hg in water/solids/sludges, As, Se, Bi, Pb, data calculations for SST (single shell tank?) samples, Sb, Tl, Ag, Pu, O/M ratio, ignition weight loss, pH value, ammonia (N), Cr(VI), alkalinity, U, C sepn. from soil/sediment/sludge, Pu purif., total N, water, C and S, surface Cl/F, leachable Cl/F, outgassing of Ge detector dewars, gas mixing, gas isotopic analysis, XRF of metals/alloys/compounds, H in Zircaloy, H/O in metals, inpurity extraction, reduced/total Fe in glass, free acid in U/Pu solns, density of solns, Kr/Xe isotopesmore » in FFTF cover gas, H by combustion, MS of Li and Cs isotopes, MS of lanthanide isotopes, GC operation, total Na on filters, XRF spectroscopy QC, multichannel analyzer operation, total cyanide in water/solid/sludge, free cyanide in water/leachate, hydrazine conc., ICP-MS, {sup 99}Tc, U conc./isotopes, microprobe analysis of solids, gas analysis, total cyanide, H/N{sub 2}O in air, and pH in soil.« less

Multiscale structural characterizations of mixed U(iv)-An(iii) oxalates (An(iii) = Pu or Am) combining XAS and XRD measurements.

PubMed

Arab-Chapelet, B; Martin, P M; Costenoble, S; Delahaye, T; Scheinost, A C; Grandjean, S; Abraham, F

2016-04-28

Mixed actinide(III,IV) oxalates of the general formula M2.2UAn(C2O4)5·nH2O (An = Pu or Am and M = H3O(+) and N2H5(+)) have been quantitatively precipitated by oxalic precipitation in nitric acid medium (yield >99%). Thorough multiscale structural characterization using XRD and XAS measurements confirmed the existence of mixed actinide oxalate solid solutions. The XANES analysis confirmed that the oxidation states of the metallic cations, tetravalent for uranium and trivalent for plutonium and americium, are maintained during the precipitation step. EXAFS measurements show that the local environments around U(+IV), Pu(+III) and Am(+III) are comparable, and the actinides are surrounded by ten oxygen atoms from five bidentate oxalate anions. The mean metal-oxygen distances obtained by XAS measurements are in agreement with those calculated from XRD lattice parameters.

Particulate, colloidal, and dissolved-phase associations of plutonium and americium in a water sample from well 1587 at the Rocky Flats Plant, Colorado

USGS Publications Warehouse

Harnish, R.A.; McKnight, Diane M.; Ranville, James F.

1994-01-01

In November 1991, the initial phase of a study to determine the dominant aqueous phases that control the transport of plutonium (Pu), americium (Am), and uranium (U) in surface and groundwater at the Rocky Flats Plant was undertaken by the U.S. Geological Survey. By use of the techniques of stirred-cell spiral-flow filtration and crossflow ultrafiltration, particles of three size fractions were collected from a 60-liter sample of water from well 1587 at the Rocky Flats Plant. These samples and corresponding filtrate samples were analyzed for Pu and Am. As calculated from the analysis of filtrates, 65 percent of Pu 239 and 240 activity in the sample was associated with particulate and largest colloidal size fractions. Particulate (22 percent) and colloidal (43 percent) fractions were determined to have significant activities in relation to whole-water Pu activity. Am and Pu 238 activities were too low to be analyzed. Examination and analyses of the particulate and colloidal phases indicated the presence of mineral species (iron oxyhydroxides and clay minerals) and natural organic matter that can facilitate the transport of actinides in ground water. High concentrations of the transition metals copper and zinc in the smallest colloid fractions strongly indicate a potential for organic complexation of metals, and potentially of actinides, in this size fraction.

Levels, distribution and bioavailability of transuranic elements released in the Palomares accident (Spain).

PubMed

Jiménez-Ramos, M C; Vioque, I; García-Tenorio, R; García León, M

2008-11-01

The current levels and distribution of the remaining transuranic contamination present in the terrestrial area affected by the nuclear Palomares accident have been evaluated through the determination of the Pu-isotopes and (241)Am concentrations in soils collected 35 years after the accident. In addition, after confirming that most of the contamination is present in particulate form, some bioavailability laboratory-based experiments, based on the use of single extractants, were performed as an essential step in order to study the behaviour of the Pu contamination in the soils from the affected areas.

TANK 40 FINAL SB7B CHEMICAL CHARACTERIZATION RESULTS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bannochie, C.

2012-03-15

A sample of Sludge Batch 7b (SB7b) was taken from Tank 40 in order to obtain radionuclide inventory analyses necessary for compliance with the Waste Acceptance Product Specifications (WAPS). The SB7b WAPS sample was also analyzed for chemical composition including noble metals and fissile constituents, and these results are reported here. These analyses along with the WAPS radionuclide analyses will help define the composition of the sludge in Tank 40 that is currently being fed to the Defense Waste Processing Facility (DWPF) as SB7b. At the Savannah River National Laboratory (SRNL) the 3-L Tank 40 SB7b sample was transferred frommore » the shipping container into a 4-L high density polyethylene bottle and solids were allowed to settle over the weekend. Supernate was then siphoned off and circulated through the shipping container to complete the transfer of the sample. Following thorough mixing of the 3-L sample, a 558 g sub-sample was removed. This sub-sample was then utilized for all subsequent analytical samples. Eight separate aliquots of the slurry were digested, four with HNO{sub 3}/HCl (aqua regia) in sealed Teflon{reg_sign} vessels and four with NaOH/Na{sub 2}O{sub 2} (alkali or peroxide fusion) using Zr crucibles. Two Analytical Reference Glass - 1 (ARG-1) standards were digested along with a blank for each preparation. Each aqua regia digestion and blank was diluted to 1:100 mL with deionized water and submitted to Analytical Development (AD) for inductively coupled plasma - atomic emission spectroscopy (ICP-AES) analysis, inductively coupled plasma - mass spectrometry (ICP-MS) analysis, atomic absorption spectroscopy (AA) for As and Se, and cold vapor atomic absorption spectroscopy (CV-AA) for Hg. Equivalent dilutions of the alkali fusion digestions and blank were submitted to AD for ICP-AES analysis. Tank 40 SB7b supernate was collected from a mixed slurry sample in the SRNL Shielded Cells and submitted to AD for ICP-AES, ion chromatography (IC), total base/free OH{sup -}/other base, total inorganic carbon/total organic carbon (TIC/TOC) analyses, and Cs-137 gamma scan. Weighted dilutions of slurry were submitted for IC, TIC/TOC, and total base/free OH{sup -}/other base analyses. Activities for U-233, U-235, and Pu-239 were determined from the ICP-MS data for the aqua regia digestions of the Tank 40 WAPS slurry using the specific activity of each isotope. The Pu-241 value was determined from a Pu-238/-241 method developed by SRNL AD and previously described. The following conclusions were drawn from the analytical results reported here: (1) The ratios of the major elements for the SB7b WAPS sample are different from those measured for the SB7a WAPS sample. There is less Al and Mn relative to Fe than the previous sludge batch. (2) The elemental composition of this sample and the analyses conducted here are reasonable and consistent with DWPF batch data measurements in light of DWPF pre-sample concentration and SRAT product heel contributions to the DWPF SRAT receipt analyses. The element ratios for Al/Fe, Ca/Fe, Mn/Fe, and U/Fe agree within 10% between this work and the DWPF Sludge Receipt and Adjustment Tank (SRAT) receipt analyses. (3) Sulfur in the SB7b WAPS sample is 82% soluble, slightly less than results reported for SB3, SB4, and SB6 samples but unlike the 50% insoluble sulfur observed in the SB5 WAPS sample. In addition, 23% of the soluble sulfur is not present as sulfate in SB7b. (4) The average activities of the fissile isotopes of interest in the SB7b WAPS sample are (in {mu}Ci/g of total dried solids): 4.22E-02 U-233, 6.12E-04 U-235, 1.08E+01 Pu-239, and 5.09E+01 Pu-241. The full radionuclide composition will be reported in a future document. (5) The fission product noble metal and Ag concentrations appear to have largely peaked in previous DWPF sludge batches, with the exception of Ru, which still shows a slight increase in SB7b.« less

Photofission product yields of 238U and 239Pu with 22-MeV bremsstrahlung

NASA Astrophysics Data System (ADS)

Wen, Xianfei; Yang, Haori

2016-06-01

In homeland security and nuclear safeguards applications, non-destructive techniques to identify and quantify special nuclear materials are in great demand. Although nuclear materials naturally emit characteristic radiation (e.g. neutrons, γ-rays), their intensity and energy are normally low. Furthermore, such radiation could be intentionally shielded with ease or buried in high-level background. Active interrogation techniques based on photofission have been identified as effective assay approaches to address this issue. In designing such assay systems, nuclear data, like photofission product yields, plays a crucial role. Although fission yields for neutron-induced reactions have been well studied and readily available in various nuclear databases, data on photofission product yields is rather scarce. This poses a great challenge to the application of photofission techniques. In this work, short-lived high-energy delayed γ-rays from photofission of 238U were measured in between linac pulses. In addition, a list-mode system was developed to measure relatively long-lived delayed γ-rays from photofission of 238U and 239Pu after the irradiation. Time and energy information of each γ-ray event were simultaneously recorded by this system. Cumulative photofission product yields were then determined using the measured delayed γ-ray spectra.

The Need for Precise and Well-documented Experimental Data on Prompt Fission Neutron Spectra from Neutron-induced Fission of {sup 239}Pu

DOE Office of Scientific and Technical Information (OSTI.GOV)

Neudecker, D., E-mail: dneudecker@lanl.gov; Taddeucci, T.N.; Haight, R.C.

2016-01-15

The spectrum of neutrons emitted promptly after {sup 239}Pu(n,f)—a so-called prompt fission neutron spectrum (PFNS)—is a quantity of high interest, for instance, for reactor physics and global security. However, there are only few experimental data sets available that are suitable for evaluations. In addition, some of those data sets differ by more than their 1-σ uncertainty boundaries. We present the results of MCNP studies indicating that these differences are partly caused by underestimated multiple scattering contributions, over-corrected background, and inconsistent deconvolution methods. A detailed uncertainty quantification for suitable experimental data was undertaken including these effects, and test-evaluations were performed withmore » the improved uncertainty information. The test-evaluations illustrate that the inadequately estimated effects and detailed uncertainty quantification have an impact on the evaluated PFNS and associated uncertainties as well as the neutron multiplicity of selected critical assemblies. A summary of data and documentation needs to improve the quality of the experimental database is provided based on the results of simulations and test-evaluations. Given the possibly substantial distortion of the PFNS by multiple scattering and background effects, special care should be taken to reduce these effects in future measurements, e.g., by measuring the {sup 239}Pu PFNS as a ratio to either the {sup 235}U or {sup 252}Cf PFNS.« less

Thorium Fuel Cycle Option Screening in the United States

DOE Office of Scientific and Technical Information (OSTI.GOV)

Taiwo, Temitope A.; Kim, Taek K.; Wigeland, Roald A.

2016-05-01

As part of a nuclear fuel cycle Evaluation and Screening (E&S) study, a wide-range of thorium fuel cycle options were evaluated and their performance characteristics and challenges to implementation were compared to those of other nuclear fuel cycle options based on criteria specified by the Nuclear Energy Office of the U.S. Department of Energy (DOE). The evaluated nuclear fuel cycles included the once-through, limited, and continuous recycle options using critical or externally-driven nuclear energy systems. The E&S study found that the continuous recycle of 233U/Th in fuel cycles using either thermal or fast reactors is an attractive promising fuel cyclemore » option with high effective fuel resource utilization and low waste generation, but did not perform quite as well as the continuous recycle of Pu/U using a fast critical system, which was identified as one of the most promising fuel cycle options in the E&S study. This is because compared to their uranium counterparts the thorium-based systems tended to have higher radioactivity in the short term (about 100 years post irradiation) because of differences in the fission product yield curves, and in the long term (100,000 years post irradiation) because of the decay of 233U and daughters, and because of higher mass flow rates due to lower discharge burnups. Some of the thorium-based systems also require enriched uranium support, which tends to be detrimental to resource utilization and waste generation metrics. Finally, similar to the need for developing recycle fuel fabrication, fuels separations and fast reactors for the most promising options using Pu/U recycle, the future thorium-based fuel cycle options with continuous recycle would also require such capabilities, although their deployment challenges are expected to be higher since such facilities have not been developed in the past to a comparable level of maturity for Th-based systems.« less

Analysis of key safety metrics of thorium utilization in LWRs

DOE PAGES

Ade, Brian J.; Bowman, Stephen M.; Worrall, Andrew; ...

2016-04-08

Here, thorium has great potential to stretch nuclear fuel reserves because of its natural abundance and because it is possible to breed the 232Th isotope into a fissile fuel ( 233U). Various scenarios exist for utilization of thorium in the nuclear fuel cycle, including use in different nuclear reactor types (e.g., light water, high-temperature gas-cooled, fast spectrum sodium, and molten salt reactors), along with use in advanced accelerator-driven systems and even in fission-fusion hybrid systems. The most likely near-term application of thorium in the United States is in currently operating light water reactors (LWRs). This use is primarily based onmore » concepts that mix thorium with uranium (UO 2 + ThO 2) or that add fertile thorium (ThO 2) fuel pins to typical LWR fuel assemblies. Utilization of mixed fuel assemblies (PuO 2 + ThO 2) is also possible. The addition of thorium to currently operating LWRs would result in a number of different phenomenological impacts to the nuclear fuel. Thorium and its irradiation products have different nuclear characteristics from those of uranium and its irradiation products. ThO 2, alone or mixed with UO 2 fuel, leads to different chemical and physical properties of the fuel. These key reactor safety–related issues have been studied at Oak Ridge National Laboratory and documented in “Safety and Regulatory Issues of the Thorium Fuel Cycle” (NUREG/CR-7176, U.S. Nuclear Regulatory Commission, 2014). Various reactor analyses were performed using the SCALE code system for comparison of key performance parameters of both ThO 2 + UO 2 and ThO 2 + PuO 2 against those of UO 2 and typical UO 2 + PuO 2 mixed oxide fuels, including reactivity coefficients and power sharing between surrounding UO 2 assemblies and the assembly of interest. The decay heat and radiological source terms for spent fuel after its discharge from the reactor are also presented. Based on this evaluation, potential impacts on safety requirements and identification of knowledge gaps that require additional analysis or research to develop a technical basis for the licensing of thorium fuel are identified.« less

The heartbeat of the volcano: The discovery of episodic activity at Prometheus on Io

USGS Publications Warehouse

Davies, A.G.; Wilson, L.; Matson, D.; Leone, G.; Keszthelyi, L.; Jaeger, W.

2006-01-01

The temporal signature of thermal emission from a volcano is a valuable clue to the processes taking place both at and beneath the surface. The Galileo Near Infrared Mapping Spectrometer (NIMS) observed the volcano Prometheus, on the jovian moon Io, on multiple occasions between 1996 and 2002. The 5 micron (??m) brightness of this volcano shows considerable variation from orbit to orbit. Prometheus exhibits increases in thermal emission that indicate episodic (though non-periodic) effusive activity in a manner akin to the current Pu'u 'O'o-Kupaianaha (afterwards referred to as the Pu'u 'O'o) eruption of Kilauea, Hawai'i. The volume of material erupted during one Prometheus eruption episode (defined as the interval from minimum thermal emission to peak and back to minimum) from 6 November 1996 to 7 May 1997 is estimated to be ???0.8 km3, with a peak instantaneous volumetric flux (effusion rate) of ???140 m3 s-1, and an averaged volumetric flux (eruption rate) of ???49 m3 s-1. These quantities are used to model subsurface structure, magma storage and magma supply mechanisms, and likely magma chamber depth. Prometheus appears to be supplied by magma from a relatively shallow magma chamber, with a roof at a minimum depth of ???2-3 km and a maximum depth of ???14 km. This is a much shallower depth range than sources of supply proposed for explosive, possibly ultramafic, eruptions at Pillan and Tvashtar. As Prometheus-type effusive activity is widespread on Io, shallow magma chambers containing magma of basaltic or near-basaltic composition and density may be common. This analysis strengthens the analogy between Prometheus and Pu'u 'O'o, at least in terms of eruption style. Even though the style of eruption appears to be similar (effusive emplacement of thin, insulated, compound pahoehoe flows) the scale of activity at Prometheus greatly exceeds current activity at Pu'u 'O'o in terms of volume erupted, area covered, and magma flux. Whereas the estimated magma chamber at Prometheus dwarfs the Pu'u 'O'o magma chamber, it fits within expectations if the Pu'u 'O'o chamber were scaled for the greater volumetric flux and lower gravity of Io. Recent volumetric eruption rates derived from Galileo data for Prometheus were considerably smaller than the rate that produced the extensive flows formed in the ???17 years between the Voyager and Galileo missions. These smaller eruption rates, coupled with the fact that flows are not expanding laterally, may mean that the immediate heat source that generates the Prometheus plume is simultaneously running out of available volatiles and the thermal energy that drives mobilization of volatiles. This raises the question of whether the current Prometheus eruption is in its last throes. ?? 2006 Elsevier Inc.

Ensemble positive unlabeled learning for disease gene identification.

PubMed

Yang, Peng; Li, Xiaoli; Chua, Hon-Nian; Kwoh, Chee-Keong; Ng, See-Kiong

2014-01-01

An increasing number of genes have been experimentally confirmed in recent years as causative genes to various human diseases. The newly available knowledge can be exploited by machine learning methods to discover additional unknown genes that are likely to be associated with diseases. In particular, positive unlabeled learning (PU learning) methods, which require only a positive training set P (confirmed disease genes) and an unlabeled set U (the unknown candidate genes) instead of a negative training set N, have been shown to be effective in uncovering new disease genes in the current scenario. Using only a single source of data for prediction can be susceptible to bias due to incompleteness and noise in the genomic data and a single machine learning predictor prone to bias caused by inherent limitations of individual methods. In this paper, we propose an effective PU learning framework that integrates multiple biological data sources and an ensemble of powerful machine learning classifiers for disease gene identification. Our proposed method integrates data from multiple biological sources for training PU learning classifiers. A novel ensemble-based PU learning method EPU is then used to integrate multiple PU learning classifiers to achieve accurate and robust disease gene predictions. Our evaluation experiments across six disease groups showed that EPU achieved significantly better results compared with various state-of-the-art prediction methods as well as ensemble learning classifiers. Through integrating multiple biological data sources for training and the outputs of an ensemble of PU learning classifiers for prediction, we are able to minimize the potential bias and errors in individual data sources and machine learning algorithms to achieve more accurate and robust disease gene predictions. In the future, our EPU method provides an effective framework to integrate the additional biological and computational resources for better disease gene predictions.

A Specific Long-Term Plan for Management of U.S. Nuclear Spent Fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Levy, Salomon

2006-07-01

A specific plan consisting of six different steps is proposed to accelerate and improve the long-term management of U.S. Light Water Reactor (LWR) spent nuclear fuel. The first step is to construct additional, centralized, engineered (dry cask) spent fuel facilities to have a backup solution to Yucca Mountain (YM) delays or lack of capacity. The second step is to restart the development of the Integral Fast Reactor (IFR), in a burner mode, because of its inherent safety characteristics and its extensive past development in contrast to Acceleration Driven Systems (ADS). The IFR and an improved non-proliferation version of its pyro-processingmore » technology can burn the plutonium (Pu) and minor actinides (MA) obtained by reprocessing LWR spent fuel. The remaining IFR and LWR fission products will be treated for storage at YM. The radiotoxicity of that high level waste (HLW) will fall below that of natural uranium in less than one thousand years. Due to anticipated increased capital, maintenance, and research costs for IFR, the third step is to reduce the required number of IFRs and their potential delays by implementing multiple recycles of Pu and Neptunium (Np) MA in LWR. That strategy is to use an advanced separation process, UREX+, and the MIX Pu option where the role and degradation of Pu is limited by uranium enrichment. UREX+ will decrease proliferation risks by avoiding Pu separation while the MIX fuel will lead to an equilibrium fuel recycle mode in LWR which will reduce U. S. Pu inventory and deliver much smaller volumes of less radioactive HLW to YM. In both steps two and three, Research and Development (R and D) is to emphasize the demonstration of multiple fuel reprocessing and fabrication, while improving HLW treatment, increasing proliferation resistance, and reducing losses of fissile material. The fourth step is to license and construct YM because it is needed for the disposal of defense wastes and the HLW to be generated under the proposed plan. The fifth step consists of developing a risk informed methodology to assess the various options available for disposition of LWR spent fuel and to select among them. The sixth step is to modify the current U. S. infrastructure and to create a climate to increase the utilization of uranium and the sustainability of nuclear generated electricity. (author)« less

Radionuclide Concentrations in Soils and Vegetation at Low-Level Radioactive Waste Disposal Area G during the 1997 Growing Season

DOE Office of Scientific and Technical Information (OSTI.GOV)

L. Naranjo, Jr.; P. R. Fresquez; R. J. Wechsler

1998-08-01

Soil and overstory and understory vegetation (washed and unwashed) collected at eight locations within and around Area G-a low-level radioactive solid-waste disposal facility at Los Alamos National Laboratory-were analyzed for 3H, 238Pu, 239Pu, 137CS, 234U, 235U, 228AC, Be, 214Bi, 60Co, 40& 54Mn, 22Na, 214Pb and 208Tl. In general, most radionuclide concentrations, with the exception of 3Ef and ~9Pu, in soils and overstory and understory vegetation collected from within and around Area G were within upper (95'%) level background concentrations. Although 3H concentrations in vegetation from most sites were significantly higher than background (>2 pCi mL-l), concentrations decreased markedly in comparisonmore » to last year's results. The highest `H concentration in vegetation was detected from a juniper tree that was growing over tritium shaft /+150; it contained 530,000 pCi 3H mL-l. Also, as in the pas~ the transuranic waste pad area contained the highest levels of 239Pu in soils and in understory vegetation as compared to other areas at Area G.« less

Closure Report for Corrective Action Unit 415: Project 57 No. 1 Plutonium Dispersion (NTTR) Nevada Test and Training Range, Nevada, Revision 0 with ROTC-1

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cabble, Kevin J.; Boehlecke, Robert F.

This Closure Report (CR) presents information supporting the closure of Corrective Action Unit (CAU) 415: Project 57 No. 1 Plutonium Dispersion, which is located on Range 4808A of the Nevada Test and Training Range (NTTR). This CR complies with the requirements of the Federal Facility Agreement and Consent Order (FFACO) that was agreed to by the State of Nevada; U.S. Department of Energy (DOE), Environmental Management; U.S. Department of Defense; and DOE, Legacy Management. CAU 415 comprises one corrective action site (CAS): NAFR-23-02, Pu Contaminated Soil. The purpose of this CR is to provide justification and documentation supporting the recommendationmore » that no further corrective action is needed for CAU 415 based on the implementation of the corrective action of Closure in Place.« less

Simulation of Flow and Long-Term Plutonium (Pu) Transport in the Vadose Zone at the Savannah River National Laboratory (SRNL)

NASA Astrophysics Data System (ADS)

Demirkanli, I.; Molz, F. J.; Kaplan, D. I.; Fjeld, R. A.; Serkiz, S. M.

2006-05-01

An improved understanding of flow and radionuclide transport in vadose zone sediments is fundamental to all types of future planning involving radioactive materials. One way to obtain such understanding is to perform long-term experimental studies of Pu transport in complex natural systems. With this in mind, a series of field experiments were initiated at the SRNL in the early 1980s. Lysimeters containing sources of different Pu oxidation states were placed in the shallow subsurface and left open to the natural environment for 2 to 11 years. At the end of the experiments, Pu activities were measured along vertical cores obtained from the lysimeters. Pu distributions were anomalous in nature, with transport from oxidized Pu sources being less than expected, and a small fraction of Pu from reduced sources moving more. Laboratory studies with lysimeter sediments suggested that surface-mediated, oxidation/reduction (redox) reactions could be responsible for the anomalous behavior, and this hypothesis is tested by performing both steady-state and transient Pu transport simulations that include retardation along with first-order redox reactions on mineral surfaces. Based on the simulations, we conclude that the surface-mediated, redox hypothesis is consistent with the observed downward Pu activity profiles in the experiments, and such profiles are captured well by a steady-state, net downward, flow model. (Discussion is presented as to why a steady model appears to work in a highly transient flow environment.) The redox model explains how Pu(V/VI) sources release activity that moves downward more slowly than expected based on adsorptive retardation alone, and how Pu(III/IV) sources result in a small fraction of activity that moves downward more rapidly than expected. The calibrated parameter values were robust and relatively well-defined throughout all four sets of simulations. Pu(V/VI) (i.e., oxidized Pu)retardation factors were about 15, and reduced Pu(III/IV) retardation factors were about 10,000. For these values, ko (1st order oxidation rate) averaged 2.4x10-7/hr with a standard deviation of 1.6x10-7, and kr (reduction rate)was 7.1x10-4/hr with a standard deviation of 1.6x10-4. Preliminary transient flow simulations showed a very slight increase in the fitted reaction rate constants, but otherwise reproduced the steady-state results. To date, neither approach is able to simulate the observed Pu movement above the source.

From pumice to obsidian: eruptive behaviors that produce tephra-flow dyads. II- The 114ka trachyte eruption at Pu'u Wa'awa'a (Hawai'i).

NASA Astrophysics Data System (ADS)

Shea, T.; Leonhardi, T. C.; Giachetti, T.; Larsen, J. F.; Lindoo, A. N.

2014-12-01

Associations of tephra and lava flow/domes produced by eruptions involving evolved magmas are a common occurrence in various types of volcanic settings (e.g. Pu'u Wa'awa'a ~114ka, Hawaii; South Mono ~AD625, California; Newberry Big Obsidian flow ~AD700, Oregon; Big Glass Mountain ~AD1100, California; Inyo ~AD1350, California, Chaitén AD2008-2009, Chile; Cordón Caulle AD2011-2012, Chile), ejecting up to a few cubic km of material (tephra+flow/dome). Most, if not all, of these eruptions have in common the paradoxical coexistence of (1) eruptive styles which are inferred to be sustained in nature (subplinian and plinian), with (2) a pulsatory behavior displayed by the resulting fall deposits, and (3) the coeval ejection of vesicular tephra and pyroclastic obsidian. Through two case studies, we explore this apparent set of paradoxes, and their significance in understanding transitions from explosive to effusive behavior. In this second case study (also cf. Shea et al., same session), we present new field, textural and geochemical data pertaining to the 114ka Pu'u Wa'awa'a trachyte eruption in Hawai'i. This large volume (>5 km3) event produced both a tephra cone (~1.6 km in diameter) and a thick (>250 m) lava flow, which have been largely covered by the more recent basaltic Mauna Loa and Hualalai lava flows. The trachyte tephra contains juvenile material displaying a large textural variety (pumice, scoria, obsidian, microcrystalline trachyte and banded-clasts), which can be linked with the extent of degassing and the formation of feldspar microlites. Notably, the abundance of microlites can be used to reconstruct an ascent and devolatilization history that accounts for all the seemingly contradictory observations.

Positive-unlabeled learning for disease gene identification

PubMed Central

Yang, Peng; Li, Xiao-Li; Mei, Jian-Ping; Kwoh, Chee-Keong; Ng, See-Kiong

2012-01-01

Background: Identifying disease genes from human genome is an important but challenging task in biomedical research. Machine learning methods can be applied to discover new disease genes based on the known ones. Existing machine learning methods typically use the known disease genes as the positive training set P and the unknown genes as the negative training set N (non-disease gene set does not exist) to build classifiers to identify new disease genes from the unknown genes. However, such kind of classifiers is actually built from a noisy negative set N as there can be unknown disease genes in N itself. As a result, the classifiers do not perform as well as they could be. Result: Instead of treating the unknown genes as negative examples in N, we treat them as an unlabeled set U. We design a novel positive-unlabeled (PU) learning algorithm PUDI (PU learning for disease gene identification) to build a classifier using P and U. We first partition U into four sets, namely, reliable negative set RN, likely positive set LP, likely negative set LN and weak negative set WN. The weighted support vector machines are then used to build a multi-level classifier based on the four training sets and positive training set P to identify disease genes. Our experimental results demonstrate that our proposed PUDI algorithm outperformed the existing methods significantly. Conclusion: The proposed PUDI algorithm is able to identify disease genes more accurately by treating the unknown data more appropriately as unlabeled set U instead of negative set N. Given that many machine learning problems in biomedical research do involve positive and unlabeled data instead of negative data, it is possible that the machine learning methods for these problems can be further improved by adopting PU learning methods, as we have done here for disease gene identification. Availability and implementation: The executable program and data are available at http://www1.i2r.a-star.edu.sg/∼xlli/PUDI/PUDI.html. Contact: xlli@i2r.a-star.edu.sg or yang0293@e.ntu.edu.sg Supplementary information: Supplementary Data are available at Bioinformatics online. PMID:22923290

Americium, plutonium and uranium contamination and speciation in well waters, streams and atomic lakes in the Sarzhal region of the Semipalatinsk Nuclear Test Site, Kazakhstan.

PubMed

León Vintró, L; Mitchell, P I; Omarova, A; Burkitbayev, M; Jiménez Nápoles, H; Priest, N D

2009-04-01

New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel'kem 1 and Tel'kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that (241)Am, (239,240)Pu and (238)U concentrations in well waters within the study area are in the range 0.04-87mBq dm(-3), 0.7-99mBq dm(-3), and 74-213mBq dm(-3), respectively, and for (241)Am and (239,240)Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01mBq dm(-3), 0.08mBq dm(-3) and 0.32mBq dm(-3) for (241)Am, (239,240)Pu and (238)U, respectively. The (235)U/(238)U isotopic ratio in almost all well and stream waters is slightly elevated above the 'best estimate' value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53-85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11-42microSv (mean 21microSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel'kem explosions.

Fission product yield measurements using monoenergetic photon beams

NASA Astrophysics Data System (ADS)

Krishichayan; Bhike, M.; Tonchev, A. P.; Tornow, W.

2017-09-01

Measurements of fission products yields (FPYs) are an important source of information on the fission process. During the past couple of years, a TUNL-LANL-LLNL collaboration has provided data on the FPYs from quasi monoenergetic neutron-induced fission on 235U, 238U, and 239Pu and has revealed an unexpected energy dependence of both asymmetric fission fragments at energies below 4 MeV. This peculiar FPY energy dependence was more pronounced in neutron-induced fission of 239Pu. In an effort to understand and compare the effect of the incoming probe on the FPY distribution, we have carried out monoenergetic photon-induced fission experiments on the same 235U, 238U, and 239Pu targets. Monoenergetic photon beams of Eγ = 13.0 MeV were provided by the HIγS facility, the world's most intense γ-ray source. In order to determine the total number of fission events, a dual-fission chamber was used during the irradiation. These irradiated samples were counted at the TUNL's low-background γ-ray counting facility using high efficient HPGe detectors over a period of 10 weeks. Here we report on our first ever photofission product yield measurements obtained with monoenegetic photon beams. These results are compared with neutron-induced FPY data.

Soils element activities for the period October 1973--September 1974

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fowler, E.B.; Essington, E.H.; White, M.G.

Soils Element activities were conducted on behalf of the U. S. Atomic Energy Commission's Nevada Applied Ecology Group (NAEG) program to provide source term information for the other program elements and maintain continuous cognizance of program requirements for sampling, sample preparation, and analysis. Activities included presentation of papers; participation in workshops; analysis of soil, vegetation, and animal tissue samples for $sup 238$Pu, $sup 239-240$Pu, $sup 241$Am, $sup 137$Cs, $sup 60$Co, and gamma scan for routine and laboratory quality control purposes; preparation and analysis of animal tissue samples for NAEG laboratory certification; studies on a number of analytical, sample preparation, andmore » sample collection procedures; and contributions to the evaluation of procedures for calculation of specialized counting statistics. (auth)« less

Ya B Zeldovich and nuclear power

NASA Astrophysics Data System (ADS)

Ponomarev, L. I.

2014-03-01

The idea on a homogeneous nuclear reactor, first suggested by Ya B Zeldovich and Yu B Khariton in 1939, has since had its ups and downs and is now re-emerging, enriched with the knowledge and experience accumulated over the years having past. One of the current versions of the idea, the fast molten-salt reactor with a U-Pu fuel cycle, is presented in this paper.

Sodium hydrogen carbonate as an alternative blowing agent in the preparation of palm-based polyurethane foam

NASA Astrophysics Data System (ADS)

Shakir, Amira Shakim Abdul; Badri, Khairiah Haji; Hua, Chia Chin

2016-11-01

An environmental-friendly blowing agent has been used to fabricate flexible polyurethane (PU) foam. Polyurethane foam was prepared from palm kernel oil-based monoester polyol (PKO-p) via prepolymerization method. Acetone has been used as solvent in this study. The developed polyurethane foam was characterized using tensile, differential scanning calorimetry analysis (DSC), thermogravimetric analysis (TGA), optical microscope and drop shape analyzer. The mechanical properties of the PU-reference (PU-R) and PU-NaHCO3 foam was analyzed by tensile using ASTM D 3574-01. From the results, the elongation of PU- NaHCO3 shows reduction to 26.3 % compared to PU-R. The DSC showed two glass transition temperatures in all samples that belonged to the PU-R and PU-NaHCO3. TGA revealed that the incorporation of sodium hydrogen carbonate into the PU system did not show significant difference as compared to the control PU. The morphology of both PU was investigated using optical microscope. Contact angle has been measured to determine the hydrophobicity of the PU. The PU- NaHCO3 exhibited an increase in contact angle (93.1°).

THERMODYNAMICS AND KINETICS OF PHASE TRANSFORMATIONS IN PLUTONIUM ALLOYS - PART I

DOE Office of Scientific and Technical Information (OSTI.GOV)

Turchi, P A; Kaufman, L; Liu, Z

2004-08-18

In this report we investigate order, stability, and phase transformations for a series of actinide-based alloys. The statics and kinetics of precipitation and ordering in this class of alloys are modeled with a scheme that couples fundamental information on the alloy energetics obtained from experimental and assessed thermo-chemical data to the CALPHAD approach commonly used in industry for designing alloys with engineering specificity with the help of the Thermo-Calc software application. The CALPHAD approach is applied to the study of the equilibrium thermodynamic properties of Pu-based alloys, Pu-X, where X=Al, Fe, Ga. The assessment of the equilibrium phase diagrams inmore » the whole range of alloy composition has been performed with the PARROT module of the Thermo-Calc application software. Predictions are made on the low temperature and Pu-rich side of the phase diagrams of Pu-Ga and Pu-Al for which controversy has been noted in the past. The validity of the assessed thermo-chemical database will be discussed by comparing predicted heats of transformation for pure Pu with measured values from differential scanning calorimetry analysis. An overall picture for the stability properties of Pu-Ga and Pu-Al that reconciles the results of past studies carried out on these alloys is proposed. Results on phase stability in the ternary Fe-Ga-Pu and Al-Fe-Pu alloys are discussed. The information collected in this study is then used to model metastability, long-term stability and aging for this class of alloys by coupling Thermo-Calc with DICTRA, a series of modules that allow the analysis of DIffusion Controlled TRAnsformations. Kinetics information is then summarized in so-called TTT (temperature-time-transformations) diagrams for the most relevant phases of actinide alloys. Specifically, results are presented on kinetics of phase transformations associated with the eutectoid-phase decomposition reaction occurring at low temperature, and with the martensitic transformation that takes place at low Ga content in Pu-Ga alloys. Finally, after a summary of the most salient results, suggestions are made for further studies at the micro- and mesoscales.« less

Extremely Rapid Crystal Fractionation During Episodes 30-31 of the Pu`u O`o Eruption: Implications for Magma Chamber Processes

NASA Astrophysics Data System (ADS)

Garcia, M. O.; Rhodes, J. M.; Pietruszka, A. J.; Rose, W. I.

2002-12-01

The Pu`u O`o eruption offers excellent opportunities to examine petrologic and geochemical processes in shallow, basaltic magma chamber due to the intense, multi-disciplinary monitoring of its activity, frequent sampling and repeated eruptions at the same vent. Strong compositional variations were observed during some of the high fire-fountaining (400 m) episodes in 1985. Following a 20-30 day hiatus in eruptive activity, the shallow magma chamber was largely evacuated during brief (1-2 day) eruptions. Samples collected during these episodes, especially at the beginning and end, document the compositional variation between and during eruptive episodes. Lavas and tephra from episodes 30 and 31 showed a remarkable and systematic variation (2 wt% increase in MgO; 7% decrease in incompatible elements like Ba) during and between these episodes. Most of the intra-episode lava compositional variation was observed during a brief period (<2 hours) with little variation before or after. Olivines in these weakly prophyritic Pu`u O`o lavas are in equilibrium with the host rock composition indicating that compositional variation is not related to magma mixing or accumulation of olivine. We interpret the variation to reflect crystal fractionation within the shallow (tens to hundreds of meter deep) Pu`u O`o magma chamber. This extremely high rate of crystallization (up to 0.3%/day) and cooling (2°C/day), compared to estimates of 1°C/year for the rift zone interior, must reflect the high surface area of the dike-shaped and open topped magma chamber. These features may represent the tapping of a diffusive interface separating well mixed zones of hotter and more primitive magma in the lower part of the chamber from cooler, somewhat evolved magma above.

A comparison of two micro-beam X-ray emission techniques for actinide elemental distribution in microscopic particles originating from the hydrogen bombs involved in the Palomares (Spain) and Thule (Greenland) accidents

NASA Astrophysics Data System (ADS)

Jimenez-Ramos, M. C.; Eriksson, M.; García-López, J.; Ranebo, Y.; García-Tenorio, R.; Betti, M.; Holm, E.

2010-09-01

In order to validate and to gain confidence in two micro-beam techniques: particle induced X-ray emission with nuclear microprobe technique (μ-PIXE) and synchrotron radiation induced X-ray fluorescence in a confocal alignment (confocal SR μ-XRF) for characterization of microscopic particles containing actinide elements (mixed plutonium and uranium) a comparative study has been performed. Inter-comparison of the two techniques is essential as the X-ray production cross-sections for U and Pu are different for protons and photons and not well defined in the open literature, especially for Pu. The particles studied consisted of nuclear weapons material, and originate either in the so called Palomares accident in Spain, 1966 or in the Thule accident in Greenland, 1968. In the determination of the average Pu/U mass ratios (not corrected by self-absorption) in the analysed microscopic particles the results from both techniques show a very good agreement. In addition, the suitability of both techniques for the analysis with good resolution (down to a few μm) of the Pu/U distribution within the particles has been proved. The set of results obtained through both techniques has allowed gaining important information concerning the characterization of the remaining fissile material in the areas affected by the aircraft accidents. This type of information is essential for long-term impact assessments of contaminated sites.

Raman spectroscopy characterization of actinide oxides (U 1-yPu y)O 2: Resistance to oxidation by the laser beam and examination of defects

NASA Astrophysics Data System (ADS)

Jégou, C.; Caraballo, R.; Peuget, S.; Roudil, D.; Desgranges, L.; Magnin, M.

2010-10-01

Structural changes in four (U 1-yPu y)O 2 materials with very different plutonium concentrations (0 ⩽ y ⩽ 1) and damage levels (up to 110 dpa) were studied by Raman spectroscopy. The novel experimental approach developed for this purpose consisted in using a laser beam as a heat source to assess the reactivity and structural changes of these materials according to the power supplied locally by the laser. The experiments were carried out in air and in water with or without hydrogen peroxide. As expected, the material response to oxidation in air depends on the plutonium content of the test oxide. At the highest power levels U 3O 8 generally forms with UO 2 whereas no significant change in the spectra indicating oxidation is observed for samples with high plutonium content ( 239PuO 2). Samples containing 25 wt.% plutonium exhibit intermediate behavior, typified mainly by a higher-intensity 632 cm -1 peak and the disappearance of the 1LO peak at 575 cm -1. This can be attributed to the presence of anion sublattice defects without any formation of higher oxides. The range of materials examined also allowed us to distinguish partly the chemical effects of alpha self-irradiation. The results obtained with water and hydrogen peroxide (a water radiolysis product) on a severely damaged 238PuO 2 specimen highlight a specific behavior, observed for the first time.

Activity measurements of a suite of radionuclides (241Am, 239,240Pu, 238Pu, 238U, 234U, 235U, 232Th, 230Th, 228Th, 228Ra, 137Cs, 210Pb, 90Sr and 40K) in biota reference material (Ocean Shellfish): CCRI(II)-S3

NASA Astrophysics Data System (ADS)

Nour, S.; Karam, L. R.; Inn, K. G. W.

2012-01-01

In 2005, the CCRI decided that a comparison undertaken from 2002 to 2008 by the NIST (under the auspices of the Inter-America Metrology System [SIM]) in the development of a new biota (Ocean Shellfish) standard reference material (SRM) was sufficiently well constructed that it could be converted into a supplementary comparison under CCRI(II), with comparison identifier CCRI(II)-S3. This would enable the comparison to be used to support calibration and measurement capability (CMC) claims for radionuclide measurements in reference materials (specifically, animal-based organic materials). Previous comparisons of radionuclides have been of single or multiple nuclides in non-complex matrices and results of such could not be extended to support capabilities to measure the same nuclides in reference materials. The results of this comparison have been used to determine the certified reference value of the SRM. The key comparison working group (KCWG) of the CCRI(II) has approved this approach as a mechanism to link all the results to certified 'reference values' in lieu of the key comparison reference value (KCRV) of these specified radionuclides in this type of matrix (shellfish) so as to support CMCs of similar materials submitted by the present participants. Main text. To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database kcdb.bipm.org/. The final report has been peer-reviewed and approved for publication by the CCRI, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

The coupling between flame surface dynamics and species mass conservation in premixed turbulent combustion

NASA Technical Reports Server (NTRS)

Trouve, A.; Veynante, D.; Bray, K. N. C.; Mantel, T.

1994-01-01

Current flamelot models based on a description of the flame surface dynamics require the closure of two inter-related equations: a transport equation for the mean reaction progress variable, (tilde)c, and a transport equation for the flame surface density, Sigma. The coupling between these two equations is investigated using direct numerical simulations (DNS) with emphasis on the correlation between the turbulent fluxes of (tilde)c, bar(pu''c''), and Sigma, (u'')(sub S)Sigma. Two different DNS databases are used in the present work: a database developed at CTR by A. Trouve and a database developed by C. J. Rutland using a different code. Both databases correspond to statistically one-dimensional premixed flames in isotropic turbulent flow. The run parameters, however, are significantly different, and the two databases correspond to different combustion regimes. It is found that in all simulated flames, the correlation between bar(pu''c'') and (u'')(sub S)Sigma is always strong. The sign, however, of the turbulent flux of (tilde)c or Sigma with respect to the mean gradients, delta(tilde)c/delta(x) or delta(Sigma)/delta(x), is case-dependent. The CTR database is found to exhibit gradient turbulent transport of (tilde)c and Sigma, whereas the Rutland DNS features counter-gradient diffusion. The two databases are analyzed and compared using various tools (a local analysis of the flow field near the flame, a classical analysis of the conservation equation for (tilde)(u''c''), and a thin flame theoretical analysis). A mechanism is then proposed to explain the discrepancies between the two databases and a preliminary simple criterion is derived to predict the occurrence of gradient/counter-gradient turbulent diffusion.

Extension of the Dytlewski-style dead time correction formalism for neutron multiplicity counting to any order

NASA Astrophysics Data System (ADS)

Croft, Stephen; Favalli, Andrea

2017-10-01

Neutron multiplicity counting using shift-register calculus is an established technique in the science of international nuclear safeguards for the identification, verification, and assay of special nuclear materials. Typically passive counting is used for Pu and mixed Pu-U items and active methods are used for U materials. Three measured counting rates, singles, doubles and triples are measured and, in combination with a simple analytical point-model, are used to calculate characteristics of the measurement item in terms of known detector and nuclear parameters. However, the measurement problem usually involves more than three quantities of interest, but even in cases where the next higher order count rate, quads, is statistically viable, it is not quantitatively applied because corrections for dead time losses are currently not available in the predominant analysis paradigm. In this work we overcome this limitation by extending the commonly used dead time correction method, developed by Dytlewski, to quads. We also give results for pents, which may be of interest for certain special investigations. Extension to still higher orders, may be accomplished by inspection based on the sequence presented. We discuss the foundations of the Dytlewski method, give limiting cases, and highlight the opportunities and implications that these new results expose. In particular there exist a number of ways in which the new results may be combined with other approaches to extract the correlated rates, and this leads to various practical implementations.

Extension of the Dytlewski-style dead time correction formalism for neutron multiplicity counting to any order

DOE Office of Scientific and Technical Information (OSTI.GOV)

Croft, Stephen; Favalli, Andrea

Here, neutron multiplicity counting using shift-register calculus is an established technique in the science of international nuclear safeguards for the identification, verification, and assay of special nuclear materials. Typically passive counting is used for Pu and mixed Pu-U items and active methods are used for U materials. Three measured counting rates, singles, doubles and triples are measured and, in combination with a simple analytical point-model, are used to calculate characteristics of the measurement item in terms of known detector and nuclear parameters. However, the measurement problem usually involves more than three quantities of interest, but even in cases where themore » next higher order count rate, quads, is statistically viable, it is not quantitatively applied because corrections for dead time losses are currently not available in the predominant analysis paradigm. In this work we overcome this limitation by extending the commonly used dead time correction method, developed by Dytlewski, to quads. We also give results for pents, which may be of interest for certain special investigations. Extension to still higher orders, may be accomplished by inspection based on the sequence presented. We discuss the foundations of the Dytlewski method, give limiting cases, and highlight the opportunities and implications that these new results expose. In particular there exist a number of ways in which the new results may be combined with other approaches to extract the correlated rates, and this leads to various practical implementations.« less

Extension of the Dytlewski-style dead time correction formalism for neutron multiplicity counting to any order

DOE PAGES

Croft, Stephen; Favalli, Andrea

2017-07-16

Here, neutron multiplicity counting using shift-register calculus is an established technique in the science of international nuclear safeguards for the identification, verification, and assay of special nuclear materials. Typically passive counting is used for Pu and mixed Pu-U items and active methods are used for U materials. Three measured counting rates, singles, doubles and triples are measured and, in combination with a simple analytical point-model, are used to calculate characteristics of the measurement item in terms of known detector and nuclear parameters. However, the measurement problem usually involves more than three quantities of interest, but even in cases where themore » next higher order count rate, quads, is statistically viable, it is not quantitatively applied because corrections for dead time losses are currently not available in the predominant analysis paradigm. In this work we overcome this limitation by extending the commonly used dead time correction method, developed by Dytlewski, to quads. We also give results for pents, which may be of interest for certain special investigations. Extension to still higher orders, may be accomplished by inspection based on the sequence presented. We discuss the foundations of the Dytlewski method, give limiting cases, and highlight the opportunities and implications that these new results expose. In particular there exist a number of ways in which the new results may be combined with other approaches to extract the correlated rates, and this leads to various practical implementations.« less

Fission track astrology of three Apollo 14 gas-rich breccias

NASA Technical Reports Server (NTRS)

Graf, H.; Shirck, J.; Sun, S.; Walker, R.

1973-01-01

The three Apollo 14 breccias 14301, 14313, and 14318 all show fission xenon due to the decay of Pu-244. To investigate possible in situ production of the fission gas, an analysis was made of the U-distribution in these three breccias. The major amount of the U lies in glass clasts and in matrix material and no more than 25% occurs in distinct high-U minerals. The U-distribution of each breccia is discussed in detail. Whitlockite grains in breccias 14301 and 14318 found with the U-mapping were etched and analyzed for fission tracks. The excess track densities are much smaller than indicated by the Xe-excess. Because of a preirradiation history documented by very high track densities in feldspar grains, however, it is impossible to attribute the excess tracks to the decay of Pu-244. A modified track method has been developed for measuring average U-concentrations in samples containing a heterogeneous distribution of U in the form of small high-U minerals. The method is briefly discussed, and results for the rocks 14301, 14313, 14318, 68815, 15595, and the soil 64421 are given.

Fission cross-sections, prompt fission neutron and γ-ray emission in request for nuclear applications

NASA Astrophysics Data System (ADS)

Hambsch, F.-J.; Salvador-Castiñeira, P.; Oberstedt, S.; Göök, A.; Billnert, R.

2016-06-01

In recent years JRC-IRMM has been investigating fission cross-sections of 240,242Pu in the fast-neutron energy range relevant for innovative reactor systems and requested in the High Priority Request List (HPRL) of the OECD/Nuclear Energy Agency (NEA). In addition to that, prompt neutron multiplicities are being investigated for the major isotopes 235U, 239Pu in the neutron-resonance region using a newly developed scintillation detector array (SCINTIA) and an innovative modification of the Frisch-grid ionisation chamber for fission-fragment detection. These data are highly relevant for improved neutron data evaluation and requested by the OECD/Working Party on Evaluation Cooperation (WPEC). Thirdly, also prompt fission γ-ray emission is investigated using highly efficient lanthanide-halide detectors with superior timing resolution. Again, those data are requested in the HPRL for major actinides to solve open questions on an under-prediction of decay heat in nuclear reactors. The information on prompt fission neutron and γ-ray emission is crucial for benchmarking nuclear models to study the de-excitation process of neutron-rich fission fragments. Information on γ-ray emission probabilities is also useful in decommissioning exercises on damaged nuclear power plants like Fukushima Daiichi to which JRC-IRMM is contributing. The results on the 240,242Pu fission cross section, 235U prompt neutron multiplicity in the resonance region and correlations with fission fragments and prompt γ-ray emission for several isotopes will be presented and put into perspective.

Rigid palm oil-based polyurethane foam reinforced with diamine-modified montmorillonite nanoclay

NASA Astrophysics Data System (ADS)

Haziq Dzulkifli, Mohd; Yazid Yahya, Mohd; Majid, Rohah A.

2017-05-01

This paper presents work on organically-modified montmorillonite (MMT) nanoclay embedded in rigid palm oil-based polyurethane (PU) foam. MMT was modified with organic surfactant diamino propane (DAP). PU foam was fabricated in closed mold, and the amount of DAP-MMT was varied in each foam formulation. The obtained foam was tested for its microstructure and morphology. Appearance of peaks from infra-red spectra corresponding to N-H, C=O, and C-N confirms the formation of PU networks. Scanning electron microscopy (SEM) revealed fine, closed-cellular structure at low clay loading; increasing DAP-MMT content induced larger cell sizes with blowholes. X-ray diffraction (XRD) indicates fully-exfoliated clays at 1 wt. % and partial-exfoliation at 3 wt. % clay loading, suggesting clumping of clays as DAP-MMT content increased.

PU-ICE Summary Information.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moore, Michael

The Generator Knowledge Report for the Plutonium Isentropic Compression Experiment Containment Systems (GK Report) provides information for the Plutonium Isentropic Compression Experiment (Pu- ICE) program to support waste management and characterization efforts. Attachment 3-18 presents generator knowledge (GK) information specific to the eighteenth Pu-ICE conducted in August 2015, also known as ‘Shot 18 (Aug 2015) and Pu-ICE Z-2841 (1).’ Shot 18 (Aug 2015) was generated on August 28, 2015 (1). Calculations based on the isotopic content of Shot 18 (Aug 2015) and the measured mass of the containment system demonstrate the post-shot containment system is low-level waste (LLW). Therefore, thismore » containment system will be managed at Sandia National Laboratory/New Mexico (SNL/NM) as LLW. Attachment 3-18 provides documentation of the TRU concentration and documents the concentration of any hazardous constituents.« less

Mound Laboratory activities for the Division of Physical Research: July--December 1975

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1976-05-14

Research and development are reported in the following areas: isotope separation and production for Ar, C, He, Kr, Ne, O, S, and Xe; testing of cubic B crystals for superconductivity; metal hydride research on band theory and electronic structure and spin-lattice relaxation times for VH/sub x/; separation chemistry of Pu, /sup 231/Pa, /sup 230/Th, /sup 229/Th, and /sup 234/U; adsorption of U and Pu by bone char; separation research for Ca and S isotopes; molecular beam scattering for Ar--Kr; and transport properties for the systems Ne--Ar, Ne--Kr, and Ar--Kr. (JSR)

Synthesis and X-ray Crystallography of [Mg(H2O)6][AnO2(C2H5COO)3]2 (An = U, Np, or Pu).

PubMed

Serezhkin, Viktor N; Grigoriev, Mikhail S; Abdulmyanov, Aleksey R; Fedoseev, Aleksandr M; Savchenkov, Anton V; Serezhkina, Larisa B

2016-08-01

Synthesis and X-ray crystallography of single crystals of [Mg(H2O)6][AnO2(C2H5COO)3]2, where An = U (I), Np (II), or Pu (III), are reported. Compounds I-III are isostructural and crystallize in the trigonal crystal system. The structures of I-III are built of hydrated magnesium cations [Mg(H2O)6](2+) and mononuclear [AnO2(C2H5COO)3](-) complexes, which belong to the AB(01)3 crystallochemical group of uranyl complexes (A = AnO2(2+), B(01) = C2H5COO(-)). Peculiarities of intermolecular interactions in the structures of [Mg(H2O)6][UO2(L)3]2 complexes depending on the carboxylate ion L (acetate, propionate, or n-butyrate) are investigated using the method of molecular Voronoi-Dirichlet polyhedra. Actinide contraction in the series of U(VI)-Np(VI)-Pu(VI) in compounds I-III is reflected in a decrease in the mean An═O bond lengths and in the volume and sphericity degree of Voronoi-Dirichlet polyhedra of An atoms.

Prompt fission neutron spectra from fission induced by 1 to 8 MeV neutrons on U235 and Pu239 using the double time-of-flight technique

NASA Astrophysics Data System (ADS)

Noda, S.; Haight, R. C.; Nelson, R. O.; Devlin, M.; O'Donnell, J. M.; Chatillon, A.; Granier, T.; Bélier, G.; Taieb, J.; Kawano, T.; Talou, P.

2011-03-01

Prompt fission neutron spectra from U235 and Pu239 were measured for incident neutron energies from 1 to 200 MeV at the Weapons Neutron Research facility (WNR) of the Los Alamos Neutron Science Center, and the experimental data were analyzed with the Los Alamos model for the incident neutron energies of 1-8 MeV. A CEA multiple-foil fission chamber containing deposits of 100 mg U235 and 90 mg Pu239 detected fission events. Outgoing neutrons were detected by the Fast Neutron-Induced γ-Ray Observer array of 20 liquid organic scintillators. A double time-of-flight technique was used to deduce the neutron incident energies from the spallation target and the outgoing energies from the fission chamber. These data were used for testing the Los Alamos model, and the total kinetic energy parameters were optimized to obtain a best fit to the data. The prompt fission neutron spectra were also compared with the Evaluated Nuclear Data File (ENDF/B-VII.0). We calculate average energies from both experimental and calculated fission neutron spectra.

The high-temperature heat capacity of the (Th,U)O 2 and (U,Pu)O 2 solid solutions

DOE PAGES

Valu, S. O.; Benes, O.; Manara, D.; ...

2016-11-09

The enthalpy increment data for the (Th,U)O 2 and (U,Pu)O 2 solid solutions are reviewed and complemented with new experimental data (400–1773 K) and many-body potential model simulations. The results of the review show that from room temperature up to about 2000 K the enthalpy data are in agreement with the additivity rule (Neumann-Kopp) in the whole composition range. Above 2000 K the effect of Oxygen Frenkel Pair (OFP) formation leads to an excess enthalpy (heat capacity) that is modeled using the enthalpy and entropy of OFP formation from the end-members. Here, a good agreement with existing experimental work ismore » observed, and a reasonable agreement with the results of the many-body potential model, which indicate the presence of the diffuse Bredig (superionic) transition that is not found in the experimental enthalpy increment data.« less

Crater Floor and Lava Lake Dynamics Measured with T-LIDAR at Pu`u`O`o Crater, Hawai`i

NASA Astrophysics Data System (ADS)

Brooks, B. A.; Kauahikaua, J. P.; Foster, J. H.; Poland, M. P.

2007-12-01

We used a near-infrared (1.2 micron wavelength) tripod-based scanning LiDAR system (T-LIDAR) to capture crater floor and lava lake dynamics in unprecedented detail at P`u`u `O`o crater on Kilauea volcano, Hawai`i. In the ~40 days following the June 17-19 intrusion/eruption, Pu`u `O`o crater experienced substantial deformation comprising 2 collapse events bracketing rapid filling of the crater by a lava lake. We surveyed the crater floor with centimeter-scale spot-spacings from 3 different vantage points on July 13 and from one vantage point on July 24. Data return was excellent despite heavy fume on July 24 that obscured nearly all of the crater features, including the walls and floor. We formed displacement fields by aligning identical features from different acquisition times in zones on the relatively stable crater walls. From July 13, over a period of several hours, we imaged ~2 m of differential lava lake surface topography from the upwelling (eastern) to downstream (western) portion of the flowing lava lake. From July 13 to July 24, the lava lake level dropped by as much as 20 meters in a zone confined by flanking levees. Our results confirm the utility of T-LiDAR as a new tool for detailed volcano geodesy studies and suggest potential applications in volcano hazards monitoring.

Particular features of ternary fission induced by polarized neutrons in the major actinides U,235233 and Pu,241239

NASA Astrophysics Data System (ADS)

Gagarski, A.; Gönnenwein, F.; Guseva, I.; Jesinger, P.; Kopatch, Yu.; Kuzmina, T.; Lelièvre-Berna, E.; Mutterer, M.; Nesvizhevsky, V.; Petrov, G.; Soldner, T.; Tiourine, G.; Trzaska, W. H.; Zavarukhina, T.

2016-05-01

Ternary fission in (n ,f ) reactions was studied with polarized neutrons for the isotopes U,235233 and Pu,241239. A cold longitudinally polarized neutron beam was available at the High Flux Reactor of the Institut Laue-Langevin in Grenoble, France. The beam was hitting the fissile targets mounted at the center of a reaction chamber. Detectors for fission fragments and ternary particles were installed in a plane perpendicular to the beam. In earlier work it was discovered that the angular correlations between neutron spin and the momenta of fragments and ternary particles were very different for 233U or 235U. These correlations could now be shown to be simultaneously present in all of the above major actinides though with different weights. For one of the correlations it was observed that up to scission the compound nucleus is rotating with the axis of rotation parallel to the neutron beam polarization. Entrained by the fragments also the trajectories of ternary particles are turned away albeit by a smaller angle. The difference in turning angles becomes observable upon reversing the sense of rotation by flipping neutron spin. All turning angles are smaller than 1∘. The phenomenon was called the ROT effect. As a distinct second phenomenon it was found that for fission induced by polarized neutrons an asymmetry in the emission probability of ternary particles relative to a plane formed by fragment momentum and neutron spin appears. The asymmetry is attributed to the Coriolis force present in the nucleus while it is rotating up to scission. The size of the asymmetry is typically 10-3. This asymmetry was termed the TRI effect. The interpretation of both effects is based on the transition state model. Both effects are shown to be steered by the properties of the collective (J ,K ) transition states which are specific for any of the reactions studied. The study of asymmetries of ternary particle emission in fission induced by slow polarized neutrons provides a new method for the spectroscopy of transition states (J ,K ) near the fission barrier. Implications of collective rotation on fragment angular momenta are discussed.

Determination of the fast-neutron-induced fission cross-section of 242Pu at nELBE

NASA Astrophysics Data System (ADS)

Kögler, Toni; Beyer, Roland; Junghans, Arnd R.; Schwengner, Ronald; Wagner, Andreas

2018-03-01

The fast-neutron-induced fission cross section of 242Pu was determined in the energy range of 0.5 MeV to 10MeV at the neutron time-of-flight facility nELBE. Using a parallel-plate fission ionization chamber this quantity was measured relative to 235U(n,f). The number of target nuclei was thereby calculated by means of measuring the spontaneous fission rate of 242Pu. An MCNP 6 neutron transport simulation was used to correct the relative cross section for neutron scattering. The determined results are in good agreement with current experimental and evaluated data sets.

Splinter Protection for Airbase Firefighting Resources

DTIC Science & Technology

1989-12-01

shotcrete) arch structure. The system was developed by Earth Systems, Inc. (ESI) of Durango , Colorado . The concept consists of the reinforced concrete floor...by ESI of Durango , Colorado . Appendix B presents a portion of the ESI construction manual that is supplied with their structural kit. Only the portion...Construction Manual for Shotcrete Arch Structure is copyrightea; it is the sole property of SEARTH SYSTEMS, INC., P.U. box 3270, Durango , Colorado . The

The Pu'u 'O'o-Kupaianaha Eruption of Kilauea Volcano, Hawaii: The First 20 Years

USGS Publications Warehouse

Heliker, Christina C.; Swanson, Donald A.; Takahashi, Taeko Jane

2003-01-01

The Pu'u 'O'o-Kupaianaha eruption started on January 3, 1983. The ensuing 20-year period of nearly continuous eruption is the longest at Kilauea Volcano since the famous lava-lake activity of the 19th century. No rift-zone eruption in more than 600 years even comes close to matching the duration and volume of activity of these past two decades. Fortunately, such a landmark event came during a period of remarkable technological advancements in volcano monitoring. When the eruption began, the Global Positioning System (GPS) and the Geographic Information System (GIS) were but glimmers on the horizon, broadband seismology was in its infancy, and the correlation spectrometer (COSPEC), used to measure SO2 flux, was still very young. Now, all of these techniques are employed on a daily basis to track the ongoing eruption and construct models about its behavior. The 12 chapters in this volume, written by present or past Hawaiian Volcano Observatory staff members and close collaborators, celebrate the growth of understanding that has resulted from research during the past 20 years of Kilauea's eruption. The chapters range widely in emphasis, subject matter, and scope, but all present new concepts or important modifications of previous ideas - in some cases, ideas long held and cherished.

Topological analysis of void space in phosphate frameworks: Assessing storage properties for the environmentally important guest molecules and ions: CO 2, H 2O, UO 2, PuO 2, U, Pu, Sr 2+, Cs +, CH 4, and H 2

DOE PAGES

Cramer, Alisha J.; Cole, Jacqueline M.

2016-06-27

The entrapment of environmentally important materials to enable containment of polluting wastes from industry or energy production, storage of alternative fuels, or water sanitation, is of vital and immediate importance. Many of these materials are small molecules or ions that can be encapsulated via their adsorption into framework structures to create a host-guest complex. This is an ever-growing field of study and, as such, the search for more suitable porous materials for environmental applications is fundamental to progress. However, many industrial areas that require the use of adsorbents are fraught with practical challenges such as high temperatures, rapid gas expansion,more » radioactivity, or repetitive gas cycling, that the host material must withstand. Inorganic phosphates have a proven history of rigid structures, thermal stability, and are suspected to possess good resistance to radiation over geologic time scales. Furthermore, various experimental studies have established their ability to adsorb small molecules, such as water. In light of this, all known crystal structures of phosphate frameworks with meta- (P 3O 9) or ultra- (P 5O 14) stoichiometries are combined in a data-mining survey together with all theoretically possible structures of Ln aP bO c (where a, b, c are any integer, and Ln = La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, or Tm) that are statistically likely to form. Topological patterns within these framework structures are used to assess their suitability for hosting a variety of small guest molecules or ions that are important for environmental applications: CO 2, H 2O, UO 2, PuO 2, U, Pu, Sr 2+, Cs +, CH 4 and H 2. A range of viable phosphate-based host-guest complexes are identified from this data-mining and pattern-based structural analysis. Moreover, distinct topological preferences for hosting such guests are found, and metaphosphate stoichiometries are generally preferred over ultraphosphate configurations.« less

VEPP Exercise: Volcanic Activity and Monitoring of Pu`u `O`o, Kilauea Volcano, Hawaii

NASA Astrophysics Data System (ADS)

Rodriguez, L. A.

2010-12-01

A 10-week project will be tested during the Fall semester 2010, for a Volcanic Hazards elective course, for undergraduate Geology students of the University of Puerto Rico at Mayaguez. This exercise was developed during the Volcanoes Exploration Project: Pu`u `O`o (VEPP) Workshop, held on the Big Island of Hawaii in July 2010. For the exercise the students will form groups (of 2-4 students), and each group will be assigned a monitoring technique or method, among the following: seismic (RSAM data), deformation (GPS and tilt data), observations (webcam and lava flow maps), gas and thermal monitoring. The project is designed for Geology undergraduates who have a background in introductory geology, types of volcanoes and eruptions, magmatic processes, characteristics of lava flows, and other related topics. It is divided in seven tasks, starting with an introduction and demonstration of the VEPP website and the VALVE3 software, which is used to access monitoring data from the current eruption of Pu`u `O`o, Kilauea volcano, Hawaii. The students will also familiarize themselves with the history of Kilauea volcano and its current eruption. At least weekly the groups will acquire data (mostly near-real-time) from the different monitoring techniques, in the form of time series, maps, videos, and images, in order to identify trends in the data. The groups will meet biweekly in the computer laboratory to work together in the analysis and interpretation of the data, with the support of the instructor. They will give reports on the progress of the exercise, and will get feedback from the instructor and from the other expert groups. All groups of experts will relate their findings to the recent and current activity of Kilauea volcano, and the importance of their specific type of monitoring. The activity will culminate with a written report and an oral presentation. The last task of the project consists of a wrap-up volcano monitoring exercise, in which the students will participate in a 1-hr discussion and will report on what they think will happen at Kilauea in the near future. Students will be evaluated based on group participation, progress reports and discussions, the written and oral reports, and the final wrap-up exercise. This project can be modified to be based on any 10-week period in the eruption, for which data can be accessed through the VEPP web site. It can also include data from other volcanoes, if data are available from volcano observatories and/or government agencies.

AMS of the Minor Plutonium Isotopes

NASA Astrophysics Data System (ADS)

Steier, P.; Hrnecek, E.; Priller, A.; Quinto, F.; Srncik, M.; Wallner, A.; Wallner, G.; Winkler, S.

2013-01-01

VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure 239Pu, 240Pu, 241Pu, 242Pu and 244Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of 244Pu/239Pu = (5.7 ± 1.0) × 10-5 based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the 242Pu/240Pu ratio as an estimate of the initial 241Pu/239Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method.

Real time studies of Elastic Moduli Pu Aging using Resonant Ultrasound Spectroscopy

NASA Astrophysics Data System (ADS)

Maiorov, Boris

Elastic moduli are fundamental thermodynamic susceptibilities that connect directly to thermodynamics, electronic structure and give important information about mechanical properties. To determine the time evolution of the elastic properties in 239Pu and it Ga alloys, is imperative to study its phase stability and self-irradiation damage process. The most-likely sources of these changes include a) ingrowth of radioactive decay products like He and U, b) the introduction of radiation damage, c) δ-phase instabilities towards α-Pu or to Pu3Ga. The measurement of mechanical resonance frequencies can be made with extreme precision and used to compute the elastic moduli without corrections giving important insight in this problem. Using Resonant Ultrasound Spectroscopy, we measured the time dependence of the mechanical resonance frequencies of fine-grained polycrystalline δ-phase 239Pu, from 300K up to 480K. At room temperature, the shear modulus shows an increase in time (stiffening), but the bulk modulus decreases (softening). These are the first real-time measurements of room temperature aging of the elastic moduli, and the changes are consistent with elastic moduli measurements performed on 44 year old δ-Pu. As the temperature is increased, the rate of change increases exponentially, with both moduli becoming stiffer with time. For T>420K an abrupt change in the time dependence is observed indicating that the bulk and shear moduli have opposite rates of change. Our measurements provide a basis for ruling out the decomposition of δ-Pu towards α-Pu or Pu3Ga, and indicate a complex defect-related scenario from which we are gathering important clues.

Durability test on irradiated rock-like oxide fuels

NASA Astrophysics Data System (ADS)

Kuramoto, K.; Nitani, N.; Yamashita, T.

2003-06-01

For a profitable use of Pu, Japan Atomic Energy Research Institute has been promoting researches for once-through type fuels. The strategy consists of stable rock-like oxide fuel fabrication in conventional fuel facilities followed by almost complete Pu burning in LWR and disposal of chemically stable spent fuel without further processing. Because leach rates of hazardous nuclides, such as TRU and β-emitters, that have long half-lives, are very important for the evaluation of geological safety, leaching tests in deionized water at 363 K were performed with reference to the MCC-1 method. Five irradiated fuel pellets, a single phase fuel of a yttria-stabilized zirconia (YSZ) containing UO 2 (U-YSZ), two fuels of U-YSZ particle dispersed in MgAl 2O 4 (SPI) or Al 2O 3 (COR) matrix, two homogeneous-blended fuels of U-YSZ and SPI or COR powders, were submitted to the tests. Stainless steel containers with Au coating and ethylene propylene diene monomer were used as leaching vessels and packing, respectively. The evaluated normalized leach rates of Zr, U and Pu were obviously lower than those of the other important elements and nuclides. Americium, Np and especially Y showed unexpectedly high evaluated normalized leach rates. The volatile elements, Cs and I, showed enhanced leaching within particle-dispersed type fuels because of crack formation around the particle.

Surface modified and medicated polyurethane materials capable of controlling microorganisms causing foot skin infection in athletes.

PubMed

Gnanasundaram, Saraswathy; Ranganathan, Mohan; Das, Bhabendra Nath; Mandal, Asit Baran

2013-02-01

Foot odor and foot infection are major problems of athletes and persons with hyperhidrosis. Many shoes especially sports shoes have removable cushion insoles/foot beds for foot comfort. Polyurethane (PU) foam and elastomer have been used as cushion insole in shoes. In the present work, new insole materials based on porous viscoelastic PU sheets having hydrophilic property and antimicrobial drug coating to control foot infection and odor were developed. Bacteria and fungus that are causing infection and bad odor of the foot of athletes were isolated by microbial cell culturing of foot sweat. The surface of porous viscoelastic PU sheets was modified using hydrophilic polymers and coated with antimicrobial agent, silver sulfadiazine (SS). The surface modified PU sheets were characterized using ATR-FTIR, TGA, DSC, SEM, contact angle measurement and water absorption study. Results had shown that modified PU sheets have hydrophilicity greater than that of original PU sheet. FTIR spectra and SEM pictures confirmed modification of PU surface with hydrophilic polymers and coating with SS. Minimum inhibitory concentration studies indicated that SS has activity on all isolated bacteria of athletic foot sweat. The maximum inhibition was found for Pseudomonas (20mm) followed by Micrococci (17 mm), Diphtheroids (16 mm) and Staphylococci (12 mm). During perspiration of foot the hydrophilic polymers on PU surface will swell and release SS. Future work will confirm the application of these materials as inserts in athletic shoes. Copyright © 2012 Elsevier B.V. All rights reserved.

Autonomic stress reactivity and craving in individuals with problematic Internet use.

PubMed

Moretta, Tania; Buodo, Giulia

2018-01-01

The link between autonomic stress reactivity and subjective urge/craving has been less systematically examined in behavioral addictions (i.e. problematic Internet use) than in substance use disorders. The present study investigated whether problematic Internet users (PU) show enhanced autonomic stress reactivity than non-PU, indexed by lower Heart Rate Variability (HRV) and higher Skin Conductance Level (SCL) reactivity during the Trier Social Stress Test (TSST), whether greater reactivity is related to stronger Internet craving, and whether problematic Internet usage is associated with some dysfunctional psychological features. Based on their Internet Addiction Test scores, participants were divided into PU (N = 24) and non-PU (N = 21). Their heart rate and skin conductance were continuously recorded during baseline, social stressors, and recovery. Craving for Internet usage were collected using a Likert scale before and after the TSST. The SDNN, an overall measure of HRV, was significantly lower in PU than non-PU during baseline, but not during and after stressful task. Furthermore, only among PU a significant negative correlation emerged between SDNN during recovery and craving ratings after the test. No group differences emerged for SCL. Lastly, PU endorsed more mood, obsessive-compulsive, and alcohol-related problems. Our findings suggest that problems in controlling one's use of the Internet may be related to reduced autonomic balance at rest. Moreover, our results provide new insights into the characterization of craving in PIU, indicating the existence of a relationship between craving for Internet usage and reduced autonomic flexibility.

Gamma-ray mirror technology for NDA of spent fuel

DOE Office of Scientific and Technical Information (OSTI.GOV)

Descalle, M. A.; Ruz-Armendariz, J.; Decker, T.

Direct measurements of gamma rays emitted by fissile material have been proposed as an alternative to measurements of the gamma rays from fission products. From a safeguards applications perspective, direct detection of uranium (U) and plutonium (Pu) K-shell fluorescence emission lines and specific lines from some of their isotopes could lead to improved shipper-receiver difference or input accountability at the start of Pu reprocessing. However, these measurements are difficult to implement when the spent fuel is in the line-of-sight of the detector, as the detector is exposed to high rates dominated by fission product emissions. To overcome the combination ofmore » high rates and high background, grazing incidence multilayer mirrors have been proposed as a solution to selectively reflect U and Pu hard X-ray and soft gamma rays in the 90 to 420 keV energy into a high-purity germanium (HPGe) detector shielded from the direct line-of-sight of spent fuel. Several groups demonstrated that K-shell fluorescence lines of U and Pu in spent fuel could be detected with Ge detectors. In the field of hard X-ray optics the performance of reflective multilayer coated reflective optics was demonstrated up to 645 keV at the European Synchrotron Radiation Facility. Initial measurements conducted at Oak Ridge National Laboratory with sealed sources and scoping experiments conducted at the ORNL Irradiated Fuels Examination Laboratory (IFEL) with spent nuclear fuel further demonstrated the pass-band properties of multilayer mirrors for reflecting specific emission lines into 1D and 2D HPGe detectors, respectively.« less

Actinide Sorption in Rainier Mesa Tunnel Waters from the Nevada Test Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhao, P; Zavarin, M; Leif, R

2007-12-17

The sorption behavior of americium (Am), plutonium (Pu), neptunium (Np), and uranium (U) in perched Rainier Mesa tunnel water was investigated. Both volcanic zeolitized tuff samples and groundwater samples were collected from Rainier Mesa, Nevada Test Site, NV for a series of batch sorption experiments. Sorption in groundwater with and without the presence of dissolved organic matter (DOM) was investigated. Am(III) and Pu(IV) are more soluble in groundwater that has high concentrations of DOM. The sorption K{sub d} for Am(III) and Pu(IV) on volcanic zeolitized tuff was up to two orders of magnitude lower in samples with high DOM (15more » to 19 mg C/L) compared to samples with DOM removed (< 0.4 mg C/L) or samples with naturally low DOM (0.2 mg C/L). In contrast, Np(V) and U(VI) sorption to zeolitized tuff was much less affected by the presence of DOM. The Np(V) and U(VI) sorption Kds were low under all conditions. Importantly, the DOM was not found to significantly sorb to the zeolitized tuff during these experiment. The concentration of DOM in groundwater affects the transport behavior of actinides in the subsurface. The mobility of Am(III) and Pu(IV) is significantly higher in groundwater with elevated levels of DOM resulting in potentially enhanced transport. To accurately model the transport behavior of actinides in groundwater at Rainier Mesa, the low actinide Kd values measured in groundwater with high DOM concentrations must be incorporated in predictive transport models.« less

Heterogeneous UO2 fuel irradiated up to a high burn-up: Investigation of the HBS and of fission product releases

NASA Astrophysics Data System (ADS)

Noirot, J.; Lamontagne, J.; Nakae, N.; Kitagawa, T.; Kosaka, Y.; Tverberg, T.

2013-11-01

A UO2 fuel with a heterogeneous distribution of 235U was irradiated up to a high burn-up in the Halden Boiling Water Reactor (HBWR). The last 100 days of irradiation were performed with an increased level of linear power. The effect of the heterogeneous fissile isotope distribution on the formation of the HBS was studied free of the possible influence of Pu which exists in heterogeneous MOX fuels. The HBS formed in 235U-rich agglomerates and its main characteristics were very similar to those of the HBS formed in Pu-rich agglomerates of heterogeneous MOX fuels. The maximum local contents of Nd and Xe before HBS formation were studied in this fuel. In addition to a Pu effect that promotes the HBS phenomenon, comparison with previous results for heterogeneous MOX fuels showed that the local fission product concentration was not the only parameter that has to be taken into consideration. It appears that the local actinide depletion by fission and/or the energy locally deposited through electronic interactions in the fission fragment recoils also have an effect on the HBS formation threshold. Moreover, a major release of fission gases from the peripheral 235U-rich agglomerates of HBS bubbles and a Cs radial movement are also evidenced in this heterogeneous UO2. Cs deposits on the peripheral grain boundaries, including the HBS grain boundaries, are considered to reveal the release paths. SUP>235U-rich agglomerates, SUP>235U-poor areas, an intermediate phase with intermediate 235U concentrations. Short fuel rods were fabricated with these pellets. The main characteristics of these fuel rods are shown in Table 1.These rods were irradiated to high burn-ups in the IFA-609/626 of the HBWR and then one was irradiated in the IFA-702 for 100 days. Fig. 2 shows the irradiation history of this fuel. The final average burn-up of the rod was 69 GWd/tU. Due to the flux differences along the rod, however, the average burn-up of the cross section examined was 63 GWd/tU. This fuel experienced high linear powers during the first year of irradiation, but at the end of the IFA-609/626 period, the average linear power of the rod was around 12 kW/m. In the IFA-702, the power was gradually increased over 7 days from 12 kW/m to 22.5 kW/m before it was decreased again to reach ˜19 kW/m at the end of the 100 days forming this part of the irradiation. A LEICA (DM RXA2) optical microscope. A shielded electronic microprobe (EPMA) SX-100R by CAMECA. A shielded scanning electron microscope (SEM): the Philips XL30. Image acquisitions were performed using the ADDA "SIS" system with the AnalySIS software for image analysis. A shielded secondary ion mass spectrometer (SIMS): the CAMECA IMS 6f was capable of analysing the same samples as the SEM and EPMA [16-22]. In the central part of the pellet for all three phases, Xe precipitated into bubbles with very little Xe remaining outside the bubbles. Some Xe-filled bubbles were detected under the surface in this area. They appear as bright spots. Around mid-radius on the periphery of the 235U-poor areas and in the intermediate phase, Xe was depleted on the periphery of the grains. This depletion was not associated with Xe-filled bubbles that would be detected under the polished surface. Moreover, no large intergranular open bubbles were visible. Therefore, this missing gas must have been released. In the 235U-rich agglomerates all over the section, Xe precipitated into bubbles with very little Xe remaining outside the bubbles. The Xe quantitative analyses through 235U-rich agglomerates on the pellet periphery (Fig. 9) confirmed the low quantity of Xe remaining outside the bubbles. This Xe content was around 0.1 wt%. Fig. 10 shows the Xe and Nd EPMA quantitative measurements along a radius of the cross section. In this figure and in Fig. 9, the weight percentage scales were set so that the two profiles would be almost identical without Xe release or precipitation. Along the Xe axis, the Nd profile can be considered as the local Xe production. Fig. 10 shows that the Xe measurement all through the central part is low except for a few points corresponding to unopened but close to the polished surface and detected by EPMA. These points correspond to the bright spots detected in the central part in Fig. 8. High concentrations were detected locally all over the radius on the Nd profile. They correspond to the 235U-rich agglomerates or their surroundings. Outside the central part, these high Nd concentrations correspond to low Xe concentrations, consistent with the maps in Fig. 8 and the detailed analyses across large 235U-rich agglomerates (Fig. 9).Fig. 11 shows a set of Xe (wt%) and (145Nd + 146Nd)/heavy metal radial profiles both acquired by SIMS. Three profiles are show for each set: one in the 235U-rich agglomerates, one in the 235U-poor areas and one in the intermediate phase. The three phases are not homogeneous themselves. This induces differences between (145Nd + 146Nd)/HM SIMS measurement points of a given phase. The (145Nd + 146Nd)/HM results are a reference for the Xe measurements, giving an estimation of the relative Xe local production. The (145Nd + 146Nd)/HM was high in the 235U-rich agglomerates, lower in the intermediate phase and even lower in the 235U-poor areas. Differences similar to those obtained herein between the phases would have been found in the Xe measurements if no release had occurred in any of those phases. The Xe (wt%) results show that this is not the case. The Xe measurements were quite similar in the intermediate phase and in the 235U-poor areas; they would have been higher in the intermediate phase if no release had occurred. The Xe measurements in the 235U-rich agglomerates were very low and lower than in the two other phases. For the 235U-rich agglomerates, there was a very big difference, across the entire radius, between the Xe measured and the Xe local production.In the SIMS Xe measurements, local depth profiles show peaks on a base line [19]. The base line corresponds to the solid solution Xe and to the nano-bubbles. The peaks correspond to Xe in larger bubbles opened by ion beam fuel sputtering. The SIMS total values correspond to the Xe outside these bubbles plus the Xe trapped in these bubbles.Fig. 12 shows the total Xe SIMS results (already shown in Fig. 11) together with the base line measurements for each measurement point and in separate graphs for each phase. The Xe EPMA quantitative measurements used as a background for these three graphs are the same as those in Fig. 10 and are the same for the three graphs, without any phase distinction. The SIMS Xe relative measurements were calibrated through a correspondence between the SIMS base line results and the EPMA measurements [20]. As expected, the SIMS base line profile was consistent with the EPMA all along the profile for each corresponding phase. For example, the SIMS base line in the 235U-rich agglomerates corresponds to the low EPMA measurement points of the Xe in this zone, i.e. the points of the EPMA profile in the 235U-rich agglomerates. By way of comparison between the Xe and the Nd measurements (the latter being rescaled to be representative of the creation level of Xe), Fig. 11 made it possible to identify two main parts on the Xe SIMS radius: The central part 0R to ˜0.5R: In the intermediate phase and the 235U-poor areas, the SIMS total was used to identify this part as a release area. The average fraction of gas measured in the bubbles (the ratio between the gas in the bubbles and the total measurement) was between 60% and 90%. The Xe content outside the bubbles was very low. In the 235U-rich agglomerates, the SIMS total represents only a small fraction of the produced Xe, which means that a large fraction of the Xe is released or not detected by SIMS due to the large size of some agglomerate bubbles compared with the volume of the crater analysed. sim;0.5R to ˜1R: The 235U-poor areas are not release areas. The fraction of gas in bubbles measured in these areas remained low, ˜5%. The intermediate phase is a release area with moderate release. The average fraction of gas measured in the bubbles was around 20%. In the 235U-rich agglomerates, the Xe SIMS total was very low. This part is a release area. Sharp transitions between initial microstructure and the HBS, often inside one grain. Increase in the resulting grain size with increasing distance from the pellet periphery. The grain sizes are in fact consistent with the MOX measurements [2]. Increase in the bubble size with the increasing distance from the pellet periphery, consistent with the MOX measurements. Smaller bubbles tend to be found in the peripheral part of the 235U-rich agglomerates rather than in their central part. Sharp transition, around 0.5R, between the peripheral area where the conventional form of HBS forms in the 235U-rich agglomerates and the central part where much larger bubbles form and where the grain size is also clearly larger. Xe concentration of 0.1 wt% outside the bubbles in the HBS areas is consistent with the [2] MOX measurements at equivalent local burn-ups. The heterogeneous MOX fuels examinations have firmly established that the HBS can extend outside the Pu-rich agglomerates due to the implantation of fission products around these agglomerates. Similarly, it has been shown that the small Pu-rich agglomerates can remain with the initial microstructure even if there is a similar actual local burn-up, a large rate of fission products being implanted outside the agglomerates themselves so that the local fission product concentration remains low.In this 235U heterogeneous UO2, the Xe and Nd concentration levels reached at the HBS formation limit ranged between 0.8 wt% and 1.1 wt% for Xe and between 0.63 wt% and 0.83 wt% for Nd. These ranges are similar to what was reported in [23] for the UO2 rim. These limits are, however, slightly higher than those found for Pu-rich agglomerates in heterogeneous MOX fuels in [2] or in [24]. Nonetheless, they are clearly lower than the concentrations reached without HBS in the special Pu-poor spots in [2]. In these spots, UO2 particles in heterogeneous MOX were really close or even surrounded by Pu-rich areas. As a result, their fission product content, due to recoil, was almost the same as that in the surrounding Pu-rich agglomerates themselves despite a very low actual local burn-up. In these special UO2 spots in MOX fuel, 1.4 wt% was reached for Xe and no HBS formed.If these high Xe concentrations without HBS in the special spots in [2] were made possible by the very low Pu local concentration only, very high Xe concentrations should have been common around the heterogeneous UO2 fuel 235U-rich agglomerates, since the Pu level was low everywhere in this fuel. This is not what was observed.Even if this effect due to a high fission product level reached without the formation of a HBS (as reported in [2] for heterogeneous MOX fuels in the special spots) is partially due to the very low local Pu level, it does not seem to be the only reason. It also seems to be partly due to the very low level of actual fissions occurring there. Between a rich agglomerate and such a highly implanted area there is: The same local fission product build-up and associated damage (due to cascades from the nuclei interactions during the last part of the fission fragment recoil). A large difference in the actinide isotope depletion to the extent that a difference in chemical composition exists between the two. A difference in the electronic excitation level at the beginning of the fission fragment recoil, higher in Pu agglomerates and in 235U-rich agglomerates than in the low fissile content areas, even surrounded by rich areas. The last two points may have an effect on the formation of a HBS though this paper cannot say which one is the most significant.The highest levels reached for Xe and Nd without HBS in the 235U heterogeneous fuel are very likely to correspond to places where the initial 235U content was particularly low but where fission recoil led to these high levels. The maximum concentrations of fission products reached before the formation of a HBS in the 235U heterogeneous fuel are lower than for the heterogeneous MOX special Pu-poor spots. This is most certainly due to the local 235U initial concentration in the 235U-poor areas which is nonetheless high when compared with the initial Pu concentrations in the Pu-poor areas in the MOX fuel. Consequently, there are more fission reactions there in the heterogeneous UO2 fuel than in the MOX fuel.This fission and/or fission spike effect has in fact little impact on the overall fuel behaviour, be it homogeneous or heterogeneous, but it has to be taken into account in the separate-effect experiments where unirradiated UO2 is submitted to ion irradiation to simulate the irradiation effects [9,25-30]. The depletion of the actinide isotopes cannot be simulated in these experiments. The IFA-702 re-irradiation, with the high power during the last period of the irradiation most certainly having played a role. The other major difference between this fuel was irradiated under BWR conditions, whereas those used in [2] were all PWR fuels. The images of the IFA-702 heterogeneous UO2 fuel on the periphery show that an internal zirconia layer was formed during the irradiation, which is a sign of gap closure under hot conditions, though a thin gap was still measured at room temperature. Therefore, the stress field in the pellet of this fuel must have been significantly different from that of the fuel used in [2]. The resulting release is all the more interesting since the release path is more or less revealed by the Cs deposits. This Cs is released from the hot central part of the pellet and is not only in the fuel-cladding gap and along the obvious radial cracks, but also in: All the grain boundaries around those radial cracks. The HBS 235U-rich agglomerates around those radial cracks. Like for Xe, the general trend for Cs was a release from the 235U peripheral agglomerates. The higher Cs measurement in the 235U-rich agglomerates close to the radial cracks results from both this release and the deposition of the Cs released from the hot central part.This singular release of Xe from the HBS bubbles of the 235U-rich agglomerates on the fuel periphery is all the more surprising that the Pu-rich agglomerates of the MIMAS MOX fuel irradiated under the same conditions [15] retained their fission gases in these areas. We found no definitive reason for that difference. the fission product implantation level has an effect. the local Pu content has also an effect. the actual local burn-up has an effect. This effect may be linked to fission through the local depletion of the fissile isotopes which changes the local chemical composition, as well as to the higher energy deposited there by electronic interactions at the beginning of the fission fragment recoils when compared with implanted areas with a low actual burn-up. Moreover, the major release of fission gases from the peripheral 235U-rich agglomerate HBS bubbles was evidenced in this heterogeneous UO2 fuel.The radial movement of Cs from the central part of the pellet towards its periphery was shown. This involved a deposition at the grain boundaries, including the HBS ones, around the radial cracks in the periphery. This showed the intergranular paths existing for the release of fission gases and Cs all through the fuel periphery. Grain Equivalent Circular Diameter (ECD) for which half of the surface is made of smaller grains and half of larger grains

The Fathers Day Eruption of Kilauea, Volcano, Hawaii: a gas Emissions Perspective

NASA Astrophysics Data System (ADS)

Sutton, A.; Elias, T.

2007-12-01

Gas release events from Kilauea's summit magma reservoir and East Rift Zone (ERZ) before and during the June 17, 2007 Fathers Day eruptive sequence provide evidence of correlated summit and rift processes and illustrate how perturbations in magma supply from depth can disrupt steady processes at the surface. Changes in summit CO2 emission rates are thought to reflect changes in deep magma supply and the movement of magma into the rift zone. During the several years preceding the Fathers Day activity, Kilauea had undergone a surge of magma supply and effusive output, as evidenced by gas release and cross-caldera extension. In 2004, the CO2 emission rate, which had been quasi-steady, below 10,000 tonnes/day for the preceeding eight years, began to increase. By mid-2004 the rate had doubled, and by 2005, had tripled, reaching nearly 30,000 t/d. The peak and subsequent decline in summit CO2 attended a similar pattern in east rift SO2 emissions, which are used at Kilauea as one proxy for effusion rate. The surge in magma supply and lava effusion rate may have unsettled Kilauea's plumbing enough to set the stage for the subsequent Fathers Day intrusive and eruptive activity. As magma was withdrawn from the summit reservoir on 17 June 2007, forming the dike that intruded the Upper East Rift Zone, overburden pressure in the reservoir decreased allowing dissolved gases to exsolve and escape from the melt. The more soluble SO2, would be more affected by this pressure change than CO2, which exsolves at much greater depth. Summit SO2 emissions increased nearly four-fold as the summit deflated and summit and Upper East Rift tremor spiked. Increased ambient gas concentrations downwind of Halema`uma`u Crater resulted from the sharp increase in SO2 emission rates and caused the national park to close Crater Rim Drive in this area for several days. The Fathers Day intrusion, subsequent collapses at Pu`u `O`o, and the brief eruption at Kane Nui O Hamo (KNH) profoundly changed ERZ gases as well. SO2 emissions declined dramatically from Pu`u `O`o, dropping below 100 t/d by early July and remained low for several weeks even after lava reappeared in Pu`u `O`o. This overall decline in east rift gas release is reasonably consistent with the observed eruptive events: the dike likely robbed the magma supply but produced only the scanty KNH eruption, and the thinness of the dike geometry proved a poor conduit for SO2 release from depth. The beginning of the 21 July fissure activity reflected a return of magma and significant gas release to the Pu`u `O`o area as pressure within the shallow vent system exceeded structural integrity of the edifice. Following a brief increase in SO2 emissions at the onset of fissure activity, values declined, while effusion remained high. The low level of SO2 release, which persisted for the first several weeks of this fissure activity possibly reflected displacement of old rift-stored magma with newer magma coming from the summit and passing beneath the Pu`u `O`o system. Beginning 12 August, Pu`u `O`o re-emerged as Kilauea's primary SO2 degassing source, even though all extrusion as of this writing is occurring from the fissure system east of the cone. Currently, Kilauea appears to be following a pattern similar to that of the 1986-1991 Kupaianaha era, wherein most SO2 release was from Pu`u `O`o while active extrusion occurred down rift.

Dynamical Aspects of Quasifission Process in Heavy-Ion Reactions

NASA Astrophysics Data System (ADS)

Knyazheva, G. N.; Itkis, I. M.; Kozulin, E. M.

2015-06-01

The study of mass-energy distributions of binary fragments obtained in the reactions of 36S, 48Ca, 58Fe and 64Ni ions with the 232Th, 238U, 244Pu and 248Cm at energies below and above the Coulomb barrier is presented. For all the reactions the main component of the distributions corresponds to asymmetrical mass division typical for asymmetric quasifission process. To describe the quasifission mass distribution the simple method has been proposed. This method is based on the driving potential of the system and time dependent mass drift. This procedure allows to estimate QF time scale from the measured mass distributions. It has been found that the QF time exponentially decreases when the reaction Coulomb factor Z1Z2 increases.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Drell, S.; Jeanloz, R.; Cornwall, J.

This study is a follow-on to the review made by JASON during its 1997 Summer Study of what is known about the aging of critical constituents, particularly the high explosives, metals (Pu, U), and polymers in the enduring stockpile. The JASON report (JSR-97-320) that summarized the findings was based on briefings by the three weapons labs (LANL, LLNL, SNL). They presented excellent technical analyses covering a broad range of scientific and engineering problems pertaining to determining signatures of aging. But the report also noted: `Missing, however, from the briefings and the written documents made available to us by the labsmore » and DOE, was evidence of an adequately sharp focus and high priorities on a number of essential near-term needs of maintaining weapons in the stockpile.« less

Studies of Plutonium-238 Production at the High Flux Isotope Reactor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lastres, Oscar; Chandler, David; Jarrell, Joshua J

The High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL) is a versatile 85 MW{sub th}, pressurized, light water-cooled and -moderated research reactor. The core consists of two fuel elements, an inner fuel element (IFE) and an outer fuel element (OFE), each constructed of involute fuel plates containing high-enriched-uranium (HEU) fuel ({approx}93 wt% {sup 235}U/U) in the form of U{sub 3}O{sub 8} in an Al matrix and encapsulated in Al-6061 clad. An over-moderated flux trap is located in the center of the core, a large beryllium reflector is located on the outside of the core, and two controlmore » elements (CE) are located between the fuel and the reflector. The flux trap and reflector house numerous experimental facilities which are used for isotope production, material irradiation, and cold/thermal neutron scattering. Over the past five decades, the US Department of Energy (DOE) and its agencies have been producing radioisotope power systems used by the National Aeronautics and Space Administration (NASA) for unmanned, long-term space exploration missions. Plutonium-238 is used to power Radioisotope Thermoelectric Generators (RTG) because it has a very long half-life (t{sub 1/2} {approx} 89 yr.) and it generates about 0.5 watts/gram when it decays via alpha emission. Due to the recent shortage and uncertainty of future production, the DOE has proposed a plan to the US Congress to produce {sup 238}Pu by irradiating {sup 237}Np as early as in fiscal year 2011. An annual production rate of 1.5 to 2.0 kg of {sup 238}Pu is expected to satisfy these needs and could be produced in existing national nuclear facilities like HFIR and the Advanced Test Reactor (ATR) at the Idaho National Laboratory (INL). Reactors at the Savannah River Site were used in the past for {sup 238}Pu production but were shut down after the last production in 1988. The nation's {sup 237}Np inventory is currently stored at INL. A plan for producing {sup 238}Pu at US research reactor facilities such as the High Flux Isotope Reactor at ORNL has been initiated by the US DOE and NASA for space exploration needs. Two Monte Carlo-based depletion codes, TRITON (ORNL) and VESTA (IRSN), were used to study the {sup 238}Pu production rates with varying target configurations in a typical HFIR fuel cycle. Preliminary studies have shown that approximately 11 grams and within 15 to 17 grams of {sup 238}Pu could be produced in the first irradiation cycle in one small and one large VXF facility, respectively, when irradiating fresh target arrays as those herein described. Important to note is that in this study we discovered that small differences in assumptions could affect the production rates of Pu-238 observed. The exact flux at a specific target location can have a significant impact upon production, so any differences in how the control elements are modeled as a function of exposure, will also cause differences in production rates. In fact, the surface plot of the large VXF target Pu-238 production shown in Figure 3 illustrates that the pins closest to the core can potentially have production rates as high as 3 times those of pins away from the core, thus implying that a cycle-to-cycle rotation of the targets may be well advised. A methodology for generating spatially-dependent, multi-group self-shielded cross sections and flux files with the KENO and CENTRM codes has been created so that standalone ORIGEN-S inputs can be quickly constructed to perform a variety of {sup 238}Pu production scenarios, i.e. combinations of the number of arrays loaded and the number of irradiation cycles. The studies herein shown with VESTA and TRITON/KENO will be used to benchmark the standalone ORIGEN.« less

The ongoing Puʻu ʻŌʻō eruption of Kīlauea Volcano, Hawaiʻi: 30 years of eruptive activity

USGS Publications Warehouse

Orr, Tim R.; Heliker, Christina; Patrick, Matthew R.

2013-01-01

The Puʻu ʻŌʻō eruption of Kīlauea Volcano is its longest rift-zone eruption in more than 500 years. Since the eruption began in 1983, lava flows have buried 48 square miles (125 square kilometers) of land and added about 500 acres (200 hectares) of new land to the Island of Hawaiʻi. The eruption not only challenges local communities, which must adapt to an ever-changing and sometimes-destructive environment, but has also drawn millions of visitors to Hawaiʻi Volcanoes National Park. U.S. Geological Survey (USGS) scientists closely monitor and evaluate hazards at Hawaiʻi’s volcanoes and also work with park rangers to help ensure safe lava viewing for visitors.

Hydrothermal Alteration of Glass from Underground Nuclear Tests: Formation and Transport of Pu-clay Colloids at the Nevada National Security Site

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zavarin, M.; Zhao, P.; Joseph, C.

2015-05-27

The testing of nuclear weapons at the Nevada National Security Site (NNSS), formerly the Nevada Test Site (NTS), has led to the deposition of substantial quantities of plutonium into the environment. Approximately 2.8 metric tons (3.1×10 4 TBq) of Pu were deposited in the NNSS subsurface as a result of underground nuclear testing. While 3H is the most abundant anthropogenic radionuclide deposited in the NNSS subsurface (4.7×10 6 TBq), plutonium is the most abundant from a molar standpoint. The only radioactive elements in greater molar abundance are the naturally occurring K, Th, and U isotopes. 239Pu and 240Pu represent themore » majority of alpha-emitting Pu isotopes. The extreme temperatures associated with underground nuclear tests and the refractory nature of Pu results in most of the Pu (98%) being sequestered in melted rock, referred to as nuclear melt glass (Iaea, 1998). As a result, Pu release to groundwater is controlled, in large part, by the leaching (or dissolution) of nuclear melt glass over time. The factors affecting glass dissolution rates have been studied extensively. The dissolution of Pu-containing borosilicate nuclear waste glasses at 90ºC has been shown to lead to the formation of dioctahedral smectite colloids. Colloid-facilitated transport of Pu at the NNSS has been observed. Recent groundwater samples collected from a number of contaminated wells have yielded a wide range of Pu concentrations from 0.00022 to 2.0 Bq/L. While Pu concentrations tend to fall below the Maximum Contaminant Level (MCL) established by the Environmental Protection Agency (EPA) for drinking water (0.56 Bq/L), we do not yet understand what factors limit the Pu concentration or its transport behavior. To quantify the upper limit of Pu concentrations produced as a result of melt glass dissolution and determine the nature of colloids and Pu associations, we performed a 3 year nuclear melt glass dissolution experiment across a range of temperatures (25-200 °C) that represent hydrothermal conditions representative of the underground nuclear test cavities (when groundwater has re-saturated the nuclear melt glass and glass dissolution occurs). Colloid loads and Pu concentrations were monitored along with the mineralogy of both the colloids and the secondary mineral phases. The intent was to establish an upper limit for Pu concentrations at the NNSS, provide context regarding the Pu concentrations observed at the NNSS to date and the Pu concentrations that may be observed in the future. The results provide a conceptual model for the risks posed by Pu migration at the NNSS.« less

Nuclear forensics of a non-traditional sample: Neptunium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Doyle, Jamie L.; Schwartz, Daniel; Tandon, Lav

Recent nuclear forensics cases have focused primarily on plutonium (Pu) and uranium (U) materials. By definition however, nuclear forensics can apply to any diverted nuclear material. This includes neptunium (Np), an internationally safeguarded material like Pu and U, that could offer a nuclear security concern if significant quantities were found outside of regulatory control. This case study couples scanning electron microscopy (SEM) with quantitative analysis using newly developed specialized software, to evaluate a non-traditional nuclear forensic sample of Np. Here, the results of the morphological analyses were compared with another Np sample of known pedigree, as well as other traditionalmore » actinide materials in order to determine potential processing and point-of-origin.« less

Nuclear forensics of a non-traditional sample: Neptunium

DOE PAGES

Doyle, Jamie L.; Schwartz, Daniel; Tandon, Lav

2016-05-16

Recent nuclear forensics cases have focused primarily on plutonium (Pu) and uranium (U) materials. By definition however, nuclear forensics can apply to any diverted nuclear material. This includes neptunium (Np), an internationally safeguarded material like Pu and U, that could offer a nuclear security concern if significant quantities were found outside of regulatory control. This case study couples scanning electron microscopy (SEM) with quantitative analysis using newly developed specialized software, to evaluate a non-traditional nuclear forensic sample of Np. Here, the results of the morphological analyses were compared with another Np sample of known pedigree, as well as other traditionalmore » actinide materials in order to determine potential processing and point-of-origin.« less

Hybrid systems for transuranic waste transmutation in nuclear power reactors: state of the art and future prospects

NASA Astrophysics Data System (ADS)

Yurov, D. V.; Prikhod'ko, V. V.

2014-11-01

The features of subcritical hybrid systems (HSs) are discussed in the context of burning up transuranic wastes from the U-Pu nuclear fuel cycle. The advantages of HSs over conventional atomic reactors are considered, and fuel cycle closure alternatives using HSs and fast neutron reactors are comparatively evaluated. The advantages and disadvantages of two HS types with neutron sources (NSs) of widely different natures -- nuclear spallation in a heavy target by protons and nuclear fusion in magnetically confined plasma -- are discussed in detail. The strengths and weaknesses of HSs are examined, and demand for them for closing the U-Pu nuclear fuel cycle is assessed.

Following electron impact excitations of Rn, Ra, Th, U and Pu single atom L sub-shells ionization cross section calculations by using Lotz’s equation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ayinol, M., E-mail: aydinolm@dicle.edu.tr; Aydeniz, D., E-mail: daydeniz@hotmail.com

L shell ionization cross section and L{sub i} subshells ionization cross sections of Rn, Ra, Th, U, Pu atoms calculated. For each of atoms, ten different electron impact energy values (E{sub o}) are used. Calculations carried out by using Lotz equation in Matlab. First, calculations done for non-relativistic case by using non-relativistic Lotz equation then repeated with relativistic Lotz equation. σ{sub L} total and σ{sub Li}(i = 1,2,3) subshells ionisation cross section values obtained for E{sub o} values in the energy range of E{sub Li}

Expedition Six Flight Engineer Donald R. Pettit is loading software on PC in U.S. Lab

NASA Image and Video Library

2002-12-06

ISS006-E-07133 (9 December 2002) --- Astronaut Donald R. Pettit, Expedition 6 NASA ISS science officer, works to set up Pulmonary Function in Flight (PuFF) hardware in preparation for a Human Research Facility (HRF) experiment in the Destiny laboratory on the International Space Station (ISS). Expedition 6 is the fourth and final expedition crew to perform the HRF/PuFF Experiment on the ISS.

Expedition Six Flight Engineer Donald R. Pettit is loading software on PC in U.S. Lab

NASA Image and Video Library

2002-12-06

ISS006-E-07134 (9 December 2002) --- Astronaut Donald R. Pettit, Expedition Six NASA ISS science officer, works to set up Pulmonary Function in Flight (PuFF) hardware in preparation for a Human Research Facility (HRF) experiment in the Destiny laboratory on the International Space Station (ISS). Expedition Six is the fourth and final expedition crew to perform the HRF/PuFF Experiment on the ISS.

Improvement of INVS Measurement Uncertainty for Pu and U-Pu Nitrate Solution

DOE Office of Scientific and Technical Information (OSTI.GOV)

Swinhoe, Martyn Thomas; Menlove, Howard Olsen; Marlow, Johnna Boulds

2017-04-27

In the Tokai Reprocessing Plant (TRP) and the Plutonium Conversion Development Facility (PCDF), a large amount of plutonium nitrate solution which is recovered from light water reactor (LWR) and advanced thermal reactor (ATR), FUGEN are being stored. Since the solution is designated as a direct use material, the periodical inventory verification and flow verification are being conducted by Japan Safeguard Government Office (JSGO) and International Atomic Agency (IAEA).

Oxidation and reduction behaviors of a prototypic MgO-PuO2-x inert matrix fuel

NASA Astrophysics Data System (ADS)

Miwa, Shuhei; Osaka, Masahiko

2017-04-01

Oxidation and reduction behaviors of prototypic MgO-based inert matrix fuels (IMFs) containing PuO2-x were experimentally investigated by means of thermogravimetry. The oxidation and reduction kinetics of the MgO-PuO2-x specimen were determined. The oxidation and reduction rates of the MgO-PuO2-x were found to be low compared with those of PuO2-x. It is note that the changes in O/Pu ratios of MgO-PuO2-x from stoichiometry were smaller than those of PuO2-x at high oxygen partial pressure.

A compact gas-filled avalanche counter for DANCE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, C. Y.; Chyzh, A.; Kwan, E.

2012-08-04

A compact gas-filled avalanche counter for the detection of fission fragments was developed for a highly segmented 4π γ-ray calorimeter, namely the Detector for Advanced Neutron Capture Experiments located at the Lujan Center of the Los Alamos Neutron Science Center. It has been used successfully for experiments with 235U, 238Pu, 239Pu, and 241Pu isotopes to provide a unique signature to differentiate the fission from the competing neutron-capture reaction channel. We also used it to study the spontaneous fission in 252Cf. The design and performance of this avalanche counter for targets with extreme α-decay rate up to ~2.4×108/s are described.

Zirconia ceramics for excess weapons plutonium waste

NASA Astrophysics Data System (ADS)

Gong, W. L.; Lutze, W.; Ewing, R. C.

2000-01-01

We synthesized a zirconia (ZrO 2)-based single-phase ceramic containing simulated excess weapons plutonium waste. ZrO 2 has large solubility for other metallic oxides. More than 20 binary systems A xO y-ZrO 2 have been reported in the literature, including PuO 2, rare-earth oxides, and oxides of metals contained in weapons plutonium wastes. We show that significant amounts of gadolinium (neutron absorber) and yttrium (additional stabilizer of the cubic modification) can be dissolved in ZrO 2, together with plutonium (simulated by Ce 4+, U 4+ or Th 4+) and impurities (e.g., Ca, Mg, Fe, Si). Sol-gel and powder methods were applied to make homogeneous, single-phase zirconia solid solutions. Pu waste impurities were completely dissolved in the solid solutions. In contrast to other phases, e.g., zirconolite and pyrochlore, zirconia is extremely radiation resistant and does not undergo amorphization. Baddeleyite (ZrO 2) is suggested as the natural analogue to study long-term radiation resistance and chemical durability of zirconia-based waste forms.

Neutronics Benchmarks for the Utilization of Mixed-Oxide Fuel: Joint U.S./Russian Progress Report for Fiscal Year 1997

DOE Office of Scientific and Technical Information (OSTI.GOV)

Akkurt, H

2001-01-11

In 1967, a series of critical experiments were conducted at the Westinghouse Reactor Evaluation Center (WREC) using mixed-oxide (MOX) PuO{sub 2}-UO{sub 2} and/or UO{sub 2} fuels in various lattices and configurations . These experiments were performed under the joint sponsorship of the Empire State Atomic Development Associates (ESADA) plutonium program and Westinghouse . The purpose of these experiments was to develop experimental data to validate analytical methods used in the design of a plutonium-bearing replacement fuel for water reactors. Three different fuels were used during the experimental program: two MOX fuels and a low-enriched UO{sub 2} fuel. The MOX fuelsmore » were distinguished by their {sup 240}Pu content: 8 wt% {sup 240}Pu and 24 wt% {sup 240}Pu. Both MOX fuels contained 2.0 wt % PuO{sub 2} in natural UO{sub 2} . The UO{sub 2} fuel with 2.72 wt % enrichment was used for comparison with the plutonium data and for use in multiregion experiments.« less

Experimental criticality specifications. An annotated bibliography through 1977

DOE Office of Scientific and Technical Information (OSTI.GOV)

Paxton, H.C.

1978-05-01

The compilation of approximately 300 references gives sources of experimental criticality parameters of systems containing /sup 235/U, /sup 233/U, and /sup 239/Pu. The intent is to cover basic data for criticality safety applications. The references are arranged by subject.

Promising Fuel Cycle Options for R&D – Results, Insights, and Future Directions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wigeland, Roald Arnold

2015-05-01

The Fuel Cycle Options (FCO) campaign in the U.S. DOE Fuel Cycle Research & Development Program conducted a detailed evaluation and screening of nuclear fuel cycles. The process for this study was described at the 2014 ICAPP meeting. This paper reports on detailed insights and questions from the results of the study. The comprehensive study identified continuous recycle in fast reactors as the most promising option, using either U/Pu or U/TRU recycle, and potentially in combination with thermal reactors, as reported at the ICAPP 2014 meeting. This paper describes the examination of the results in detail that indicated that theremore » was essentially no difference in benefit between U/Pu and U/TRU recycle, prompting questions about the desirability of pursuing the more complex U/TRU approach given that the estimated greater challenges for development and deployment. The results will be reported from the current effort that further explores what, if any, benefits of TRU recycle (minor actinides in addition to plutonium recycle) may be in order to inform decisions on future R&D directions. The study also identified continuous recycle using thorium-based fuel cycles as potentially promising, in either fast or thermal systems, but with lesser benefit. Detailed examination of these results indicated that the lesser benefit was confined to only a few of the evaluation metrics, identifying the conditions under which thorium-based fuel cycles would be promising to pursue. For the most promising fuel cycles, the FCO is also conducting analyses on the potential transition to such fuel cycles to identify the issues, challenges, and the timing for critical decisions that would need to be made to avoid unnecessary delay in deployment, including investigation of issues such as the effects of a temporary lack of plutonium fuel resources or supporting infrastructure. These studies are placed in the context of an overall analysis approach designed to provide comprehensive information to the decision-making process.« less

Novel composite membrane coated with a poly(diallyldimethylammonium chloride)/urushi semi-interpenetrating polymer network for non-aqueous redox flow battery application

NASA Astrophysics Data System (ADS)

Cho, Eunhae; Won, Jongok

2016-12-01

Novel composite membranes of a semi-interpenetrating network (semi-IPN) coated on the surfaces of a porous Celgard 2400 support are prepared and investigate for application in a non-aqueous redox flow battery (RFB). A natural polymer, urushi, is used for the matrix because of its high mechanical robustness, and poly(diallyldimethylammonium chloride) (PDDA) provides anionic exchange sites. The PDDA/urushi (P/U) semi-IPN film is prepared by the photo polymerization of urushiol in the presence of PDDA. The thin layer composed of the P/U semi-IPN on the porous support provides selectivity while maintaining the ion conductivity. The coulombic and energy efficiencies increase with increasing amounts of PDDA in the P/U semi-IPN layer, and the values reach 69.5% and 42.5%, respectively, for the one containing 40 wt% of PDDA. These values are substantially higher than those of the Neosepta AHA membrane and the Celgard membrane, indicating that the selective layer reduces the crossover of the redox active species through the membrane. This result implies that the formation of composite membranes using semi-IPN selective layers on the dimensionally stable porous membrane enable the successful use of a non-aqueous RFB for future energy storage systems.

Fusion-fission and quasifission of superheavy systems with Z =110 -116 formed in 48Ca-induced reactions

NASA Astrophysics Data System (ADS)

Kozulin, E. M.; Knyazheva, G. N.; Itkis, I. M.; Itkis, M. G.; Bogachev, A. A.; Chernysheva, E. V.; Krupa, L.; Hanappe, F.; Dorvaux, O.; Stuttgé, L.; Trzaska, W. H.; Schmitt, C.; Chubarian, G.

2014-11-01

Background: In heavy-ion-induced reactions the mechanism leading to the formation of the compound nucleus and the role of quasifission is still not clear. Purpose: Investigation of the quasifission process of superheavy composite systems with Z =110 -116 and comparison with properties of fusion-fission and quasifission of lighter composite systems. Method: Mass and energy distributions of fissionlike fragments formed in the reactions 48Ca+232Th, 238U , 244Pu , and 248Cm at energies near the Coulomb barrier have been measured using the double-arm time-of-flight spectrometer CORSET at the U-400 cyclotron of the FLNR JINR. Results: The most probable fragment masses as well as total kinetic energies and their dispersions in dependence on the interaction energies and ion-target combinations have been studied for asymmetric and symmetric fragments formed in the reactions. The capture cross sections were obtained for the reactions 48Ca+244Pu and 248Cm . The lower limits for fission barriers of 283 -286Cn , 289 -292Fl , and 293 -296Lv compound nuclei were estimated. Conclusions: Analysis of the properties of symmetric fragments has shown that a significant part of these fragments may be attributed to fusion-fission process for the reactions 48Ca +238U , 244Pu , and 248Cm .

Investigations of systems ThO 2-MO 2-P 2O 5 (M=U, Ce, Zr, Pu). Solid solutions of thorium-uranium (IV) and thorium-plutonium (IV) phosphate-diphosphates

NASA Astrophysics Data System (ADS)

Dacheux, N.; Podor, R.; Brandel, V.; Genet, M.

1998-02-01

In the framework of nuclear waste management aiming at the research of a storage matrix, the chemistry of thorium phosphates has been completely re-examined. In the ThO 2-P 2O 5 system a new compound thorium phosphate-diphosphate Th 4(PO 4) 4P 2O 7 has been synthesized. The replacement of Th 4+ by a smaller cation like U 4+ and Pu 4+ in the thorium phosphate-diphosphate (TPD) lattice has been achieved. Th 4- xU x(PO 4) 4P 2O 7 and Th 4- xPu x(PO 4) 4P 2O 7 solid solutions have been synthesized through wet and dry processes with 0< x<3.0 for uranium and 0< x<1.0 for plutonium. From the variation of the unit cell parameters, an upper x value equal to 1.67 has been estimated for the thorium-plutonium (IV) phosphate-diphosphate solid solutions. Two other tetravalent cations, Ce 4+ and Zr 4+, cannot be incorporated in the TPD lattice: cerium (IV) because of its reduction into Ce (III) at high temperature, and zirconium probably because of its too small radius compared to thorium.

Fission Product Yield Study of 235U, 238U and 239Pu Using Dual-Fission Ionization Chambers

NASA Astrophysics Data System (ADS)

Bhatia, C.; Fallin, B.; Howell, C.; Tornow, W.; Gooden, M.; Kelley, J.; Arnold, C.; Bond, E.; Bredeweg, T.; Fowler, M.; Moody, W.; Rundberg, R.; Rusev, G.; Vieira, D.; Wilhelmy, J.; Becker, J.; Macri, R.; Ryan, C.; Sheets, S.; Stoyer, M.; Tonchev, A.

2014-05-01

To resolve long-standing differences between LANL and LLNL regarding the correct fission basis for analysis of nuclear test data [M.B. Chadwick et al., Nucl. Data Sheets 111, 2891 (2010); H. Selby et al., Nucl. Data Sheets 111, 2891 (2010)], a collaboration between TUNL/LANL/LLNL has been established to perform high-precision measurements of neutron induced fission product yields. The main goal is to make a definitive statement about the energy dependence of the fission yields to an accuracy better than 2-3% between 1 and 15 MeV, where experimental data are very scarce. At TUNL, we have completed the design, fabrication and testing of three dual-fission chambers dedicated to 235U, 238U, and 239Pu. The dual-fission chambers were used to make measurements of the fission product activity relative to the total fission rate, as well as for high-precision absolute fission yield measurements. The activation method was employed, utilizing the mono-energetic neutron beams available at TUNL. Neutrons of 4.6, 9.0, and 14.5 MeV were produced via the 2H(d,n)3He reaction, and for neutrons at 14.8 MeV, the 3H(d,n)4He reaction was used. After activation, the induced γ-ray activity of the fission products was measured for two months using high-resolution HPGe detectors in a low-background environment. Results for the yield of seven fission fragments of 235U, 238U, and 239Pu and a comparison to available data at other energies are reported. For the first time results are available for neutron energies between 2 and 14 MeV.

Experimental Investigations into U/TRU Recovery using a Liquid Cadmium Cathode and Salt Containing High Rare Earth Concentrations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shelly X. Li; Steven D. Herrmann; Michael F. Simpson

2009-09-01

Experimental Investigations into U/TRU Recovery using a Liquid Cadmium Cathode and Salt Containing High Rare Earth Concentrations Shelly X. Li, Steven D. Herrmann, and Michael F. Simpson Pyroprocessing Technology Department Idaho National Laboratory P.O. Box 1625, Idaho Falls, ID 83415 USA Abstract - A series of six bench-scale liquid cadmium cathode (LCC) tests was performed to obtain basic separation data with focus on the behavior of rare earth elements. The electrolyte used for the tests was a mixed salt from the Mk-IV and Mk-V electrorefiners, in which spent metal fuels from Experimental Breeder Reactor-II (EBR-II) had been processed. Rare earthmore » (RE) chlorides, such as NdCl3, CeCl3, LaCl3, PrCl3, SmCl3, and YCl3, were spiked into the salt prior to the first test to create an extreme case for investigating rare earth contamination of the actinides collected by a LCC. For the first two LCC tests, an alloy with the nominal composition of 41U-30Pu-5Am-3Np-20Zr-1RE was loaded into the anode baskets as the feed material. The anode feed material for Runs 3 to 6 was spent ternary fuel (U-19Pu-10Zr). The Pu/U ratio in the salt varied from 0.6 to 1.3. Chemical and radiochemical analytical results confirmed that U and transuranics can be collected into the LCC as a group under the given run conditions. The RE contamination level in the LCC product was up to 6.7 wt% of the total metal collected. The detailed data for partitioning of actinides and REs in the salt and Cd phases are reported in the paper.« less

Concentrations of selected radionuclides and their spatial distribution in marine sediments from the northwestern Gulf, Kuwait.

PubMed

Uddin, Saif; Behbehani, Montaha

2018-02-01

This study focuses on creating a baseline for 40 K, 210 Pb, 137 Cs, 90 Sr, 226 Ra, 228 Ra, 238 U, 235 U, 234 U, 239+240 Pu and 238 Pu in marine sediments in the northwestern Gulf. The respective measured concentration ranges were 386-489, 32.3-48.8, 1.5-2.9, 4.53-5.42, 18.3-23.1, 18.8-23.0, 22.3-30.5, 0.99-1.33, 25.6-34.8, 0.30-0.93, and 0.0008-0.00018Bqkg -1 . The levels of these radionuclides are generally comparable to values reported for other marine waters in the northern hemisphere. The 137 Cs activity in the Gulf sediments offshore Kuwait is an order of magnitude lower compared to sediments from northeastern Iran. Other than that finding, no hot spots were observed in sediments adjacent to power and desalination plants, oil and gas industrial activities or wastewater treatment facilities. These data will serve as a baseline to gauge possible future inputs of radionuclides in the northern Gulf. The calculated average ratio of 235 U/ 238 U activity in the area is in agreement with the reported figure of the natural uranium ratio, suggesting the absence of depleted uranium (DU) at all the stations. The low concentration of 239+240 Pu suggests that there is no significant source of plutonium except that from atmospheric fallout from weapon testing and possible dry deposition via long-range dust transport. Copyright © 2017 Elsevier Ltd. All rights reserved.

Static headspace analysis using polyurethane phases--application to roasted coffee volatiles characterization.

PubMed

Rodrigues, C; Portugal, F C M; Nogueira, J M F

2012-01-30

Static headspace sorptive extraction using polyurethane foams (HSSE(PU)) followed by gas chromatography coupled to mass spectrometry is proposed for volatile analysis. The application of this novel analytical approach to characterize the volatiles profile from roasted coffee samples, selected as model system, revealed remarkable advantages under convenient experimental conditions. The comparison of HSSE(PU) with other well-established procedures, such as headspace sorptive extraction using polydimethylsiloxane (HSSE(PDMS)) and headspace solid phase microextraction using carboxen/polydimethylsiloxane fibers (HS-SPME(CAR/PDMS)), showed that the former presented much higher capacity, sensitivity and even selectivity, where larger abundance and number of roasted coffee volatile compounds (e.g. furans, pyrazines, ketones, acids and pyrroles) could be achieved, under similar experimental conditions. The data presented herein proved, for the first time, that PU foams present great performance for static headspace sorption-based procedures, showing to be an alternative polymeric phase for volatile analysis. Copyright © 2011 Elsevier B.V. All rights reserved.

Reductive Dissolution of PuO2(am): The Effect of Fe(II) and Hydroquinone

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rai, Dhanpat; Gorby, Yuri A.; Fredrickson, Jim K.

2002-06-01

SYNOPIS-Reducing agents commonly present in geologic environments can increase solubility of PuO2(am), which is otherwise very insoluble, by many orders of magnitude through reduction of Pu(IV) to Pu(III). The reduction reactions involving Fe(II) and hydroquinone, hitherto unquantified under environmental pH values, were found to be relatively fast and controlled the extent of PuO2(am) dissolution: a decrease in redox potential (pe + pH) resulted in concomitant increase in PuO2(am) solubility.

Radiochemical determination of 237NP in soil samples contaminated with weapon grade plutonium

NASA Astrophysics Data System (ADS)

Antón, M. P.; Espinosa, A.; Aragón, A.

2006-01-01

The Palomares terrestrial ecosystem (Spain) constitutes a natural laboratory to study transuranics. This scenario is partially contaminated with weapon-grade plutonium since the burnout and fragmentation of two thermonuclear bombs accidentally dropped in 1966. While performing radiometric measurements in the field, the possible presence of 237Np was observed through its 29 keV gamma emission. To accomplish a detailed characterization of the source term in the contaminated area using the isotopic ratios Pu-Am-Np, the radiochemical isolation and quantification by alpha spectrometry of 237Np was initiated. The selected radiochemical procedure involves separation of Np from Am, U and Pu with ionic resins, given that in soil samples from Palomares 239+240Pu levels are several orders of magnitude higher than 237Np. Then neptunium is isolated using TEVA organic resins. After electrodeposition, quantification is performed by alpha spectrometry. Different tests were done with blank solutions spiked with 236Pu and 237Np, solutions resulting from the total dissolution of radioactive particles and soil samples. Results indicate that the optimal sequential radionuclide separation order is Pu-Np, with decontamination percentages obtained with the ionic resins ranging from 98% to 100%. Also, the addition of NaNO2 has proved to be necessary, acting as a stabilizer of Pu-Np valences.

Energy dependence of the prompt γ -ray emission from the ( d , p ) -induced fission of U * 234 and Pu * 240

DOE PAGES

Rose, Sunniva J.; Zeiser, Fabio; Wilson, J. N.; ...

2017-07-05

Prompt-fission γ rays are responsible for approximately 5% of the total energy released in fission, and therefore important to understand when modeling nuclear reactors. In this work we present prompt γ-ray emission characteristics in fission as a function of the nuclear excitation energy of the fissioning system. Emitted γ-ray spectra were measured, and γ-ray multiplicities and average and total γ energies per fission were determined for the 233U(d,pf) reaction for excitation energies between 4.8 and 10 MeV, and for the 239Pu(d,pf) reaction between 4.5 and 9 MeV. The spectral characteristics show no significant change as a function of excitation energymore » above the fission barrier, despite the fact that an extra ~5 MeV of energy is potentially available in the excited fragments for γ decay. The measured results are compared with model calculations made for prompt γ-ray emission with the fission model code gef. In conclusion, further comparison with previously obtained results from thermal neutron induced fission is made to characterize possible differences arising from using the surrogate (d,p) reaction.« less

The Pu`u `O`o-Kupaianaha Eruption of Kilauea Volcano: The First 20 Years

NASA Astrophysics Data System (ADS)

Heliker, C.

2002-12-01

The Pu`u `O`o-Kupaianaha eruption on Kilauea's east rift zone, which began January 3, 1983, is the volcano's longest rift-zone eruption during at least the past 600 years. The early years of the eruption were memorable for lava fountains as high as 460 m that erupted episodically from the Pu`u `O`o vent. From June 1983 through June 1986, 44 episodes of fountaining fed channeled `a`a flows and built a cinder-and-spatter cone 255-m high. For the past 16 years, however, the activity has been dominated by nearly continuous effusion, low eruption rates, and emplacement of tube-fed pahoehoe flows. The change in eruptive style began in July 1986, when the activity shifted 3 km downrift to a new vent, Kupaianaha, where overflows from a lava pond built a broad, low shield, 1 km in diameter and 56 m high. For much of the next 5.5 years, tubes delivered lava to the ocean, 12 km away. In February 1992, the Kupaianaha vent died, and the eruption returned to Pu`u `O`o, where a series of flank vents on the southwest side of the cone has erupted nearly continuously for 11 years, again producing a shield and tube-fed pahoehoe flows to the coast. Since late 1986, lava has entered the ocean over 70 percent of the time. More than 210 hectares of new land have formed during this eruption, as lava deltas build seaward over steep, prograding submarine slopes of hyaloclastic debris and pillow lava. The estimated long-term effusion rate of this eruption, averaged over its first 19 years, is approximately 0.12 km3 per year (dense-rock equivalent). The total volume of lava produced, 2.1 km3, accounts for over half the volume erupted by Kilauea in the last 160 years. The composite flow field covers 105 km2 of the volcano's south flank and spans 14.5 km at the coastline, forming a lava plain 10-35 m thick. The Pu`u `O`o-Kupaianaha eruption also ranks as Hawaii's most destructive of the past two centuries. Lava flows repeatedly invaded communities on Kilauea's southern coast, destroying 186 houses and prompting a federal disaster declaration in 1990. As the eruption approaches its 20th anniversary, the State of Hawaii has shown renewed interest in seeking a politically and fiscally acceptable means to restrict development in areas with a high hazard of lava-flow inundation.

Fission fragment yield distribution in the heavy-mass region from the 239Pu (nth,f ) reaction

NASA Astrophysics Data System (ADS)

Gupta, Y. K.; Biswas, D. C.; Serot, O.; Bernard, D.; Litaize, O.; Julien-Laferrière, S.; Chebboubi, A.; Kessedjian, G.; Sage, C.; Blanc, A.; Faust, H.; Köster, U.; Ebran, A.; Mathieu, L.; Letourneau, A.; Materna, T.; Panebianco, S.

2017-07-01

The fission fragment yield distribution has been measured in the 239Pu(nth,f ) reaction in the mass region of A =126 to 150 using the Lohengrin recoil-mass spectrometer. Three independent experimental campaigns were performed, allowing a significant reduction of the uncertainties compared to evaluated nuclear data libraries. The long-standing discrepancy of around 10% for the relative yield of A =134 reported in JEF-2.2 and JEFF-3.1.1 data libraries is finally solved. Moreover, the measured mass distribution in thermal neutron-induced fission does not show any significant dip around the shell closure (A =136 ) as seen in heavy-ion fission data of 208Pb(18O, f ) and 238U(18O, f ) reactions. Lastly, comparisons between our experimental data and the predictions from Monte Carlo codes (gef and fifrelin) are presented and discussed.

Evidence for live 247Cm in the early solar system

USGS Publications Warehouse

Tatsumoto, M.; Shimamura, T.

1980-01-01

Variations of the 238U/235U ratio in the Allende meteorite, ranging from -35% to + 19%, are interpreted as evidence of live 247Cm in the early Solar System. The amounts of these and other r-products in the Solar System indicate values of (9,000??3,000) Myr for the age of the Galaxy and ??? 8 Myr for the time between the end of nucleosynthesis and the formation of meteoritic grains. Three possible explanations are presented for the different values of the latter time period which are indicated by the decay products of 247Cm, 26Al, 244Pu and 129I. ?? 1980 Nature Publishing Group.

The Xenon record of Earth's early differentiaiton

NASA Astrophysics Data System (ADS)

Peto, M. K.; Mukhopadhyay, S.; Kelley, K. A.

2011-12-01

Xenon isotopes in mantle derived rocks provide information on the early differentiation of the silicate mantle of our planet. {131,132 134,136}Xe isotopes are produced by the spontaneous fission of two different elements: the now extinct radionuclide 244Pu, and the long-lived 238U. These two parent nuclides, however, yield rather different proportion of fissiogenic Xenon isotopes. Hence, the proportion of Pu- to U-derived fission xenon is indicative of the degree and rate of outgassing of a mantle reservoir. Recent data obtained from Iceland in our lab confirm that the Xenon isotopic composition of the plume source(s) is characterized by lower 136Xe/130Xe ratios than the MORB source and the Iceland plume is more enriched in the Pu-derived Xenon component. These features are interpreted as reflecting different degrees of outgassing and appear not to be the result of preferential recycling of Xenon to the deep mantle. To further investigate how representative the Icelandic measurements might be of other mantle plumes, we measured noble gases (He, Ne, Ar, Xe) in gas-rich basalt glasses from the Rochambeau Ridge (RR) in the Northern Lau Basin. Recent work suggests the presence of a "Samoan-like" OIB source in the northern Lau Basin and our measurements were performed on samples with plume-like 3He/4He ratios (15-28 RA) [1]. The Xenon isotopic measurements indicate that the maximum measured 136Xe/130Xe ratios in the Rochambeau samples are similar to Iceland. In particular, for one of the gas rich samples we were able to obtain 77 different isotopic measurements through step-crushing. Preliminary investigation of this sample suggests higher Pu- to U-derived fission Xenon than in MORBs. To quantitatively evaluate the degree and rate of outgassing of the plume and MORB reservoirs, particularly during the first few hundred million years of Earth's history, we have modified a geochemical reservoir model that was previously developed to investigate mantle overturn and mixing from He, Ar and lithophile isotopes [2]. We will present the results from this geochemical reservoirs model, which is constrained by our high precision dataset from the Rochambeau Rift (Northern Lau Basin) and Iceland along with the Xenon dataset from popping rock [3]. [1] Lupton et al., GRL, 2009. [2] Gonnermann and Mukhopadhyay, Nature, 2009. [3] Kunz et al., Science, 1998.

The thermal conductivity of mixed fuel U xPu 1-xO 2: molecular dynamics simulations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Xiang-Yang; Cooper, Michael William Donald; Stanek, Christopher Richard

2015-10-16

Mixed oxides (MOX), in the context of nuclear fuels, are a mixture of the oxides of heavy actinide elements such as uranium, plutonium and thorium. The interest in the UO 2-PuO 2 system arises from the fact that these oxides are used both in fast breeder reactors (FBRs) as well as in pressurized water reactors (PWRs). The thermal conductivity of UO 2 fuel is an important material property that affects fuel performance since it is the key parameter determining the temperature distribution in the fuel, thus governing, e.g., dimensional changes due to thermal expansion, fission gas release rates, etc. Formore » this reason it is important to understand the thermal conductivity of MOX fuel and how it differs from UO 2. Here, molecular dynamics (MD) simulations are carried out to determine quantitatively, the effect of mixing on the thermal conductivity of U xPu 1-xO 2, as a function of PuO 2 concentrations, for a range of temperatures, 300 – 1500 K. The results will be used to develop enhanced continuum thermal conductivity models for MARMOT and BISON by INL. These models express the thermal conductivity as a function of microstructure state-variables, thus enabling thermal conductivity models with closer connection to the physical state of the fuel.« less

The time scale of quasifission process in reactions with heavy ions

NASA Astrophysics Data System (ADS)

Knyazheva, G. N.; Itkis, I. M.; Kozulin, E. M.

2014-05-01

The study of mass-energy distributions of binary fragments obtained in the reactions of 36S, 48Ca, 58Fe and 64Ni ions with the 232Th, 238U, 244Pu and 248Cm at energies below and above the Coulomb barrier is presented. These data have been measured by two time-of-flight CORSET spectrometer. The mass resolution of the spectrometer for these measurements was about 3u. It allows to investigate the features of mass distributions with good accuracy. The properties of mass and TKE of QF fragments in dependence on interaction energy have been investigated and compared with characteristics of the fusion-fission process. To describe the quasifission mass distribution the simple method has been proposed. This method is based on the driving potential of the system and time dependent mass drift. This procedure allows to estimate QF time scale from the measured mass distributions. It has been found that the QF time exponentially decreases when the reaction Coulomb factor Z1Z2 increases.

Static electric dipole polarizabilities of An(5+/6+) and AnO2 (+/2+) (An = U, Np, and Pu) ions.

PubMed

Parmar, Payal; Peterson, Kirk A; Clark, Aurora E

2014-12-21

The parallel components of static electric dipole polarizabilities have been calculated for the lowest lying spin-orbit states of the penta- and hexavalent oxidation states of the actinides (An) U, Np, and Pu, in both their atomic and molecular diyl ion forms (An(5+/6+) and AnO2 (+/2+)) using the numerical finite-field technique within a four-component relativistic framework. The four-component Dirac-Hartree-Fock method formed the reference for MP2 and CCSD(T) calculations, while multireference Fock space coupled-cluster (FSCC), intermediate Hamiltonian Fock space coupled-cluster (IH-FSCC) and Kramers restricted configuration interaction (KRCI) methods were used to incorporate additional electron correlation. It is observed that electron correlation has significant (∼5 a.u.(3)) impact upon the parallel component of the polarizabilities of the diyls. To the best of our knowledge, these quantities have not been previously reported and they can serve as reference values in the determination of various electronic and response properties (for example intermolecular forces, optical properties, etc.) relevant to the nuclear fuel cycle and material science applications. The highest quality numbers for the parallel components (αzz) of the polarizability for the lowest Ω levels corresponding to the ground electronic states are (in a.u.(3)) 44.15 and 41.17 for UO2 (+) and UO2 (2+), respectively, 45.64 and 41.42 for NpO2 (+) and NpO2 (2+), respectively, and 47.15 for the PuO2 (+) ion.

Radiation Chemistry of Acetohydroxamic Acid in the UREX Process

DOE Office of Scientific and Technical Information (OSTI.GOV)

Karraker, D.G.

2002-07-31

The UREX process is being developed to process irradiated power reactor elements by dissolution in nitric acid and solvent extraction by a variation of the PUREX process.1 Rather than recovering both U and Pu, as in Purex, only U will be recovered by solvent extraction, hence the name ''UREX.'' A complexing agent, acetohydroxamic acid (AHA), will be added to the scrub stream to prevent the extraction of Pu(IV) and Np(VI). AHA (CH3C=ONHOH) is decomposed to gaseous products in waste evaporation, so no solid waste is generated by its addition. AHA is hydrolyzed in acid solution to acetic acid and hydroxylaminemore » at a rate dependent on the acid concentration.2-4 The fuel to be processed is ca 40 years cooled, 30,000-50,000 MWD/MT material; although only a few fission products remain, the Pu isotopes and 241Am generate a radiation field estimated to be 2.6E+02R during processing. (see Appendix for calculation.) This study was conducted to determine the effect of this level of radiation on the stability of AHA during processing.« less

He, Xe and Ne isotopes in a steady-state mass transport model and implications about terrestrial volatiles

NASA Technical Reports Server (NTRS)

Wasserburg, G. J.; Porcelli, D.

1994-01-01

We present a model of the steady-state transport assuming three reservoirs: a lower mantle (P) with a relatively undepleted inventory of U, Th, Pu, I, He, Ne, Xe, Ar; an upper mantle that has been extensively outgassed (D); and the atmosphere. There is mass transport at a rate M(sub PD) by plumes from the lower mantle, a fraction of which is outgassed directly into the atmosphere, while the remainder feeds matter and associated nuclei into D. D is well outgassed at spreading centers and has material containing atmospheric gases added to it by subduction. In the case of He, there is no subduction component. The approach follows the treatment of Kellogg and Wasserburg. A summary of the pertinent equations and constraints was reported earlier. The U, Th and Pu in P are estimated for Earth models from refractory element abundances in meteorites. In this model the inventory of rare gases in D is governed by the simple mixing of components from P (both radiogenic and original) with distinctive atmospheric components. In addition, alpha decay and spontaneous fission of U, and (alpha, n) reaction on oxygen from energetic alpha particles produce radiogenic/nuclear daughter products in D. These include (4)He, (136)Xe and (21)Ne. (40)K in D generates excess radiogenic (40)Ar.

The incorporation of plutonium in lanthanum zirconate pyrochlore

NASA Astrophysics Data System (ADS)

Gregg, Daniel J.; Zhang, Yingjie; Middleburgh, Simon C.; Conradson, Steven D.; Triani, Gerry; Lumpkin, Gregory R.; Vance, Eric R.

2013-11-01

The incorporation of plutonium (Pu) within lanthanum zirconate pyrochlore was investigated using air, argon, and N2-3.5%H2 sintering atmospheres together with Ca2+ and Sr2+ incorporation for charge compensation. The samples have been characterised in the first instance by X-ray diffraction (XRD), scanning electron microscopy (SEM) and diffuse reflectance spectroscopy (DRS). The results show Pu can be exchanged for La3+ on the A-site with and without charge compensation and for Zr4+ on the B-site. DRS measurements were made over the wavenumber range of 4000-19,000 cm-1 and the Pu in all air- and argon-sintered samples was found to be present as Pu4+ while that in samples sintered in N2-3.5%H2 was present as Pu3+. The Pu valence was confirmed for three of the samples using X-ray near-edge absorption spectroscopy (XANES). Pu valences >4+ were not observed in any of the samples.

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

PubMed

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

2017-10-01

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

Image processing applications: From particle physics to society

NASA Astrophysics Data System (ADS)

Sotiropoulou, C.-L.; Luciano, P.; Gkaitatzis, S.; Citraro, S.; Giannetti, P.; Dell'Orso, M.

2017-01-01

We present an embedded system for extremely efficient real-time pattern recognition execution, enabling technological advancements with both scientific and social impact. It is a compact, fast, low consumption processing unit (PU) based on a combination of Field Programmable Gate Arrays (FPGAs) and the full custom associative memory chip. The PU has been developed for real time tracking in particle physics experiments, but delivers flexible features for potential application in a wide range of fields. It has been proposed to be used in accelerated pattern matching execution for Magnetic Resonance Fingerprinting (biomedical applications), in real time detection of space debris trails in astronomical images (space applications) and in brain emulation for image processing (cognitive image processing). We illustrate the potentiality of the PU for the new applications.

Development of Core Data Set of the Officer Longitudinal Research Data Base

DTIC Science & Technology

1987-07-01

FR EQ U EN CI ES FR OM TH E OM F. J DA TA OM FF RE Q; IN FI LE...OC FR EQ ; n ~ > t-3 ctJ ~ 10 q ts:l z n t< n 0 q z t-3 (/) 0 I’Jj ~ t-3 > ts:l t’i ts:l ~ ts:l z t-3 (/) 0 1󈧏 )I ’t1 ’U tz j z 0 H X 0... FR EQ U EN CI ES FR OM TH E SO M F. I DA TA SO M FF RE Q; IN FI LE IN ; IN PU T SS N IB 4. TY R $C H A R2

Structural, electronic, and thermodynamic properties of curium dioxide: Density functional theory calculations

NASA Astrophysics Data System (ADS)

Hou, Ling; Li, Wei-Dong; Wang, Fangwei; Eriksson, Olle; Wang, Bao-Tian

2017-12-01

We present a systematic investigation of the structural, magnetic, electronic, mechanical, and thermodynamic properties of CmO2 with the local density approximation (LDA)+U and the generalized gradient approximation (GGA)+U approaches. The strong Coulomb repulsion and the spin-orbit coupling (SOC) effects on the lattice structures, electronic density of states, and band gaps are carefully studied, and compared with other A O2 (A =U , Np, Pu, and Am). The ferromagnetic configuration with half-metallic character is predicted to be energetically stable while a charge-transfer semiconductor is predicted for the antiferromagnetic configuration. The elastic constants and phonon spectra show that the fluorite structure is mechanically and dynamically stable. Based on the first-principles phonon density of states, the lattice vibrational energy is calculated using the quasiharmonic approximation. Then, the Gibbs free energy, thermal expansion coefficient, specific heat, and entropy are obtained and compared with experimental data. The mode Grüneisen parameters are presented to analyze the anharmonic properties. The Slack relation is applied to obtain the lattice thermal conductivity in temperature range of 300-1600 K. The phonon group velocities are also calculated to investigate the heat transfer. For all these properties, if available, we compare the results of CmO2 with other A O2 .

Degradation of polyurethane by bacterium isolated from soil and assessment of polyurethanolytic activity of a Pseudomonas putida strain.

PubMed

Peng, Yu-Huei; Shih, Yang-hsin; Lai, Yen-Chun; Liu, Yuan-Zan; Liu, Ying-Tong; Lin, Nai-Chun

2014-01-01

The increasing usage and the persistence of polyester polyurethane (PU) generate significant sources of environmental pollution. The effective and environmental friendly bioremediation techniques for this refractory waste are in high demand. In this study, three novel PU degrading bacteria were isolated from farm soils and activated sludge. Based upon 16S ribosomal RNA gene sequence blast, their identities were determined. Particularly robust activity was observed in Pseudomonas putida; it spent 4 days to degrade 92% of Impranil DLN(TM) for supporting its growth. The optimum temperature and pH for DLN removal by P. putida were 25 °C and 8.4, respectively. The degradation and transformation of DLN investigated by Fourier transformed infrared spectroscopy show the decrease in ester functional group and the emergence of amide group. The polyurethanolytic activities were both presented in the extracellular fraction and in the cytosol. Esterase activity was detected in the cell lysate. A 45-kDa protein bearing polyurethanolytic activity was also detected in the extracellular medium. This study presented high PU degrading activity of P. putida and demonstrated its responsible enzymes during the PU degradation process, which could be applied in the bioremediation and management of plastic wastes.

Th/U/Pu/Cm dating of galactic cosmic rays with the extremely heavy cosmic ray composition observer

NASA Astrophysics Data System (ADS)

Westphal, Andrew J.; Weaver, Benjamin A.; Tarlé, Gregory

The principal goal of ECCO, the Extremely-heavy Cosmic-ray Composition Observer, is the measurement of the age of heavy galactic cosmic-ray nuclei using the extremely rare actinides (Th, U, Pu, Cm) as clocks. ECCO is one of two cosmic-ray instruments comprising the Heavy Nuclei Explorer (HNX), which was recently selected as one of several missions for Phase A study under NASA's Small class Explorer (SMEX) program. ECCO is based on the flight heritage of Trek, an array of barium-phosphate glass tracketch detectors deployed on the Russian space station Mir from 1991-1995. Using Trek, we measured the abundances of elements with Z > 70 in the galactic cosmic rays (GCRs). Trek consisted of a 1 m 2 array of stacks of individually polished thin BP-1 glass detectors. ECCO will be a much larger instrument, but will achieve both excellent resolution and low cost through use of a novel detector configuration. Here we report the results of recent accelerator tests of the ECCO detectors that verify detector performance. We also show the expected charge and energy resolution of ECCO as a function of energy.

Finite element analysis on deformation of stretchable electronic interconnect substrate using polydimethylsiloxanes (PDMS)

NASA Astrophysics Data System (ADS)

Roslan, M. F.; Shaffiar, N. M.; Khairusshima, M. K. N.; Sharifah, I. S. S.

2018-01-01

Over the years, the technology of electronic industry has growth tremendously. Open ended research on how to make a better concept of electronic circuit is ongoing especially on the stretchable electronic devices. There are many designs to achieve stretchability in electronic circuits. The problem occurs when deformation applied to the stretchable electronic circuit, it cannot maintain its functionality. Fracture may happen on the conductor. In this research, the study on deformation of stretchable electronic interconnects substrate using Polydimethlysiloxanes is carried out. The purpose of this research are to study the axial deformation occur, to determine the optimum shape of the conductor designs (horseshoe, rectangular and u-shape design) for the stretchable electronic interconnect and to compare the mechanical properties of Polydimethlysiloxanes (PDMS) with Polyurethane (PU) using Finite Element Analysis (FEA). The simulation was done on the FE model of the stretchable circuit with dimension of 2.4 X 2.4 X 0.5 mm. The stretching of the FE model was simulated with the range of elongation at 10, 20 and 30 percent from its original length in order to find the strain value for all three of the conductor designs. The best conductor design is used to simulate with different types of substrate (PDMS and PU). From the simulation result, Horseshoe design record the lowest strain value for each elongation, followed by rectangular and U-shape design. Thus, Horseshoe is considered as the optimum design for the conductor compared to the other two designs. From the result also, it shows that PDMS substrate will offer more maximum allowable stretchability compared to PU substrates. Thus PDMS is considered as a better substrate compare to PU. PDMS is a good material to replace PU since it can perform under tension much better mechanically.

Direct Determination of the Intracellular Oxidation State of Plutonium

PubMed Central

Gorman-Lewis, Drew; Aryal, Baikuntha P.; Paunesku, Tatjana; Vogt, Stefan; Lai, Barry; Woloschak, Gayle E.; Jensen, Mark P.

2013-01-01

Microprobe X-ray absorption near edge structure (μ-XANES) measurements were used to determine directly, for the first time, the oxidation state of intracellular plutonium in individual 0.1 μm2 areas within single rat pheochromocytoma cells (PC12). The living cells were incubated in vitro for 3 hours in the presence of Pu added to the media in different oxidation states (Pu(III), Pu(IV), and Pu(VI)) and in different chemical forms. Regardless of the initial oxidation state or chemical form of Pu presented to the cells, the XANES spectra of the intracellular Pu deposits was always consistent with tetravalent Pu even though the intracellular milieu is generally reducing. PMID:21755934

Equilibrium, kinetic, and reactive transport models for plutonium

NASA Astrophysics Data System (ADS)

Schwantes, Jon Michael

Equilibrium, kinetic, and reactive transport models for plutonium (Pu) have been developed to help meet environmental concerns posed by past war-related and present and future peacetime nuclear technologies. A thorough review of the literature identified several hurdles that needed to be overcome in order to develop capable predictive tools for Pu. These hurdles include: (1) missing or ill-defined chemical equilibrium and kinetic constants for environmentally important Pu species; (2) no adequate conceptual model describing the formation of Pu oxy/hydroxide colloids and solids; and (3) an inability of two-phase reactive transport models to adequately simulate Pu behavior in the presence of colloids. A computer program called INVRS K was developed that integrates the geochemical modeling software of PHREEQC with a nonlinear regression routine. This program provides a tool for estimating equilibrium and kinetic constants from experimental data. INVRS K was used to regress on binding constants for Pu sorbing onto various mineral and humic surfaces. These constants enhance the thermodynamic database for Pu and improve the capability of current predictive tools. Time and temperature studies of the Pu intrinsic colloid were also conducted and results of these studies were presented here. Formation constants for the fresh and aged Pu intrinsic colloid were regressed upon using INVRS K. From these results, it was possible to develop a cohesive diagenetic model that describes the formation of Pu oxy/hydroxide colloids and solids. This model provides for the first time a means of deciphering historically unexplained observations with respect to the Pu intrinsic colloid, as well as a basis for simulating the behavior within systems containing these solids. Discussion of the development and application of reactive transport models is also presented and includes: (1) the general application of a 1-D in flow, three-phase (i.e., dissolved, solid, and colloidal), reactive transport model; (2) a simulation of the effects of dissolution of PuO2 solid and radiolysis on the behavior of Pu diffusing out of a confined pore space; and (3) application of a steady-state three phase reactive transport model to groundwater at the Nevada Test Site.

Energy dependence of fission product yields from 235U, 238U, and 239Pu with monoenergetic neutrons between thermal and 14.8 MeV

NASA Astrophysics Data System (ADS)

Gooden, Matthew; Arnold, Charles; Bhike, Megha; Bredeweg, Todd; Fowler, Malcolm; Krishichayan; Tonchev, Anton; Tornow, Werner; Stoyer, Mark; Vieira, David; Wilhelmy, Jerry

2017-09-01

Under a joint collaboration between TUNL-LANL-LLNL, a set of absolute fission product yield measurements has been performed. The energy dependence of a number of cumulative fission product yields (FPY) have been measured using quasi-monoenergetic neutron beams for three actinide targets, 235U, 238U and 239Pu, between 0.5 and 14.8 MeV. The FPYs were measured by a combination of fission counting using specially designed dual-fission chambers and γ-ray counting. Each dual-fission chamber is a back-to-back ionization chamber encasing an activation target in the center with thin deposits of the same target isotope in each chamber. This method allows for the direct measurement of the total number of fissions in the activation target with no reference to the fission cross-section, thus reducing uncertainties. γ-ray counting of the activation target was performed on well-shielded HPGe detectors over a period of two months post irradiation to properly identify fission products. Reported are absolute cumulative fission product yields for incident neutron energies of 0.5, 1.37, 2.4, 3.6, 4.6, 5.5, 7.5, 8.9 and 14.8 MeV. Preliminary results from thermal irradiations at the MIT research reactor will also be presented and compared to present data and evaluations. This work was performed under the auspices of the U.S. Department of Energy by Los Alamos National Security, LLC under contract DE-AC52-06NA25396, Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344 and by Duke University and Triangle Universities Nuclear Laboratory through NNSA Stewardship Science Academic Alliance grant No. DE-FG52-09NA29465, DE-FG52-09NA29448 and Office of Nuclear Physics Grant No. DE-FG02-97ER41033.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rim, Jung H.; Kuhn, Kevin J.; Tandon, Lav

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials’ properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modelling feedback andmore » trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. In conclusion, based on this investigation, the most likely intended use for these plutonium foils was 239Pu fission foil targets for physics experiments, such as cross-section measurements, etc.« less

Electrical, thermal and structural properties of plasticized waste cooking oil-based polyurethane solid polymer electrolyte

NASA Astrophysics Data System (ADS)

Huzaizi, Rahmatina Mohd; Tahir, Syuhada Mohd; Mahbor, Kamisah Mohamad

2017-12-01

Waste cooking oil-based polyol was synthesized using epoxidation and hydroxylation methods. The polyol was combined with 4,4-diphenylmethane diisocyanate to produce polyurethane (PU) to be used as polymer host in solid polymer electrolyte. 30 wt% LiClO4 was added as doping salt and two types of plasticizers were used; ethylene carbonate (PU-EC) and polyethylene glycol (PU-PEG). The SPE films were characterized using Fourier transform infrared spectroscopy, electrochemical impedance spectroscopy, differential scanning calorimetry (DSC) and X-ray diffraction (XRD). The highest conductivity achieved was 8.4 x 10-8 S cm-1 upon addition of 10 wt% EC. The XRD results showed a decrease of crystalline peaks in PU-EC and the increase in PU-PEG. DSC results revealed that the films; PU, PU-EC and PU-PEG had glass transition temperatures of 159.7, 106.0 and 179.7 °C, respectively. The results showed that the addition of EC increased the amorphous region and the free volume in the SPE structure, thus resulted in higher ionic conductivity.

Uptake and translocation of plutonium in two plant species using hydroponics.

PubMed

Lee, J H; Hossner, L R; Attrep, M; Kung, K S

2002-01-01

This study presents determinations of the uptake and translocation of Pu in Indian mustard (Brassica juncea) and sunflower (Helianthus annuus) from Pu contaminated solution media. The initial activity levels of Pu were 18.50 and 37.00 Bq ml(-1), for Pu-nitrate [239Pu(NO3)4] and for Pu-citrate [239Pu(C6H5O7)+] in nutrient solution. Plutonium-diethylenetriaminepentaacetic acid (DTPA: [239Pu-C14H23O10N3] solution was prepared by adding 0, 5, 10, and 50 microg of DTPA ml(-1) with 239Pu(NO3)4 in nutrient solution. Concentration ratios (CR, Pu concentration in dry plant material/Pu concentration in nutrient solution) and transport indices (Tl, Pu content in the shoot/Pu content in the whole plant) were calculated to evaluate Pu uptake and translocation. All experiments were conducted in hydroponic solution in an environmental growth chamber. Plutonium concentration in the plant tissue was increased with increased Pu contamination. Plant tissue Pu concentration for Pu-nitrate and Pu-citrate application was not correlated and may be dependent on plant species. For plants receiving Pu-DTPA, the Pu concentration was increased in the shoots but decreased in the roots resulting in a negative correlation between the Pu concentrations in the plant shoots and roots. The Pu concentration in shoots of Indian mustard was increased for application rates up to 10 microg DTPA ml(-1) and up to 5 microg DTPA ml(-1) for sunflower. Similar trends were observed for the CR of plants compared to the Pu concentration in the shoots and roots, whereas the Tl was increased with increasing DTPA concentration. Plutonium in shoots of Indian mustard was up to 10 times higher than that in shoots of sunflower. The Pu concentration in the apparent free space (AFS) of plant root tissue of sunflower was more affected by concentration of DTPA than that of Indian mustard.

Adaptive Unscented Kalman Filter Phase Unwrapping Method and Its Application on Gaofen-3 Interferometric SAR Data.

PubMed

Gao, Yandong; Zhang, Shubi; Li, Tao; Chen, Qianfu; Li, Shijin; Meng, Pengfei

2018-06-02

Phase unwrapping (PU) is a key step in the reconstruction of digital elevation models (DEMs) and the monitoring of surface deformation from interferometric synthetic aperture radar (SAR, InSAR) data. In this paper, an improved PU method that combines an amended matrix pencil model, an adaptive unscented kalman filter (AUKF), an efficient quality-guided strategy based on heapsort, and a circular median filter is proposed. PU theory and the existing UKFPU method are covered. Then, the improved method is presented with emphasis on the AUKF and the circular median filter. AUKF has been well used in other fields, but it is for the first time applied to interferometric images PU, to the best of our knowledge. First, the amended matrix pencil model is used to estimate the phase gradient. Then, an AUKF model is used to unwrap the interferometric phase based on an efficient quality-guided strategy based on heapsort. Finally, the key results are obtained by filtering the results using a circular median. The proposed method is compared with the minimum cost network flow (MCF), statistical cost network flow (SNAPHU), regularized phase tracking technique (RPTPU), and UKFPU methods using two sets of simulated data and two sets of experimental GF-3 SAR data. The improved method is shown to yield the greatest accuracy in the interferometric phase maps compared to the methods considered in this paper. Furthermore, the improved method is shown to be the most robust to noise and is thus most suitable for PU of GF-3 SAR data in high-noise and low-coherence regions.

Decreased solubilization of Pu(IV) polymers by humic acids under anoxic conditions

NASA Astrophysics Data System (ADS)

Xie, Jinchuan; Lin, Jianfeng; Liang, Wei; Li, Mei; Zhou, Xiaohua

2016-11-01

Pu(IV) polymer has a very low solubility (log[Pu(IV)aq]total = -10.4 at pH 7.2 and I = 0). However, some aspects of their environmental fate remain unclear. Humic acids are able to complex with Pu4+ ions and their dissolved species (<10 kD) in the groundwater (neutral to alkaline pH) may cause solubilization of the polymers. Also, humic acids have the native reducing capacity and potentially reduce the polymeric Pu(IV) to Pu(III)aq (log[Pu(III)aq]total = -5.3 at pH 7.2 and I = 0). Solubilization and reduction of the polymers can enhance their mobility in subsurface environments. Nevertheless, humic acids readily coat the surfaces of metal oxides via electrostatic interaction and ligand exchange mechanisms. The humic coatings are expected to prevent both solubilization and reduction of the polymers. Experiments were conducted under anoxic and slightly alkaline (pH 7.2) conditions in order to study whether humic acids have effects on stability of the polymers. The results show that the polymeric Pu(IV) was almost completely transformed into aqueous Pu(IV) in the presence of EDTA ligands. In contrast, the dissolved humic acids did not solubilize the polymers but in fact decreased their solubility by one order of magnitude. The humic coatings were responsible for the decreased solubilization. Such coatings limited the contact between the polymers and EDTA ligands, especially at the relatively high concentrations of humic acids (>0.57 mg/L). Solubilization of the humic-coated polymers was thus inhibited to a significant extent although EDTA, having the great complexation ability, was present in the humic solutions. Reduction of Pu(IV) polymers by the humic acids was also not observed in the absence of EDTA. In the presence of EDTA, the polymers were partially reduced to Pu(III)aq by the humic acids of 0.57 mg/L and the percentage of Pu(III)aq accounted for 51.7% of the total aqueous Pu. This demonstrates that the humic acids were able to reduce the aqueous Pu(IV), instead of the polymeric Pu(IV). Such a demonstration is supported by the very positive redox potential of aqueous Pu(IV)-EDTA complex: Eho ‧ (PuL24-/PuL25-) = 154.3 mV >>Eh (PuO2 (am) /Pu3+) = -182.7 mV calculated at 10-10 mol/L Pu3+ and pH 7.2. At the higher humic concentrations (>0.57 mg/L), the polymers were reduced to a lesser extent because the much denser humic coatings resulted in lower concentrations of the aqueous Pu(IV). Consequently, humic acids make Pu(IV) polymers pretty stable unless the artificial ligands such as EDTA are present in the groundwater.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Byerly, Benjamin L.; Stanley, Floyd; Spencer, Khal

In our study, a certified plutonium metal reference material (CRM 126) with a known production history is examined using analytical methods that are commonly employed in nuclear forensics for provenancing and attribution. Moreover, the measured plutonium isotopic composition and actinide assay are consistent with values reported on the reference material certificate. Model ages from U/Pu and Am/Pu chronometers agree with the documented production timeline. Finally, these results confirm the utility of these analytical methods and highlight the importance of a holistic approach for forensic study of unknown materials.

Green waste cooking oil-based rigid polyurethane foam

NASA Astrophysics Data System (ADS)

Enderus, N. F.; Tahir, S. M.

2017-11-01

Polyurethane is a versatile polymer traditionally prepared using petroleum-based raw material. Petroleum, however, is a non-renewable material and polyurethane produced was found to be non-biodegradable. In quest for a more environmentally friendly alternative, wastecooking oil, a highly abundant domestic waste with easily derivatized structure, is a viable candidate to replace petroleum. In this study,an investigation to determine physical and chemical properties of rigid polyurethane (PU) foam from waste cooking oil (WCO) was carried out. WCO was first adsorbed by using coconut husk activated carbon adsorbent prior to be used for polyol synthesis. The purified WCO was then used to synthesize polyol via transesterification reaction to yield alcohol groups in the WCO chains structure. Finally, the WCO-based polyol was used to prepare rigid PU foam. The optimum formulation for PU formation was found to be 90 polyol: 60 glycerol: 54 water: 40 diethanolamine: 23 diisocyanate. The rigid PU foam has density of 208.4 kg/m3 with maximum compressive strength and capability to receive load at 0.03 MPa and 0.09 kN, respectively. WCO-based PU can potentially be used to replace petroleum-based PU as house construction materials such as insulation panels.

Stream ambient noise, spectrum and propagation of sounds in the goby Padogobius martensii: sound pressure and particle velocity.

PubMed

Lugli, Marco; Fine, Michael L

2007-11-01

The most sensitive hearing and peak frequencies of courtship calls of the stream goby, Padogobius martensii, fall within a quiet window at around 100 Hz in the ambient noise spectrum. Acoustic pressure was previously measured although Padogobius likely responds to particle motion. In this study a combination pressure (p) and particle velocity (u) detector was utilized to describe ambient noise of the habitat, the characteristics of the goby's sounds and their attenuation with distance. The ambient noise (AN) spectrum is generally similar for p and u (including the quiet window at noisy locations), although the energy distribution of u spectrum is shifted up by 50-100 Hz. The energy distribution of the goby's sounds is similar for p and u spectra of the Tonal sound, whereas the pulse-train sound exhibits larger p-u differences. Transmission loss was high for sound p and u: energy decays 6-10 dB10 cm, and sound pu ratio does not change with distance from the source in the nearfield. The measurement of particle velocity of stream AN and P. martensii sounds indicates that this species is well adapted to communicate acoustically in a complex noisy shallow-water environment.

Development of a “Fission-proxy” Method for the Measurement of 14-MeV Neutron Fission Yields at CAMS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gharibyan, Narek

2016-10-25

Relative fission yield measurements were made for 50 fission products from 25.6±0.5 MeV alpha-induced fission of Th-232. Quantitative comparison of these experimentally measured fission yields with the evaluated fission yields from 14-MeV neutron-induced fission of U-235 demonstrates the feasibility of the proposed fission-proxy method. This new technique, based on the Bohr-independence hypothesis, permits the measurement of fission yields from an alternate reaction pathway (Th-232 + 25.6 MeV α → U-236* vs. U-235 + 14-MeV n → U-236*) given that the fission process associated with the same compound nucleus is independent of its formation. Other suitable systems that can potentially bemore » investigated in this manner include (but are not limited to) Pu-239 and U-237.« less

Resolving global versus local/regional Pu sources in the environment using sector ICP-MS

USGS Publications Warehouse

Ketterer, M.E.; Hafer, K.M.; Link, C.L.; Kolwaite, D.; Wilson, Jim; Mietelski, J.W.

2004-01-01

Sector inductively coupled plasma mass spectrometry is a versatile method for the determination of plutonium activities and isotopic compositions in samples containing this element at fallout levels. Typical detection limits for 239+240Pu are 0.1, 0.02 and 0.002 Bq kg -1Pu for samples sizes of 0.5 g, 3 g, and 50 g of soil, respectively. The application of sector ICP-MS-based Pu determinations is demonstrated in studies in sediment chronology, soil Pu inventory and depth distribution, and the provenance of global fallout versus local or regional Pu sources. A sediment core collected from Sloans Lake (Denver, Colorado, USA) exhibits very similar 137Cs and 239+240Pu activity profiles; 240Pu/239Pu atom ratios indicate possible small influences from the Nevada Test Site and/or the Rocky Flats Environmental Technology Site. An undisturbed soil profile from Lockett Meadow (Flagstaff, Arizona, USA) exhibits an exponential decrease in 239+240Pu activity versus depth; 240Pu/239Pu in the top 3 cm is slightly lower than the global fallout range of 0.180 ?? 0.014 due to possible regional influence of Nevada Test Site fallout. The 239??240Pu inventory at Lockett Meadow is 56 ?? 4 Bq m-2, consistent with Northern Hemisphere mid-latitude fallout. Archived NdF3 sources, prepared from Polish soils, demonstrate that substantial 239+240Pu from the 1986 Chernobyl disaster has been deposited in north eastern regions of Poland; compared to global fallout, Chernobyl Pu exhibits higher abundances of 240Pu and 241Pu. The ratios 240Pu/239pu and 241Pu/239Pu co-vary and range from 0.186-0.348 and 0.0029-0.0412, respectively, in forest soils (241Pu/239Pu = 0.2407??[240Pu/239Pu] - 0.0413; r2 = 0.9924). ?? The Royal Society of Chemistry 2004.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

The Department of Energy (DOE) has contracted with Asea Brown Boveri-Combustion Engineering (ABB-CE) to provide information on the capability of ABB-CE`s System 80 + Advanced Light Water Reactor (ALWR) to transform, through reactor burnup, 100 metric tonnes (MT) of weapons grade plutonium (Pu) into a form which is not readily useable in weapons. This information is being developed as part of DOE`s Plutonium Disposition Study, initiated by DOE in response to Congressional action. This document, Volume 1, presents a technical description of the various elements of the System 80 + Standard Plant Design upon which the Plutonium Disposition Study wasmore » based. The System 80 + Standard Design is fully developed and directly suited to meeting the mission objectives for plutonium disposal. The bass U0{sub 2} plant design is discussed here.« less

Precise 238U(n,2n)237U reaction cross-section measurements using the activation facility at TUNL

NASA Astrophysics Data System (ADS)

Krishichayan, Fnu; Bhike, M.; Tornow, W.

2014-09-01

Accurate neutron-induced 238U(n,2n)237U reaction data are required for many practical applications, especially in the field of nuclear energy, including advanced heavy water reactors, where 238U is used as the breeding material to regenerate the fissile material 239Pu. Precise (n,2n) cross-section measurements of 238U are underway at TUNL with mono-energetic neutrons in the 8.0 to 14.0 MeV energy range in steps of 0.25 MeV using the activation technique. After activation of the 0.5 inch diameter and 442 mg 238U foil, the activity of the 208 keV characteristic γ-line is tracked for 6 weeks with a high efficient HPGe clover detector to determine the initial activity needed for the cross-section determination. Results of the cross-section measurements, determined relative to 27Al and 197Au neutron activation monitor foils, and the comparison with theoretical models will be presented during the meeting.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

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 splitmore » 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. Multiple vacuum box locations may be set-up to supply several ICP-MS units with purified sample fractions such that a high sample throughput may be achieved, while still allowing for rapid measurement of short-lived actinides by alpha spectrometry.« less

Full-length U-xPu-10Zr (x = 0, 8, 19 wt.%) fast reactor fuel test in FFTF

NASA Astrophysics Data System (ADS)

Porter, D. L.; Tsai, Hanchung

2012-08-01

The Integral Fast Reactor-1 (IFR-1) experiment performed in the Fast Flux Test Facility (FFTF) was the only U-Pu-10Zr (Pu-0, 8 and 19 wt.%) metallic fast reactor test with commercial-length (91.4-cm active fuel-column length) conducted to date. With few remaining test reactors, there is little opportunity for performing another test with a long active fuel column. The assembly was irradiated to the goal burnup of 10 at.%. The beginning-of-life (BOL) peak cladding temperature of the hottest pin was 608 °C, cooling to 522 °C at end-of-life (EOL). Selected fuel pins were examined non-destructively using neutron radiography, precision axial gamma scanning, and both laser and spiral contact cladding profilometry. Destructive exams included plenum gas pressure, volume, and gas composition determinations on a number of pins followed by optical metallography, electron probe microanalysis (EPMA), and alpha and beta-gamma autoradiography on a single U-19Pu-10Zr pin. The post-irradiation examinations (PIEs) showed very few differences compared to the short-pin (34.3-cm fuel column) testing performed on fuels of similar composition in Experimental Breeder Reactor-II (EBR-II). The fuel column grew axially slightly less than observed in the short pins, but with the same pattern of decreasing growth with increasing Pu content. There was a difference in the fuel-cladding chemical interaction (FCCI) in that the maximum cladding penetration by interdiffusion with fuel/fission products did not occur at the top of the fuel column where the cladding temperature is highest, as observed in EBR-II tests. Instead, the more exaggerated fission-rate profile of the FFTF pins resulted in a peak FCCI at ˜0.7 X/L axial location along the fuel column. This resulted from a higher production of rare-earth fission products at this location and a higher ΔT between fuel center and cladding than at core center, together providing more rare earths at the cladding and more FCCI. This behavior could actually help extend the life of a fuel pin in a "long pin" reactor design to a higher peak fuel burnup.

Project Officer Training for Grants and Cooperative ...

EPA Pesticide Factsheets

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Radioactivity in trinitite six decades later.

PubMed

Parekh, Pravin P; Semkow, Thomas M; Torres, Miguel A; Haines, Douglas K; Cooper, Joseph M; Rosenberg, Peter M; Kitto, Michael E

2006-01-01

The first nuclear explosion test, named the Trinity test, was conducted on July 16, 1945 near Alamogordo, New Mexico. In the tremendous heat of the explosion, the radioactive debris fused with the local soil into a glassy material named Trinitite. Selected Trinitite samples from ground zero (GZ) of the test site were investigated in detail for radioactivity. The techniques used included alpha spectrometry, high-efficiency gamma-ray spectrometry, and low-background beta counting, following the radiochemistry for selected radionuclides. Specific activities were determined for fission products (90Sr, 137Cs), activation products (60Co, 133Ba, 152Eu, 154Eu, 238Pu, 241Pu), and the remnants of the nuclear fuel (239Pu, 240Pu). Additionally, specific activities of three natural radionuclides (40K, 232Th, 238U) and their progeny were measured. The determined specific activities of radionuclides and their relationships are interpreted in the context of the fission process, chemical behavior of the elements, as well as the nuclear explosion phenomenology.

Plutonium in the WIPP environment: its detection, distribution and behavior.

PubMed

Thakur, P; Ballard, S; Nelson, R

2012-05-01

The Waste Isolation Pilot Plant (WIPP) is the only operating deep underground geologic nuclear repository in the United States. It is located in southeastern New Mexico, approximately 655 m (2150 ft) below the surface of the Earth in a bedded Permian evaporite salt formation. This mined geologic repository is designed for the safe disposal of transuranic (TRU) wastes generated from the US defense program. Aerosol and soil samples have been collected near the WIPP site to investigate the sources of plutonium in the WIPP environment since the late 1990s, well before WIPP received its first shipment. Activities of (238)Pu, (239+240)Pu and (241)Am were determined by alpha spectrometry following a series of chemical separations. The concentrations of Al and U were determined in a separate set of samples by inductively coupled plasma mass spectrometry. The annual airborne concentrations of (239+240)Pu during the period from 1998 to 2010 show no systematic interannual variations. However, monthly (239+240)Pu particulate concentrations show a typical seasonal variation with a maximum in spring, the time when strong and gusty winds frequently give rise to blowing dust. Resuspension of soil particles containing weapons fallout is considered to be the predominant source of plutonium in the WIPP area. Further, this work characterizes the source, temporal variation and its distribution with depth in a soil profile to evaluate the importance of transport mechanisms affecting the fate of these radionuclides in the WIPP environment. The mean (137)Cs/(239+240)Pu, (241)Am/(239+240)Pu activity ratio and (240)Pu/(239)Pu atom ratio observed in the WIPP samples are consistent with the source being largely global fallout. There is no evidence of any release from the WIPP contributing to radionuclide concentrations in the environment.

Plutonium isotopes in the atmosphere of Central Europe: Isotopic composition and time evolution vs. circulation factors.

PubMed

Kierepko, Renata; Mietelski, Jerzy W; Ustrnul, Zbigniew; Anczkiewicz, Robert; Wershofen, Herbert; Holgye, Zoltan; Kapała, Jacek; Isajenko, Krzysztof

2016-11-01

This paper reports evidence of Pu isotopes in the lower part of the troposphere of Central Europe. The data were obtained based on atmospheric aerosol fraction samples collected from four places in three countries (participating in the informal European network known as the Ring of Five (Ro5)) forming a cell with a surface area of about 200,000km(2). We compared our original data sets from Krakow (Poland, 1990-2007) and Bialystok (Poland, 1991-2007) with the results from two other locations, Prague (Czech Republic; 1997-2004) and Braunschweig (Germany; 1990-2003) to find time evolution of the Pu isotopes. The levels of the activity concentration for (238)Pu and for ((239+240))Pu were estimated to be a few and some tens of nBqm(-3), respectively. However, we also noted some results were much higher (even about 70 times higher) than the average concentration of (238)Pu in the atmosphere. The achieved complex data sets were used to test a new approach to the problem of solving mixing isotopic traces from various sources (here up to three) in one sample. Results of our model, supported by mesoscale atmospheric circulation parameters, suggest that Pu from nuclear weapon accidents or tests and nuclear burnt-up fuel are present in the air. Copyright © 2016 Elsevier B.V. All rights reserved.

Response of Polyurethane to Shock Waves: An Experimental Investigation

NASA Astrophysics Data System (ADS)

Jayaram, V.; Rao, Keshava Subba; Thanganayaki, N.; Kumara, H. K. T.; Reddy, K. P. J.

Formation of polyurethane (PU) in vacuum environment and controlling density of polyurethane foams are the present day challenges. Polyurethane exists in numerous forms ranging from flexible to rigid and lightweight foams to tough, stiff elastomers [1]. PU can be used to produce lightweight foams for insulation or hard rubber used as wheels to transport heavy loads and it can be used in high pressure applications. The largest volumes of commercial PU elastomers are made from toluene diisocyanate (TDI) or diphenylmethane-4, 4'-diisocyanate (MDI) [2]. Linear polyurethanes can be processed into final products by any of the standard thermoplastic processes (injection molding, extrusion, thermoforming) as well as by low pressure cast processes in presence of catalysts. Tin, tetrabutyl titanate and zirconium chelates are few effective catalysts used to produce polyurethane for particular application [3]. Thermoset elastomers are formed due to irreversible cross-links, when polymers are chemically cured. Highly porous biodegradable PU was synthesized by thermally induced phase separation technique used in tissue engineering and also in bio-degradable based fluids [4]. Properties of PU like hardness, stress/strain modulus, tear strength etc, was determine using ASTM (American Society for Testing and Materials) standard methods. PU possesses extremely high mechanical properties, excellent abrasion, tear and extrusion resistance. It has outstanding low-temperature limit (-600C) and high temperature limit up to (1500C).

A XAS study of the local environments of cations in (U, Ce)O 2

NASA Astrophysics Data System (ADS)

Martin, Philippe; Ripert, Michel; Petit, Thierry; Reich, Tobias; Hennig, Christoph; D'Acapito, Francesco; Hazemann, Jean Louis; Proux, Olivier

2003-01-01

Mixed oxide (MOX) fuel is usually considered as a solid solution formed by uranium and plutonium dioxides. Nevertheless, some physico-chemical properties of (U 1- y, Pu y)O 2 samples manufactured under industrial conditions showed anomalies in the domain of plutonium contents ranging between 3 and 15 at.%. Cerium is commonly used as an inactive analogue of plutonium in preliminary studies on MOX fuels. Extended X-ray Absorption Fine Structure (EXAFS) measurements performed at the European Synchrotron Radiation Facility (ESRF) at the cerium and uranium edges on (U 1- y, Ce y)O 2 samples are presented and discussed. They confirmed on an atomic scale the formation of an ideal solid solution for cerium concentrations ranging between 0 and 50 at.%.

A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy

DOE PAGES

Knowles, Justin R.; Skutnik, Steven E.; Glasgow, David C.; ...

2016-06-23

Rapid non-destructive assay methods for trace fissile material analysis are needed in both nuclear forensics and safeguards communities. To address these needs, research at the High Flux Isotope Reactor Neutron Activation Analysis laboratory has developed a generalized non-destructive assay method to characterize materials containing fissile isotopes. This method relies on gamma-ray emissions from short-lived fission products and capitalizes off of differences in fission product yields to identify fissile compositions of trace material samples. Although prior work has explored the use of short-lived fission product gamma-ray measurements, the proposed method is the first to provide a holistic characterization of isotopic identification,more » mass ratios, and absolute mass determination. Successful single fissile isotope mass recoveries of less than 6% error have been conducted on standards of 235U and 239Pu as low as 12 nanograms in less than 10 minutes. Additionally, mixtures of fissile isotope standards containing 235U and 239Pu have been characterized as low as 229 nanograms of fissile mass with less than 12% error. The generalizability of this method is illustrated by evaluating different fissile isotopes, mixtures of fissile isotopes, and two different irradiation positions in the reactor. Furthermore, it is anticipated that this method will be expanded to characterize additional fissile nuclides, utilize various irradiation sources, and account for increasingly complex sample matrices.« less

A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy

NASA Astrophysics Data System (ADS)

Knowles, Justin; Skutnik, Steven; Glasgow, David; Kapsimalis, Roger

2016-10-01

Rapid nondestructive assay methods for trace fissile material analysis are needed in both nuclear forensics and safeguards communities. To address these needs, research at the Oak Ridge National Laboratory High Flux Isotope Reactor Neutron Activation Analysis facility has developed a generalized nondestructive assay method to characterize materials containing fissile isotopes. This method relies on gamma-ray emissions from short-lived fission products and makes use of differences in fission product yields to identify fissile compositions of trace material samples. Although prior work has explored the use of short-lived fission product gamma-ray measurements, the proposed method is the first to provide a complete characterization of isotopic identification, mass ratios, and absolute mass determination. Successful single fissile isotope mass recoveries of less than 6% recovery bias have been conducted on standards of 235U and 239Pu as low as 12 ng in less than 10 minutes. Additionally, mixtures of fissile isotope standards containing 235U and 239Pu have been characterized as low as 198 ng of fissile mass with less than 7% recovery bias. The generalizability of this method is illustrated by evaluating different fissile isotopes, mixtures of fissile isotopes, and two different irradiation positions in the reactor. It is anticipated that this method will be expanded to characterize additional fissile nuclides, utilize various irradiation facilities, and account for increasingly complex sample matrices.

A generalized method for characterization of 235U and 239Pu content using short-lived fission product gamma spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Knowles, Justin R.; Skutnik, Steven E.; Glasgow, David C.

Rapid non-destructive assay methods for trace fissile material analysis are needed in both nuclear forensics and safeguards communities. To address these needs, research at the High Flux Isotope Reactor Neutron Activation Analysis laboratory has developed a generalized non-destructive assay method to characterize materials containing fissile isotopes. This method relies on gamma-ray emissions from short-lived fission products and capitalizes off of differences in fission product yields to identify fissile compositions of trace material samples. Although prior work has explored the use of short-lived fission product gamma-ray measurements, the proposed method is the first to provide a holistic characterization of isotopic identification,more » mass ratios, and absolute mass determination. Successful single fissile isotope mass recoveries of less than 6% error have been conducted on standards of 235U and 239Pu as low as 12 nanograms in less than 10 minutes. Additionally, mixtures of fissile isotope standards containing 235U and 239Pu have been characterized as low as 229 nanograms of fissile mass with less than 12% error. The generalizability of this method is illustrated by evaluating different fissile isotopes, mixtures of fissile isotopes, and two different irradiation positions in the reactor. Furthermore, it is anticipated that this method will be expanded to characterize additional fissile nuclides, utilize various irradiation sources, and account for increasingly complex sample matrices.« less

Variations in trace metal and halogen ratios in magmatic gases through an eruptive cycle of the Pu'u O'o vent, Kilauea, Hawaii: July-August 1985

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miller, T.L.; Zoller, W.H.; Crowe, B.M.

1990-08-10

Particle and gas samples were obtained before and after eruptive episode 35 in July and August 1985 at the fuming Pu'u O'o vent, Kilauea volcano, Hawaii. The sampling system employed consisted of a particle filter followed by four {sup 7}LiOH treated filters to collect acidic gases. The filters were analyzed using instrumental neutron activation analysis (INAA). The results indicate that Br/Cl and Re/Cl ratios do not fluctuate through an eruption cycle but the F/Cl, F/Br and metal/Cl ratios (In and Cd) do change through the cycle. An inverse relationship between F/Cl and metal/Cl was observed. The changes are probably duemore » to influxes of relatively undegassed magma during the repose period releasing fume with lower F/Cl, F/BR and higher metal/Cl ratios. As the magma in the Pu'u O'o conduit gradually degasses either before or several days after an eruptive episode, F/Cl and F/Br ratios increase and the metal/Cl ratios decrease. One sample collected on July 24, two days before eruptive episode 35, did not follow this general trend. This can be explained by a gas pulse from a deeper, less degassed portion of magma making its way to the top of the conduit.« less

Presence de Carbone-13 dans les elements combustibles de type (U,Pu)O 2 irradies en reacteur rapide

NASA Astrophysics Data System (ADS)

Kryger, Bernard; Hagemann, Robert

1982-06-01

Du carbone-13 produit par la réaction de capture neutronique 168O + 10n → 136C + 42He se forme dans les combustibles de type oxyde irradiés en neutrons rapides. Cette réaction, dont le seuil d'énergie se situe à 2.35 MeV, conduit à la formation d'une quantité de carbone-13 qui peut varier notablement suivant le spectre neutronique du réacteur (entre 20 et 40 × 10 -6g 13C/g (U,Pu)O 2 pour une fluence de 2 × 10 23 n/cm 2). DES mesures effectuées sur le combustible et la gaine par spectrométrie de masse après irradiation montrent qu'une fraction égale ou supérieure à la moitié du carbone-13 produit dans l'oxyde peut être transférée dans la gaine. Un tel comportement nous fait considérer le carbone-13 comme un véritable marqueur du carbone plus généralement contenu dans l'oxyde et, à ce titre, la détection de cet isotope devrait contribuer à élucider tout particulièrement les mécanismes de carburation de la gaine par les combustibles (U,Pu)O 2 des réacteurs surgénérateurs.

"Variations in trace metal and halogen ratios in magmatic gases through an eruptive. Cycle of the Pu'u O'o Vent, Kilauea, Hawaii: July-August 1985""

NASA Astrophysics Data System (ADS)

Miller, Theresa L.; Zoller, William H.; Crowe, Bruce M.; Finnegan, David L.

1990-08-01

Particle and gas samples were obtained before and after eruptive episode 35 in July and August 1985 at the fuming Pu'u O'o vent, Kilauea volcano, Hawaii. The sampling system employed consisted of a particle filter followed by four 7LiOH treated filters to collect acidic gases. The filters were analyzed using instrumental neutron activation analysis (INAA). The results indicate that Br/Cl and Re/Cl ratios do not fluctuate through an eruption cycle but the F/Cl, F/Br and metal/Cl ratios (In and Cd) do change through the cycle. An inverse relationship between F/Cl and metal/Cl was observed. The changes are probably due to influxes of relatively undegassed magma during the repose period releasing fume with lower F/Cl, F/Br and higher metal/Cl ratios. As the magma in the Pu'u O'o conduit gradually degasses either before or several days after an eruptive episode, F/Cl and F/Br ratios increase and the metal/Cl ratios decrease. One sample collected on July 24, two days before eruptive episode 35, did not follow this general trend. This can be explained by a gas pulse from a deeper, less degassed portion of magma making its way to the top of the conduit.

Magma flow between summit and Pu`u `Ō`ō at K¯lauea Volcano, Hawai`i

NASA Astrophysics Data System (ADS)

Montagna, C. P.; Gonnermann, H. M.

2013-07-01

Volcanic eruptions are often accompanied by spatiotemporal migration of ground deformation, a consequence of pressure changes within magma reservoirs and pathways. We modeled the propagation of pressure variations through the east rift zone (ERZ) of K¯lauea Volcano, Hawai`i, caused by magma withdrawal during the early eruptive episodes (1983-1985) of the ongoing Pu`u `Ō`ō-Kupaianaha eruption. Eruptive activity at the Pu`u `Ō`ō vent was typically accompanied by abrupt deflation that lasted for several hours and was followed by a sudden onset of gradual inflation once the eruptive episode had ended. Similar patterns of deflation and inflation were recorded at K¯lauea's summit, approximately 15 km to the northwest, albeit with time delays of hours. These delay times can be reproduced by modeling the spatiotemporal changes in magma pressure and flow rate within an elastic-walled dike that traverses K¯lauea's ERZ. Key parameters that affect the behavior of the magma-dike system are the dike dimensions, the elasticity of the wall rock, the magma viscosity, and to a lesser degree the magnitude and duration of the pressure variations themselves. Combinations of these parameters define a transport efficiency and a pressure diffusivity, which vary somewhat from episode to episode, resulting in variations in delay times. The observed variations in transport efficiency are most easily explained by small, localized changes to the geometry of the magma pathway.

Neutron induced fission cross section measurements of 240Pu and 242Pu

NASA Astrophysics Data System (ADS)

Belloni, F.; Eykens, R.; Heyse, J.; Matei, C.; Moens, A.; Nolte, R.; Plompen, A. J. M.; Richter, S.; Sibbens, G.; Vanleeuw, D.; Wynants, R.

2017-09-01

Accurate neutron induced fission cross section of 240Pu and 242Pu are required in view of making nuclear technology safer and more efficient to meet the upcoming needs for the future generation of nuclear power plants (GEN-IV). The probability for a neutron to induce such reactions figures in the NEA Nuclear Data High Priority Request List [1]. A measurement campaign to determine neutron induced fission cross sections of 240Pu and 242Pu at 2.51 MeV and 14.83 MeV has been carried out at the 3.7 MV Van De Graaff linear accelerator at Physikalisch-Technische Bundesanstalt (PTB) in Braunschweig. Two identical Frisch Grid fission chambers, housing back to back a 238U and a APu target (A = 240 or A = 242), were employed to detect the total fission yield. The targets were molecular plated on 0.25 mm aluminium foils kept at ground potential and the employed gas was P10. The neutron fluence was measured with the proton recoil telescope (T1), which is the German primary standard for neutron fluence measurements. The two measurements were related using a De Pangher long counter and the charge as monitors. The experimental results have an average uncertainty of 3-4% at 2.51 MeV and for 6-8% at 14.81 MeV and have been compared to the data available in literature.

The Archaeology of the Bug Hill Site (34Pu-116): Pushmataha County, Oklahoma.

DTIC Science & Technology

1982-01-01

parts of the left mandible. The post cranial skeleton consisted of two cervical, eight thoracic, three lumbar vertebrae, and qi 54 Figure 14. a: Feature...partial sacrilization of the fifth lumbar vertebrae. An unexplained anomaly is the antero-lateral amputation of the styloid process of the right temporal...CM U 5CM E 60 metatarsals, and 20 ribs were present. The vertebral column is repre- sented by five cervical, ten thoracic, five lumbar , and five

Modelling the behaviour of oxide fuels containing minor actinides with urania, thoria and zirconia matrices in an accelerator-driven system

NASA Astrophysics Data System (ADS)

Sobolev, V.; Lemehov, S.; Messaoudi, N.; Van Uffelen, P.; Aı̈t Abderrahim, H.

2003-06-01

The Belgian Nuclear Research Centre, SCK • CEN, is currently working on the pre-design of the multipurpose accelerator-driven system (ADS) MYRRHA. A demonstration of the possibility of transmutation of minor actinides and long-lived fission products with a realistic design of experimental fuel targets and prognosis of their behaviour under typical ADS conditions is an important task in the MYRRHA project. In the present article, the irradiation behaviour of three different oxide fuel mixtures, containing americium and plutonium - (Am,Pu,U)O 2- x with urania matrix, (Am,Pu,Th)O 2- x with thoria matrix and (Am,Y,Pu,Zr)O 2- x with inert zirconia matrix stabilised by yttria - were simulated with the new fuel performance code MACROS, which is under development and testing at the SCK • CEN. All the fuel rods were considered to be of the same design and sizes: annular fuel pellets, helium bounded with the stainless steel cladding, and a large gas plenum. The liquid lead-bismuth eutectic was used as coolant. Typical irradiation conditions of the hottest fuel assembly of the MYRRHA subcritical core were pre-calculated with the MCNPX code and used in the following calculations as the input data. The results of prediction of the thermo-mechanical behaviour of the designed rods with the considered fuels during three irradiation cycles of 90 EFPD are presented and discussed.

PLANTS AS BIO-MONITORS FOR 137CS, 238PU, 239, 240PU AND 40K AT THE SAVANNAH RIVER SITE

DOE Office of Scientific and Technical Information (OSTI.GOV)

Caldwell, E.; Duff, M.; Ferguson, C.

2010-12-16

The nuclear fuel cycle generates a considerable amount of radioactive waste, which often includes nuclear fission products, such as strontium-90 ({sup 90}Sr) and cesium-137 ({sup 137}Cs), and actinides such as uranium (U) and plutonium (Pu). When released into the environment, large quantities of these radionuclides can present considerable problems to man and biota due to their radioactive nature and, in some cases as with the actinides, their chemical toxicity. Radionuclides are expected to decay at a known rate. Yet, research has shown the rate of elimination from an ecosystem to differ from the decay rate due to physical, chemical andmore » biological processes that remove the contaminant or reduce its biological availability. Knowledge regarding the rate by which a contaminant is eliminated from an ecosystem (ecological half-life) is important for evaluating the duration and potential severity of risk. To better understand a contaminants impact on an environment, consideration should be given to plants. As primary producers, they represent an important mode of contamination transfer from sediments and soils into the food chain. Contaminants that are chemically and/or physically sequestered in a media are less likely to be bio-available to plants and therefore an ecosystem.« less

Stress Concentrations.

DTIC Science & Technology

1982-09-01

a joJo p~ ~qJO iju;~33 oa~u UO~u~aUuo3-s;JS I I awnh!d pu1 IuwLaqdsawq aqlI i~ pjO3U u L1 t 3AIWSOd NANOHS 3AIIISOd NAMONS SQOl Q3liddV 3Y 1 0 SOV0I...caesgi 30332 50S King Avenue Drxel University Clmu.Oi 30 Department of mechanical enginserieg prof essor Graham.?. Carey ClmuOi 30 and mechanics

Analysis Of 2H-Evaporator Scale Pot Bottom Sample [HTF-13-11-28H

DOE Office of Scientific and Technical Information (OSTI.GOV)

Oji, L. N.

2013-07-15

Savannah River Remediation (SRR) is planning to remove a buildup of sodium aluminosilicate scale from the 2H-evaporator pot by loading and soaking the pot with heated 1.5 M nitric acid solution. Sampling and analysis of the scale material from the 2H evaporator has been performed so that the evaporator can be chemically cleaned beginning July of 2013. Historically, since the operation of the Defense Waste Processing Facility (DWPF), silicon in the DWPF recycle stream combines with aluminum in the typical tank farm supernate to form sodium aluminosilicate scale mineral deposits in the 2H-evaporator pot and gravity drain line. The 2H-evaporatormore » scale samples analyzed by Savannah River National Laboratory (SRNL) came from the bottom cone sections of the 2H-evaporator pot. The sample holder from the 2H-evaporator wall was virtually empty and was not included in the analysis. It is worth noting that after the delivery of these 2H-evaporator scale samples to SRNL for the analyses, the plant customer determined that the 2H evaporator could be operated for additional period prior to requiring cleaning. Therefore, there was no need for expedited sample analysis as was presented in the Technical Task Request. However, a second set of 2H evaporator scale samples were expected in May of 2013, which would need expedited sample analysis. X-ray diffraction analysis (XRD) confirmed the bottom cone section sample from the 2H-evaporator pot consisted of nitrated cancrinite, (a crystalline sodium aluminosilicate solid), clarkeite and uranium oxide. There were also mercury compound XRD peaks which could not be matched and further X-ray fluorescence (XRF) analysis of the sample confirmed the existence of elemental mercury or mercuric oxide. On ''as received'' basis, the scale contained an average of 7.09E+00 wt % total uranium (n = 3; st.dev. = 8.31E-01 wt %) with a U-235 enrichment of 5.80E-01 % (n = 3; st.dev. = 3.96E-02 %). The measured U-238 concentration was 7.05E+00 wt % (n=3, st. dev. = 8.25E-01 wt %). Analyses results for Pu-238 and Pu-239, and Pu-241 are 7.06E-05 {+-} 7.63E-06 wt %, 9.45E-04 {+-} 3.52E-05 wt %, and <2.24E-06 wt %, respectively. These results are provided so that SRR can calculate the equivalent uranium-235 concentrations for the NCSA. Because this 2H evaporator pot bottom scale sample contained a significant amount of elemental mercury (11.7 wt % average), it is recommended that analysis for mercury be included in future Technical Task Requests on 2H evaporator sample analysis at SRNL. Results confirm that the uranium contained in the scale remains depleted with respect to natural uranium. SRNL did not calculate an equivalent U-235 enrichment, which takes into account other fissionable isotopes U-233, Pu-239 and Pu-241.« less

Plutonium oxalate precipitation for trace elemental determination in plutonium materials

DOE PAGES

Xu, Ning; Gallimore, David; Lujan, Elmer; ...

2015-05-26

In this study, an analytical chemistry method has been developed that removes the plutonium (Pu) matrix from the dissolved Pu metal or oxide solution prior to the determination of trace impurities that are present in the metal or oxide. In this study, a Pu oxalate approach was employed to separate Pu from trace impurities. After Pu(III) was precipitated with oxalic acid and separated by centrifugation, trace elemental constituents in the supernatant were analyzed by inductively coupled plasma-optical emission spectroscopy with minimized spectral interferences from the sample matrix.

Nuclear Data Sheets for A = 239

DOE PAGES

Browne, E.; Tuli, J. K.

2014-11-18

Spectroscopic data and level schemes from radioactive decay and nuclear reaction studies are presented here for all nuclei with mass number A=239. In general, a relatively small amount of new data on this mass chain has been reported since the previous evaluation in 2003. However, special evaluations, such as ''Database of prompt gamma rays from slow neutron–capture from elemental analysis'' (2007ChZX), have provided additional precise data for levels in 29U. Also, new Coulomb excitation measurements in 239Pu have extended the knowledge of the 1/2[631] rotational band up to Jπ=(55/2+)Jπ=(55/2+), and that of the octupole vibrational band up to Jπ=(53/2-)Jπ=(53/2-). Formore » historical knowledge it is worth mentioning the report on the “Discovery of isotopes of the transuranium elements with 93 <= Z <= 98'' (2013Fr02), where the information for elements Np, Pu, Am, and Cf with mass number A=239 is presented. The alpha hindrance factors (HF) presented in this evaluation were calculated using values of the radius parameter (r 0) interpolated from those for even–even adjacent nuclei given by 1998Ak04.« less

Nuclear Data Sheets for A = 239

DOE Office of Scientific and Technical Information (OSTI.GOV)

Browne, E.; Tuli, J. K.

Spectroscopic data and level schemes from radioactive decay and nuclear reaction studies are presented here for all nuclei with mass number A=239. In general, a relatively small amount of new data on this mass chain has been reported since the previous evaluation in 2003. However, special evaluations, such as ''Database of prompt gamma rays from slow neutron–capture from elemental analysis'' (2007ChZX), have provided additional precise data for levels in 29U. Also, new Coulomb excitation measurements in 239Pu have extended the knowledge of the 1/2[631] rotational band up to Jπ=(55/2+)Jπ=(55/2+), and that of the octupole vibrational band up to Jπ=(53/2-)Jπ=(53/2-). Formore » historical knowledge it is worth mentioning the report on the “Discovery of isotopes of the transuranium elements with 93 <= Z <= 98'' (2013Fr02), where the information for elements Np, Pu, Am, and Cf with mass number A=239 is presented. The alpha hindrance factors (HF) presented in this evaluation were calculated using values of the radius parameter (r 0) interpolated from those for even–even adjacent nuclei given by 1998Ak04.« less

Nuclear Data Sheets for A = 239

DOE Office of Scientific and Technical Information (OSTI.GOV)

Browne, E.; Tuli, J.K.

Spectroscopic data and level schemes from radioactive decay and nuclear reaction studies are presented here for all nuclei with mass number A=239. In general, a relatively small amount of new data on this mass chain has been reported since the previous evaluation in 2003. However, special evaluations, such as “Database of prompt gamma rays from slow neutron–capture from elemental analysis” (2007ChZX), have provided additional precise data for levels in {sup 239}U. Also, new Coulomb excitation measurements in {sup 239}Pu have extended the knowledge of the 1/2[631] rotational band up to Jπ=(55/2+), and that of the octupole vibrational band up tomore » Jπ=(53/2−). For historical knowledge it is worth mentioning the report on the “Discovery of isotopes of the transuranium elements with 93 <= Z <= 98” (2013Fr02), where the information for elements Np, Pu, Am, and Cf with mass number A=239 is presented. The alpha hindrance factors (HF) presented in this evaluation were calculated using values of the radius parameter (r{sub 0}) interpolated from those for even–even adjacent nuclei given by 1998Ak04.« less

Healthy Skin Wins: A Glowing Pressure Ulcer Prevention Program That Can Guide Evidence-Based Practice.

PubMed

Martin, Donna; Albensi, Lisa; Van Haute, Stephanie; Froese, Maria; Montgomery, Mary; Lam, Mavis; Gierys, Kendra; Lajeunesse, Rob; Guse, Lorna; Basova, Nataliya

2017-12-01

In 2013, an observational survey was conducted among 242 in-patients in a community hospital with a pressure ulcer (PU) prevalence of 34.3%. An evidence-based pressure ulcer prevention program (PUPP) was then implemented including a staff awareness campaign entitled "Healthy Skin Wins" with an online tutorial about PU prevention. To determine the effectiveness of the PUPP in reducing the prevalence of PUs, to determine the effectiveness of the online tutorial in increasing hospital staff's knowledge level about PU prevention, and to explore frontline staff's perspectives of the PUPP. This was a mixed methods study. A repeat observational survey discerned if the PUPP reduced PU prevalence. A pre-test post-test design was used to determine whether hospital staff's knowledge of PU prevention was enhanced by the online tutorial. Qualitative interviews were conducted with nurses, allied health professionals, and health care aides to explore staff's perspectives of the PUPP. A comparison of initial and repeat observational surveys (n = 239) identified a statistically significant reduction in the prevalence of PU to 7.53% (p < .001). The online tutorial enhanced staff knowledge level with a statistically significantly higher mean post-test score (n = 80). Thirty-five frontline staff shared their perspectives of the PUPP with "it's definitely a combination of everything" and "there's a disconnect between what's needed and what's available" as the main themes. Incorporating evidence-based PU prevention into clinical practice greatly reduced the prevalence of PUs among hospital in-patients. Due to the small sample size for the pre-test post-test component, the effectiveness of the online tutorial in improving the knowledge level of PU prevention among hospital staff requires further research. Evidence-based PU prevention strategies are facilitated by using a multidisciplinary approach. Educational tools about PU prevention must target all members of the healthcare team including healthcare aides, patients and families. © 2017 The Authors. Worldviews on Evidence-Based Nursing published by Wiley Periodicals, Inc. on behalf of Sigma Theta Tau International The Honor Society of Nursing.

[Correlation between body mass index and development of pressure ulcers in intensive care medicine].

PubMed

Catalá Espinosa, A I; Hidalgo Encinas, Y; Cherednichenko, T; Flores Lucas, I; González Tamayo, R; García-Martínez, M Á; Herrero-Gutiérrez, E

2014-01-01

This study aims to evaluate the association between body mass index (BMI), incidence and severity of pressure ulcers (PU) in patients admitted to the Intensive Care Unit (ICU), and describe the differential prognosis of patients with PU and factors that modify it. Case-control study with observation period of 15 months. We collected baseline variables, prognostic scales, therapies and clinical outcome. Univariate analysis was performed for each outcome variable between cases and controls using the appropriate hypothesis test depending on the nature of the variables. ROC curve for BMI and PU. Logistic regression with PU as dependent variable and the covariates that reached p<0.05 in the bivariate analysis. Correlation using Pearson or Spearman was made between BMI, albumin, days to diagnosis of UPP, immobilization, and PU degree. Significance level at p <0.05. 77 patients developed PU and 231 controls were chosen. The cases had higher APACHE II (p=0.043) and SAPS 3 (p=0.023), length of stay in ICU and mechanical ventilation (p<0.001). BMI≥40 was associated with UPP (p=0.024 OR=3.23 CI95% 1.17-8.93). There was a significant association between PU degree, length of stay and MV (p<0,001), but not with immobilization, dynamic support surface and death rate. Multivariate analysis found association between PU, length of MV (p=0.013, OR 1.08, CI95% 1.01-1.16) and kidney replacement therapy (p=0.013, OR 3.55 CI95% 1.31-9.64), with BMI≥40 as a confounding factor. Length of mechanical ventilation and renal replacement therapy are risk factors for pressure ulcer development, and BMI≥40 acts as a confounding factor. PU development and its maximum degree are not associated with a worse prognosis. Copyright © 2013 Elsevier España, S.L.U. y SEEIUC. All rights reserved.

Safinamide (Newron Pharmaceuticals).

PubMed

Chazot, P L

2001-06-01

Safinamide (formerly PNU-151774E), a sodium and calcium channel modulator that also inhibits monoamine oxidase B (MAOB), is under development by Newron Pharmaceuticals for the potential treatment of epilepsy, Parkinson's disease (PD), pain and stroke [345222], [348351]. Phase I trials for epilepsy and PD have been completed, and dose-finding studies for both indications had commenced in March 2001 [401685]. The compound was previously developed by Pharmacia & Upjohn (P&U) for the potential treatment of epilepsy, an indication for which it initially reached phase I trials [294891], [345007]. Newron acquired the rights to safinamide from P&U at the end of 1998. Results from two phase I trials of the compound (single ascending dose and steady state at three doses), completed in March 2000, demonstrated that the drug is well tolerated with good bioavailability and linear pharmacokinetics [359652].