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.

U-PuO2, U-PuC, U-PuN cermet fuel for fast reactor

NASA Astrophysics Data System (ADS)

Mishra, Sudhir; Kaity, Santu; Banerjee, Joydipta; Nandi, Chiranjeet; Dey, G. K.; Khan, K. B.

2018-02-01

Cermet fuel combines beneficial properties of both ceramic and metal and attracts global interest for research as a candidate fuel for nuclear reactors. In the present study, U matrix PuC/PuN/PuO2 cermet for fast reactor have been fabricated on laboratory scale by the powder metallurgy route. Characterization of the fuel has been carried out using Dilatometer, Differential Thermal analysis (DTA), X-ray diffractometer and Optical microscope. X ray diffraction study of the fuel reveals presence of different phases. The PuN dispersed cermet was observed to have high solidus temperature as compared to PuC and PuO2 dispersed cermet. Swelling was observed in U matrix PuO2 cermet which also showed higher thermal expansion. Among the three cermets studied, U matrix PuC cermet showed maximum thermal conductivity.

Light Water Reactor Sustainability Accomplishments Report

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

McCarthy, Kathryn A.

Welcome to the 2014 Light Water Reactor Sustainability (LWRS) Program Accomplishments Report, covering research and development highlights from 2014. The LWRS Program is a U.S. Department of Energy research and development program to inform and support the long-term operation of our nation’s commercial nuclear power plants. The research uses the unique facilities and capabilities at the Department of Energy national laboratories in collaboration with industry, academia, and international partners. Extending the operating lifetimes of current plants is essential to supporting our nation’s base load energy infrastructure, as well as reaching the Administration’s goal of reducing greenhouse gas emissions to 80%more » below 1990 levels by the year 2050. The purpose of the LWRS Program is to provide technical results for plant owners to make informed decisions on long-term operation and subsequent license renewal, reducing the uncertainty, and therefore the risk, associated with those decisions. In January 2013, 104 nuclear power plants operated in 31 states. However, since then, five plants have been shut down (several due to economic reasons), with additional shutdowns under consideration. The LWRS Program aims to minimize the number of plants that are shut down, with R&D that supports long-term operation both directly (via data that is needed for subsequent license renewal), as well indirectly (with models and technology that provide economic benefits). The LWRS Program continues to work closely with the Electric Power Research Institute (EPRI) to ensure that the body of information needed to support SLR decisions and actions is available in a timely manner. This report covers selected highlights from the three research pathways in the LWRS Program: Materials Aging and Degradation, Risk-Informed Safety Margin Characterization, and Advanced Instrumentation, Information, and Control Systems Technologies, as well as a look-ahead at planned activities for 2015. If you have any questions about the information in the report, or about the LWRS Program, please contact me, Richard A. Reister (the Federal Program Manager), or the respective research pathway leader (noted on pages 26 and 27), or visit the LWRS Program website (www.inl.gov/lwrs). The annually updated Integrated Program Plan and Pathway Technical Program Plans are also available for those seeking more detailed technical Information.« less

Optimisation of composite metallic fuel for minor actinide transmutation in an accelerator-driven system

NASA Astrophysics Data System (ADS)

Uyttenhove, W.; Sobolev, V.; Maschek, W.

2011-09-01

A potential option for neutralization of minor actinides (MA) accumulated in spent nuclear fuel of light water reactors (LWRs) is their transmutation in dedicated accelerator-driven systems (ADS). A promising fuel candidate dedicated to MA transmutation is a CERMET composite with Mo metal matrix and (Pu, Np, Am, Cm)O 2-x fuel particles. Results of optimisation studies of the CERMET fuel targeting to increasing the MA transmutation efficiency of the EFIT (European Facility for Industrial Transmutation) core are presented. In the adopted strategy of MA burning the plutonium (Pu) balance of the core is minimized, allowing a reduction in the reactivity swing and the peak power form-factor deviation and an extension of the cycle duration. The MA/Pu ratio is used as a variable for the fuel optimisation studies. The efficiency of MA transmutation is close to the foreseen theoretical value of 42 kg TW -1 h -1 when level of Pu in the actinide mixture is about 40 wt.%. The obtained results are compared with the reference case of the EFIT core loaded with the composite CERCER fuel, where fuel particles are incorporated in a ceramic magnesia matrix. The results of this study offer additional information for the EFIT fuel selection.

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

Analysis of plutonium isotope ratios including 238Pu/239Pu in individual U-Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MS.

PubMed

Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

2017-04-01

Isotope ratio analysis of individual uranium-plutonium (U-Pu) mixed oxide particles contained within environmental samples taken from nuclear facilities is proving to be increasingly important in the field of nuclear safeguards. However, isobaric interferences, such as 238 U with 238 Pu and 241 Am with 241 Pu, make it difficult to determine plutonium isotope ratios in mass spectrometric measurements. In the present study, the isotope ratios of 238 Pu/ 239 Pu, 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of plutonium with UTEVA resins. Furthermore, 238 Pu/ 239 Pu isotope ratios were able to be calculated by using both the 238 Pu/( 239 Pu+ 240 Pu) activity ratios that had been measured through alpha spectrometry and the 240 Pu/ 239 Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including 238 Pu/ 239 Pu, in individual U-Pu mixed oxide particles. Copyright © 2016 Elsevier B.V. All rights reserved.

Light Water Reactor Sustainability Program A Reference Plan for Control Room Modernization: Planning and Analysis Phase

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

Jacques Hugo; Ronald Boring; Lew Hanes

2013-09-01

The U.S. Department of Energy’s Light Water Reactor Sustainability (LWRS) program is collaborating with a U.S. nuclear utility to bring about a systematic fleet-wide control room modernization. To facilitate this upgrade, a new distributed control system (DCS) is being introduced into the control rooms of these plants. The DCS will upgrade the legacy plant process computer and emergency response facility information system. In addition, the DCS will replace an existing analog turbine control system with a display-based system. With technology upgrades comes the opportunity to improve the overall human-system interaction between the operators and the control room. To optimize operatormore » performance, the LWRS Control Room Modernization research team followed a human-centered approach published by the U.S. Nuclear Regulatory Commission. NUREG-0711, Rev. 3, Human Factors Engineering Program Review Model (O’Hara et al., 2012), prescribes four phases for human factors engineering. This report provides examples of the first phase, Planning and Analysis. The three elements of Planning and Analysis in NUREG-0711 that are most crucial to initiating control room upgrades are: • Operating Experience Review: Identifies opportunities for improvement in the existing system and provides lessons learned from implemented systems. • Function Analysis and Allocation: Identifies which functions at the plant may be optimally handled by the DCS vs. the operators. • Task Analysis: Identifies how tasks might be optimized for the operators. Each of these elements is covered in a separate chapter. Examples are drawn from workshops with reactor operators that were conducted at the LWRS Human System Simulation Laboratory HSSL and at the respective plants. The findings in this report represent generalized accounts of more detailed proprietary reports produced for the utility for each plant. The goal of this LWRS report is to disseminate the technique and provide examples sufficient to serve as a template for other utilities’ projects for control room modernization.« less

In situ high temperature X-Ray diffraction study of the phase equilibria in the UO2-PuO2-Pu2O3 system

NASA Astrophysics Data System (ADS)

Belin, Renaud C.; Strach, Michal; Truphémus, Thibaut; Guéneau, Christine; Richaud, Jean-Christophe; Rogez, Jacques

2015-10-01

The region of the U-Pu-O phase diagram delimited by the compounds UO2-PuO2-Pu2O3 is known to exhibit a miscibility gap at low temperature. Consequently, MOX fuels with a composition entering this region could decompose into two fluorite phases and thus exhibit chemical heterogeneities. The experimental data on this domain found in the literature are scarce and usually provided using DTA that is not suitable for the investigation of such decomposition phenomena. In the present work, new experimental data, i.e. crystallographic phases, lattice parameters, phase fractions and temperature of phase separation, were measured in the composition range 0.14 < Pu/(U + Pu) < 0.62 and 1.85 < O/(U + Pu) < 2 from 298 to 1750 K using a novel in situ high temperature X-ray diffraction apparatus. A very good agreement is found between the temperature of phase separation determined from our results and using the thermodynamic model of the U-Pu-O system based on the CALPHAD method. Also, the combined use of thermodynamic calculations and XRD results refinement proved helpful in the determination of the O/M ratio of the samples during cooling. The methodology used in the current work might be useful to investigate other oxides systems exhibiting a miscibility gap.

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.

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

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.

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.

Preliminary fabrication and characterisation of inert matrix and thoria fuels for plutonium disposition in light water reactors

NASA Astrophysics Data System (ADS)

Vettraino, F.; Magnani, G.; La Torretta, T.; Marmo, E.; Coelli, S.; Luzzi, L.; Ossi, P.; Zappa, G.

1999-08-01

The plutonium disposition is presently acknowledged as a most urgent issue at the world level. Inert matrix and thoria fuel concepts for Pu burning in LWRs show good potential in providing effective and ultimate solutions to this issue. In non-fertile (U-free) inert matrix fuel, plutonium oxide is diluted within inert oxides such as stabilised ZrO 2, Al 2O 3, MgO or MgAl 2O 4. Thoria addition, which helps improve neutronic characteristics of inert fuels, appears as a promising variant of U-free fuel. In the context of an R&D activity aimed at assessing the feasibility of the fuel concept above, simulated fuel pellets have been produced both from dry-powder metallurgy and the sol-gel route. Results show that they can be fabricated by matching basic nuclear grade specifications such as the required geometry, density and microstructure. Some characterisation testing dealing with thermo-physical properties, ion irradiation damage and solubility also have been started. Results from thermo-physical measurements at room temperature have been achieved. A main feature stemming from solubility testing outcomes is a very high chemical stability which should render the fuel strongly diversion resistant and suitable for direct final disposal in deep geological repository (once-through solution).

Electronic and thermodynamic properties of α-Pu2O3

NASA Astrophysics Data System (ADS)

Lu, Yong; Yang, Yu; Zheng, Fawei; Zhang, Ping

2014-08-01

Based on density functional theory+U calculations and the quasi-annealing simulation method, we obtain the ground electronic state for α-Pu2O3 and present its phonon dispersion curves as well as various thermodynamic properties, which have seldom been theoretically studied because of the huge unit cell. We find that the Pu-O chemical bonding is weaker in α-Pu2O3 than in fluorite PuO2, and subsequently a frequency gap appears between oxygen and plutonium vibration density of states. Based on the calculated Helmholtz free energies at different temperatures, we further study the reaction energies for Pu oxidation, PuO2 reduction, and transformation between PuO2 and α-Pu2O3. Our reaction energy results are in agreements with available experiment. And it is revealed that high temperature and insufficient oxygen environment are in favor of the formation of α-Pu2O3.

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.

Plutonium age dating reloaded

NASA Astrophysics Data System (ADS)

Sturm, Monika; Richter, Stephan; Aregbe, Yetunde; Wellum, Roger; Mayer, Klaus; Prohaska, Thomas

2014-05-01

Although the age determination of plutonium is and has been a pillar of nuclear forensic investigations for many years, additional research in the field of plutonium age dating is still needed and leads to new insights as the present work shows: Plutonium is commonly dated with the help of the 241Pu/241Am chronometer using gamma spectrometry; in fewer cases the 240Pu/236U chronometer has been used. The age dating results of the 239Pu/235U chronometer and the 238Pu/234U chronometer are scarcely applied in addition to the 240Pu/236U chronometer, although their results can be obtained simultaneously from the same mass spectrometric experiments as the age dating result of latter. The reliability of the result can be tested when the results of different chronometers are compared. The 242Pu/238U chronometer is normally not evaluated at all due to its sensitivity to contamination with natural uranium. This apparent 'weakness' that renders the age dating results of the 242Pu/238U chronometer almost useless for nuclear forensic investigations, however turns out to be an advantage looked at from another perspective: the 242Pu/238U chronometer can be utilized as an indicator for uranium contamination of plutonium samples and even help to identify the nature of this contamination. To illustrate this the age dating results of all four Pu/U clocks mentioned above are discussed for one plutonium sample (NBS 946) that shows no signs of uranium contamination and for three additional plutonium samples. In case the 242Pu/238U chronometer results in an older 'age' than the other Pu/U chronometers, contamination with either a small amount of enriched or with natural or depleted uranium is for example possible. If the age dating result of the 239Pu/235U chronometer is also influenced the nature of the contamination can be identified; enriched uranium is in this latter case a likely cause for the missmatch of the age dating results of the Pu/U chronometers.

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%.

U, Pu, and Am nuclear signatures of the Thule hydrogen bomb debris.

PubMed

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

2008-07-01

This study concerns an arctic marine environment that was contaminated by actinide elements after a nuclear accident in 1968, the so-called Thule accident In this study we have analyzed five isolated hot particles as well as sediment samples containing particles from the weapon material for the determination of the nuclear fingerprint of the accident. We report that the fissile material in the hydrogen weapons involved in the Thule accident was a mixture of highly enriched uranium and weapon-grade plutonium and that the main fissile material was 235U (about 4 times more than the mass of 239Pu). In the five hot particles examined, the measured uranium atomic ratio was 235U/238U = 1.02 +/- 0.16 and the Pu-isotopic ratios were as follows: 24Pu/239Pu = 0.0551 +/- 0.0008 (atom ratio), 238Pu/239+240Pu = 0.0161 +/- 0.0005 (activity ratio), 241Pu/239+240Pu = 0.87 +/- 0.12 (activity ratio), and 241Am/ 239+240Pu = 0.169 +/- 0.005 (activity ratio) (reference date 2001-10-01). From the activity ratios of 241Pu/241Am, we estimated the time of production of this weapon material to be from the late 1950s to the early 1960s. The results from reanalyzed bulk sediment samples showed the presence of more than one Pu source involved in the accident, confirming earlier studies. The 238Pu/239+240PU activity ratio and the 240Pu/ 239Pu atomic ratio were divided into at least two Pu-isotopic ratio groups. For both Pu-isotopic ratios, one ratio group had identical ratios as the five hot particles described above and for the other groups the Pu isotopic ratios were lower (238Pu/ 239+240PU activity ratio approximately 0.01 and the 240Pu/P239Pu atomic ratio 0.03). On the studied particles we observed that the U/Pu ratio decreased as a function of the time these particles were present in the sediment. We hypothesis that the decrease in the ratio is due to a preferential leaching of U relative to Pu from the particle matrix.

Thermodynamic assessments and inter-relationships between systems involving Al, Am, Ga, Pu, and U

NASA Astrophysics Data System (ADS)

Perron, A.; Turchi, P. E. A.; Landa, A.; Oudot, B.; Ravat, B.; Delaunay, F.

2016-12-01

A newly developed self-consistent CALPHAD thermodynamic database involving Al, Am, Ga, Pu, and U is presented. A first optimization of the slightly characterized Am-Al and completely unknown Am-Ga phase diagrams is proposed. To this end, phase diagram features as crystal structures, stoichiometric compounds, solubility limits, and melting temperatures have been studied along the U-Al → Pu-Al → Am-Al, and U-Ga → Pu-Ga → Am-Ga series, and the thermodynamic assessments involving Al and Ga alloying are compared. In addition, two distinct optimizations of the Pu-Al phase diagram are proposed to account for the low temperature and Pu-rich region controversy. The previously assessed thermodynamics of the other binary systems (Am-Pu, Am-U, Pu-U, and Al-Ga) is also included in the database and is briefly described in the present work. Finally, predictions on phase stability of ternary and quaternary systems of interest are reported to check the consistency of the database.

Thermodynamic assessments and inter-relationships between systems involving Al, Am, Ga, Pu, and U

DOE PAGES

Perron, A.; Turchi, P. E. A.; Landa, A.; ...

2016-12-01

We present a newly developed self-consistent CALPHAD thermodynamic database involving Al, Am, Ga, Pu, and U. A first optimization of the slightly characterized Am-Al and completely unknown Am-Ga phase diagrams is proposed. To this end, phase diagram features as crystal structures, stoichiometric compounds, solubility limits, and melting temperatures have been studied along the U-Al → Pu-Al → Am-Al, and U-Ga → Pu-Ga → Am-Ga series, and the thermodynamic assessments involving Al and Ga alloying are compared. In addition, two distinct optimizations of the Pu-Al phase diagram are proposed to account for the low temperature and Pu-rich region controversy. We includedmore » the previously assessed thermodynamics of the other binary systems (Am-Pu, Am-U, Pu-U, and Al-Ga) in the database and is briefly described in the present work. In conclusion, predictions on phase stability of ternary and quaternary systems of interest are reported to check the consistency of the database.« less

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

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).

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.

Oxygen diffusion model of the mixed (U,Pu)O2 ± x: Assessment and application

NASA Astrophysics Data System (ADS)

Moore, Emily; Guéneau, Christine; Crocombette, Jean-Paul

2017-03-01

The uranium-plutonium (U,Pu)O2 ± x mixed oxide (MOX) is used as a nuclear fuel in some light water reactors and considered for future reactor generations. To gain insight into fuel restructuring, which occurs during the fuel lifetime as well as possible accident scenarios understanding of the thermodynamic and kinetic behavior is crucial. A comprehensive evaluation of thermo-kinetic properties is incorporated in a computational CALPHAD type model. The present DICTRA based model describes oxygen diffusion across the whole range of plutonium, uranium and oxygen compositions and temperatures by incorporating vacancy and interstitial migration pathways for oxygen. The self and chemical diffusion coefficients are assessed for the binary UO2 ± x and PuO2 - x systems and the description is extended to the ternary mixed oxide (U,Pu)O2 ± x by extrapolation. A simulation to validate the applicability of this model is considered.

Caustic Precipitation of Plutonium and Uranium with Gadolinium as a Neutron Poison

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

VISSER, ANN E.; BRONIKOWSKI, MICHAEL G.; RUDISILL, TRACY S.

2005-10-18

The caustic precipitation of plutonium (Pu) and uranium (U) from Pu and U-containing waste solutions has been investigated to determine whether gadolinium (Gd) could be used as a neutron poison for precipitation with greater than a fissile mass containing both Pu and enriched U. Precipitation experiments were performed using both process solution samples and simulant solutions with a range of 2.6-5.16 g/L U and 0-4.3:1 U:Pu. Analyses were performed on solutions at intermediate pH to determine the partitioning of elements for accident scenarios. When both Pu and U were present in the solution, precipitation began at pH 4.5 and bymore » pH 7, 99% of Pu and U had precipitated. When complete neutralization was achieved at pH > 14 with 1.2 M excess OH{sup -}, greater than 99% of Pu, U, and Gd had precipitated. At pH > 14, the particles sizes were larger and the distribution was a single mode. The ratio of hydrogen:fissile atoms in the precipitate was determined after both settling and centrifuging and indicates that sufficient water was associated with the precipitates to provide the needed neutron moderation for Gd to prevent a criticality in solutions containing up to 4.3:1 U:Pu and up to 5.16 g/L U.« less

Caustic Precipitation of Plutonium and Uranium with Gadolinium as a Neutron Poison

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

ANN, VISSER

2005-04-14

The caustic precipitation of plutonium (Pu) and uranium (U) from Pu and U containing waste solutions has been investigated to determine whether gadolinium (Gd) could be used as a neutron poison for precipitation with greater than a fissile mass containing both Pu and enriched U. Precipitation experiments were performed using both actual samples and simulant solutions with a range of 2.6-5.16 g/L U and 0-4.3 to 1 U to Pu. Analyses were performed on solutions at intermediate pH to determine the partitioning of elements for accident scenarios. When both Pu and U were present in the solution, precipitation began atmore » pH 4.5 and by pH 7, 99 percent of Pu and U had precipitated. When complete neutralization was achieved at pH greater than 14 with 1.2 M excess OH-, greater than 99 percent of Pu, U, and Gd had precipitated. At pH greater than 14, the particles sizes were larger and the distribution was a single mode. The ratio of hydrogen to fissile atoms in the precipitate was determined after both settling and centrifuging and indicates that sufficient water was associated with the precipitates to provide the needed neutron moderation for Gd to prevent a criticality in solutions containing up to 4.3 to 1 U to Pu and up to 5.16 g/L U.« less

Chronology of Pu isotopes and 236U in an Arctic ice core.

PubMed

Wendel, C C; Oughton, D H; Lind, O C; Skipperud, L; Fifield, L K; Isaksson, E; Tims, S G; Salbu, B

2013-09-01

In the present work, state of the art isotopic fingerprinting techniques are applied to an Arctic ice core in order to quantify deposition of U and Pu, and to identify possible tropospheric transport of debris from former Soviet Union test sites Semipalatinsk (Central Asia) and Novaya Zemlya (Arctic Ocean). An ice core chronology of (236)U, (239)Pu, and (240)Pu concentrations, and atom ratios, measured by accelerator mass spectrometry in a 28.6m deep ice core from the Austfonna glacier at Nordaustlandet, Svalbard is presented. The ice core chronology corresponds to the period 1949 to 1999. The main sources of Pu and (236)U contamination in the Arctic were the atmospheric nuclear detonations in the period 1945 to 1980, as global fallout, and tropospheric fallout from the former Soviet Union test sites Novaya Zemlya and Semipalatinsk. Activity concentrations of (239+240)Pu ranged from 0.008 to 0.254 mBq cm(-2) and (236)U from 0.0039 to 0.053 μBq cm(-2). Concentrations varied in concordance with (137)Cs concentrations in the same ice core. In contrast to previous published results, the concentrations of Pu and (236)U were found to be higher at depths corresponding to the pre-moratorium period (1949 to 1959) than to the post-moratorium period (1961 and 1962). The (240)Pu/(239)Pu ratio ranged from 0.15 to 0.19, and (236)U/(239)Pu ranged from 0.18 to 1.4. The Pu atom ratios ranged within the limits of global fallout in the most intensive period of nuclear atmospheric testing (1952 to 1962). To the best knowledge of the authors the present work is the first publication on biogeochemical cycles with respect to (236)U concentrations and (236)U/(239)Pu atom ratios in the Arctic and in ice cores. Copyright © 2013 Elsevier B.V. All rights reserved.

A new Mantle Source Tapped During Episode 55 of the Pu'u O'o Eruption From Kilauea Volcano

NASA Astrophysics Data System (ADS)

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

2005-12-01

Over 22 years of continuous geochemical monitoring of lavas from the current Pu'u O'o eruption allows us to probe the mantle and crustal processes beneath Kilauea Volcano in unparalleled detail. Episode 55 (1997-present) marks the longest and most voluminous Pu'u O'o eruptive interval. Here we present new Pb, Sr, and Nd isotopic ratios and major- and trace-element abundances for the most recent lavas (1999-2005). MgO variation diagrams show that most of the major-element variations are related to olivine fractionation. However, Pu'u O'o lavas display longer-term systematic decreases in their TiO2, K2O, P2O5 and CaO abundances (at a given MgO) due to changes in the parental magma composition. Incompatible element ratios (K2O/TiO2, Nb/Y, Nb/Zr) and MgO-normalized abundances (Sr, Rb, K) in episode 55 lavas delimit the lowest values observed during the Pu'u O'o eruption. Earlier Pu'u O'o lavas displayed a temporal decrease in highly over moderately incompatible trace-element ratios, near constant SiO2 contents, and a gradual increase in 87Sr/86Sr. However, episode 55 lavas (between days 5500-6500) record an increase in MgO-normalized SiO2 contents and even higher 87Sr/86Sr with near constant incompatible trace-element ratios. Neither a single mantle source composition nor a change in partial melting conditions can explain these observations. Based on 226Ra-230Th-238U disequilibria and partial melting modeling of trace elements, we conclude that Pu'u O'o lavas originate from at least two distinct mantle source components: (1) a recently depleted component that was subsequently remelted to explain the overall decreases of incompatible major- and trace-element ratios and abundances, and (2) a compositionally and isotopically distinct mantle component that was not previously melted within the Hawaiian plume to explain the temporal increase in 87Sr/86Sr and SiO2 abundances and the flattening trend of incompatible trace-element ratios. This second 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. These results can be explained by a recent (1999) change in the size or location of Pu'u O'o's melting region, which allowed this new source to be tapped.

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.

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

LWRS ATR Irradiation Testing Readiness Status

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

Kristine Barrett

2012-09-01

The Light Water Reactor Sustainability (LWRS) Program was established by the U.S. Department of Energy Office of Nuclear Energy (DOE-NE) to develop technologies and other solutions that can improve the reliability, sustain the safety, and extend the life of the current reactors. The LWRS Program is divided into four R&D Pathways: (1) Materials Aging and Degradation; (2) Advanced Light Water Reactor Nuclear Fuels; (3) Advanced Instrumentation, Information and Control Systems; and (4) Risk-Informed Safety Margin Characterization. This report describes an irradiation testing readiness analysis in preparation of LWRS experiments for irradiation testing at the Idaho National Laboratory (INL) Advanced Testmore » Reactor (ATR) under Pathway (2). The focus of the Advanced LWR Nuclear Fuels Pathway is to improve the scientific knowledge basis for understanding and predicting fundamental performance of advanced nuclear fuel and cladding in nuclear power plants during both nominal and off-nominal conditions. This information will be applied in the design and development of high-performance, high burn-up fuels with improved safety, cladding integrity, and improved nuclear fuel cycle economics« less

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.

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.

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

Andersson, Anders David Ragnar; Stanek, Christopher Richard; Noordhoek, Mark

Uranium silicides, in particular U 3Si 2, are being explored as an advanced nuclear fuel with increased accident tolerance as well as competitive economics compared to the baseline UO 2 fuel. They benefit from high thermal conductivity (metallic) compared to UO 2 fuel (insulator or semi-conductor) used in current Light Water Reactors (LWRs). The U-Si fuels also have higher fissile density. In order to perform meaningful engineering scale nuclear fuel performance simulations, the material properties of the fuel, including the response to irradiation environments, must be known. Unfortunately, the data available for USi fuels are rather limited, in particular formore » the temperature range where LWRs would operate. The ATF HIP is using multi-scale modeling and simulations to address this knowledge gap.« less

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

Andersson, Anders David Ragnar; Stanek, Christopher Richard; Noordhoek, Mark J.

Uranium silicides, in particular U 3Si 2, are being explored as an advanced nuclear fuel with increased accident tolerance as well as competitive economics compared to the baseline UO2 fuel. They benefit from high thermal conductivity (metallic) compared to UO 2 fuel (insulator or semi-conductor) used in current Light Water Reactors (LWRs). The U-Si fuels also have higher fissile density. In order to perform meaningful engineering scale nuclear fuel performance simulations, the material properties of the fuel, including the response to irradiation environments, must be known. Unfortunately, the data available for USi fuels are rather limited, in particular for themore » temperature range where LWRs would operate. The ATF HIP is using multi-scale modeling and simulations to address this knowledge gap.« less

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.

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.

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.

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.

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

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.

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

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

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.

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.

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

Opportunities for the Multi Recycling of Used MOX Fuel in the US - 12122

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

Murray, P.; Bailly, F.; Bouvier, E.

Over the last 50 years the US has accumulated an inventory of used nuclear fuel (UNF) in the region of 64,000 metric tons in 2010, and adds an additional 2,200 metric tons each year from the current fleet of 104 Light Water Reactors. This paper considers a fuel cycle option that would be available for a future pilot U.S. recycling plant that could take advantage of the unique opportunities offered by the age and size of the large U.S. UNF inventory. For the purpose of this scenario, recycling of UNF must use the available reactor infrastructure, currently LWR's, and themore » main product of recycling is considered to be plutonium (Pu), recycled into MOX fuel for use in these reactors. Use of MOX fuels must provide the service (burn-up) expected by the reactor operator, with the required level of safety. To do so, the fissile material concentration (Pu-239, Pu-241) in the MOX must be high enough to maintain criticality, while, in current recycle facilities, the Pu-238 content has to be kept low enough to prevent excessive heat load, neutron emission, and neutron capture during recycle operations. In most countries, used MOX fuel (MOX UNF) is typically stored after one irradiation in an LWR, pending the development of the GEN IV reactors, since it is considered difficult to directly reuse the recycled MOX fuel in LWRs due to the degraded Pu fissile isotopic composition. In the US, it is possible to blend MOX UNF with LEUOx UNF from the large inventory, using the oldest UNF first. Blending at the ratio of about one MOX UNF assembly with 15 LEUOx UNF assemblies, would achieve a fissile plutonium concentration sufficient for reirradiation in new MOX fuel. The Pu-238 yield in the new fuel will be sufficiently low to meet current fuel fabrication standards. Therefore, it should be possible in the context of the US, for discharged MOX fuel to be recycled back into LWR's, using only technologies already industrially deployed worldwide. Building on that possibility, two scenarios are assessed where current US inventory is treated; Pu recycled in LWR MOX fuels, and used MOX fuels themselves are treated in a continuous partitioning-transmutation mode (case 2a) or until the whole current UNF inventory (64,000 MT in 2010) has been treated followed by disposal of the MOX UNF to a geologic repository (case 2b). In the recycling scenario, two cases (2a and 2b) are considered. Benefits achieved are compared with the once through scenario (case 1) where UNF in the current US inventory are disposed directly to a geologic repository. For each scenario, the heat load and radioactivity of the high activity wastes disposed to a geologic repository are calculated and the savings in natural resources quantified, and compared with the once-through fuel cycle. Assuming an initial pilot recycling facility with a capacity of 800 metric tons a year of heavy metal begins operation in 2030, ∼8 metric tons per year of Pu is recovered from the LEUOx UNF inventory, and is used to produce fresh MOX fuels. At a later time, additional treatment and recycling capacities are assumed to begin operation, to accommodate blending and recycling of used MOX Pu, up to 2,400 MT/yr treatment capacity to enable processing UNF slightly faster than the rate of generation. Results of this scenario analysis study show the flexibility of the recycling scenarios so that Pu is managed in a way that avoids accumulating used MOX fuels. If at some future date, the decision is made to dispose of the MOX UNF to a geologic repository (case 2b), the scenario is neutral to final repository heat load in comparison to the direct disposal of all UNF (case 1), while diminishing use of natural uranium, enrichment, UNF accumulation, and the volume of HLW. Further recycling of Pu at the end of the scenario (case 2a) would exhibit further benefits. As expected, Pu-241 and Am-241 are the source of long term HLW heat load and Am-241 and Np-237 are the source of long term radiotoxicity. When advanced technology is available, introduction of minor actinide recycling, in addition to Pu recycling, by the end of this scenario, or sooner, would have a major impact on final repository heat load and long term radiotoxicity of the HLW. This scenario is also compatible with a gradual introduction of a small number of FR's for Pu management. (authors)« less

Chemical thermodynamic representation of (U, Pu, Am)O 2- x

NASA Astrophysics Data System (ADS)

Osaka, Masahiko; Namekawa, Takashi; Kurosaki, Ken; Yamanaka, Shinsuke

2005-09-01

The oxygen potential isotherms of (U, Pu, Am)O 2- x were represented by a chemical thermodynamic model proposed by Lindemer et al. It was assumed in the present model that (U, Pu, Am)O 2- x consisted of the chemical species [UO 2], [PuO 2], [Pu 4/3O 2], [AmO 2] and [Am 5/4O 2] in a pseudo-quaternary system by treating the reduction rates of Pu and Am as identical; furthermore an interaction between [Am 5/4O 2] and [UO 2] was introduced. The agreement between analytical and experimental isotherms was good, but the analytical values slightly overestimated the experimental values especially in the case of lower Am content. Adding an interaction between [Am 5/4O 2] and [PuO 2] to the model resulted in a better representation.

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.

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.

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

Generic repository design concepts and thermal analysis (FY11).

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

Howard, Robert; Dupont, Mark; Blink, James A.

2011-08-01

Reference concepts for geologic disposal of used nuclear fuel and high-level radioactive waste in the U.S. are developed, including geologic settings and engineered barriers. Repository thermal analysis is demonstrated for a range of waste types from projected future, advanced nuclear fuel cycles. The results show significant differences among geologic media considered (clay/shale, crystalline rock, salt), and also that waste package size and waste loading must be limited to meet targeted maximum temperature values. In this study, the UFD R&D Campaign has developed a set of reference geologic disposal concepts for a range of waste types that could potentially be generatedmore » in advanced nuclear FCs. A disposal concept consists of three components: waste inventory, geologic setting, and concept of operations. Mature repository concepts have been developed in other countries for disposal of spent LWR fuel and HLW from reprocessing UNF, and these serve as starting points for developing this set. Additional design details and EBS concepts will be considered as the reference disposal concepts evolve. The waste inventory considered in this study includes: (1) direct disposal of SNF from the LWR fleet, including Gen III+ advanced LWRs being developed through the Nuclear Power 2010 Program, operating in a once-through cycle; (2) waste generated from reprocessing of LWR UOX UNF to recover U and Pu, and subsequent direct disposal of used Pu-MOX fuel (also used in LWRs) in a modified-open cycle; and (3) waste generated by continuous recycling of metal fuel from fast reactors operating in a TRU burner configuration, with additional TRU material input supplied from reprocessing of LWR UOX fuel. The geologic setting provides the natural barriers, and establishes the boundary conditions for performance of engineered barriers. The composition and physical properties of the host medium dictate design and construction approaches, and determine hydrologic and thermal responses of the disposal system. Clay/shale, salt, and crystalline rock media are selected as the basis for reference mined geologic disposal concepts in this study, consistent with advanced international repository programs, and previous investigations in the U.S. The U.S. pursued deep geologic disposal programs in crystalline rock, shale, salt, and volcanic rock in the years leading up to the Nuclear Waste Policy Act, or NWPA (Rechard et al. 2011). The 1987 NWPA amendment act focused the U.S. program on unsaturated, volcanic rock at the Yucca Mountain site, culminating in the 2008 license application. Additional work on unsaturated, crystalline rock settings (e.g., volcanic tuff) is not required to support this generic study. Reference disposal concepts are selected for the media listed above and for deep borehole disposal, drawing from recent work in the U.S. and internationally. The main features of the repository concepts are discussed in Section 4.5 and summarized in Table ES-1. Temperature histories at the waste package surface and a specified distance into the host rock are calculated for combinations of waste types and reference disposal concepts, specifying waste package emplacement modes. Target maximum waste package surface temperatures are identified, enabling a sensitivity study to inform the tradeoff between the quantity of waste per disposal package, and decay storage duration, with respect to peak temperature at the waste package surface. For surface storage duration on the order of 100 years or less, waste package sizes for direct disposal of SNF are effectively limited to 4-PWR configurations (or equivalent size and output). Thermal results are summarized, along with recommendations for follow-on work including adding additional reference concepts, verification and uncertainty analysis for thermal calculations, developing descriptions of surface facilities and other system details, and cost estimation to support system-level evaluations.« less

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.

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

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.

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

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.

Th/U-233 multi-recycle in pressurized water reactors : feasibility study of multiple homogeneous and heterogeneous assembly designs.

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

Yun, D.; Taiwo, T. A.; Kim, T. K.

2010-10-01

The use of thorium in current or advanced light water reactors (LWRs) has been of interest in recent years. These interests have been associated with the need to increase nuclear fuel resources and the perceived non-proliferation advantages of the utilization of thorium in the fuel cycle. Various options have been considered for the use of thorium in the LWR fuel cycle. The possibility for thorium utilization in a multi-recycle system has also been considered in past literature, primarily because of the potential for near breeders with Th/U-233 in the thermal energy range. The objective of this study is to evaluatemore » the potential of Th/U-233 fuel multi-recycle in current LWRs, focusing on pressurized water reactors (PWRs). Approaches for sustainable multi-recycle without the need for external fissile material makeup have been investigated. The intent is to obtain a design that allows existing PWRs to be used with minimal modifications.« less

PRELIMINARY EVALUATION OF FeCrAl CLADDING AND U-Si FUEL FOR ACCIDENT TOLERANT FUEL CONCEPTS

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

Hales, J. D.; Gamble, K. A.

2015-09-01

Since the accident at the Fukushima Daiichi Nuclear Power Station, enhancing the accident tolerance of light water reactors (LWRs) has become an important research topic. In particular, the community is actively developing enhanced fuels and cladding for LWRs to improve safety in the event of accidents in the reactor or spent fuel pools. Fuels with enhanced accident tolerance are those that, in comparison with the standard UO2-zirconium alloy system, can tolerate loss of active cooling in the reactor core for a considerably longer time period during design-basis and beyond design-basis events while maintaining or improving the fuel performance during normalmore » operations and operational transients. This paper presents early work in developing thermal and mechanical models for two materials that may have promise: U-Si for fuel, and FeCrAl for cladding. These materials would not necessarily be used together in the same fuel system, but individually have promising characteristics. BISON, the finite element-based fuel performance code in development at Idaho National Laboratory, was used to compare results from normal operation conditions with Zr-4/UO2 behavior. In addition, sensitivity studies are presented for evaluating the relative importance of material parameters such as ductility and thermal conductivity in FeCrAl and U-Si in order to provide guidance on future experiments for these materials.« less

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.

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

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.

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.

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.

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

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.

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).

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

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

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.

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.

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.

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.)

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

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

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.

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.

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.

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.

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.

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

Thomas, Kenneth; Oxstrand, Johanna

The Digital Architecture effort is a part of the Department of Energy (DOE) sponsored Light-Water Reactor Sustainability (LWRS) Program conducted at Idaho National Laboratory (INL). The LWRS program is performed in close collaboration with industry research and development (R&D) programs that provides the technical foundations for licensing and managing the long-term, safe, and economical operation of current nuclear power plants (NPPs). One of the primary missions of the LWRS program is to help the U.S. nuclear industry adopt new technologies and engineering solutions that facilitate the continued safe operation of the plants and extension of the current operating licenses. Therefore,more » a major objective of the LWRS program is the development of a seamless digital environment for plant operations and support by integrating information from plant systems with plant processes for nuclear workers through an array of interconnected technologies. In order to get the most benefits of the advanced technology suggested by the different research activities in the LWRS program, the nuclear utilities need a digital architecture in place to support the technology. A digital architecture can be defined as a collection of information technology (IT) capabilities needed to support and integrate a wide-spectrum of real-time digital capabilities for nuclear power plant performance improvements. It is not hard to imagine that many processes within the plant can be largely improved from both a system and human performance perspective by utilizing a plant wide (or near plant wide) wireless network. For example, a plant wide wireless network allows for real time plant status information to easily be accessed in the control room, field workers’ computer-based procedures can be updated based on the real time plant status, and status on ongoing procedures can be incorporated into smart schedules in the outage command center to allow for more accurate planning of critical tasks. The goal of the digital architecture project is to provide a long-term strategy to integrate plant systems, plant processes, and plant workers. This include technologies to improve nuclear worker efficiency and human performance; to offset a range of plant surveillance and testing activities with new on-line monitoring technologies; improve command, control, and collaboration in settings such as outage control centers and work execution centers; and finally to improve operator performance with new operator aid technologies for the control room. The requirements identified through the activities in the Digital Architecture project will be used to estimate the amount of traffic on the network and hence estimating the minimal bandwidth needed.« less

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.

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.

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).

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.

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

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)

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.

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.

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

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}.

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.

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

Feasibility study of a fission-suppressed Tokamak fusion breeder

NASA Astrophysics Data System (ADS)

Moir, R. W.; Lee, J. D.; Neef, W. S., Jr.; Berwald, D. H.; Garner, J. K.; Whitley, R. H.; Ghoniem, N.; Wong, C. P. C.; Maya, I.; Schultz, K. R.

1984-12-01

The preliminary conceptual design of a tokama fissile fuel producer is described. The blanket technology is based on the fission suppressed breeding concept where neutron multiplication occurs in a bed of 2 cm diameter beryllium pebbles which are cooled by helium at 50 atmospheres pressure. Uranium-233 is bred in thorium metal fuel elements which are in the form of snap rings attached to each beryllium pebble. Tritium is bred in lithium bearing material contained in tubes immersed in the pebble bed and is recovered by a purge flow of helium. The neutron wall load is 3 MW/m(2) and the blanket material is ferritic steel. The net fissile breeding ratio is 0.54 plus or minus 30% per fusion reaction. This results in the production of 4900 kg of (223)U per year from 3000 MW of fusion power. This quantity of fuel will provide makeup fuel for about 12 LWRs of equal thermal power or about 18 1 GW sub e LWRs. The calculated cost of the produced uranium-233 is between $23/g and $53/g or equivalent to $10/kg to $90/kg of U308 depending on government financing or utility financing assumptions. Additional topics discussed include the Tokamak operating mode (both steady state and long pulse considered), the design and breeding implications of using a poloidal divertor for impurity control, reactor safety, the choice of a tritium breeder, and fuel management.

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

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

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

Simulated Fission Gas Behavior in Silicide Fuel at LWR Conditions

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

Miao, Yinbin; Mo, Kun; Yacout, Abdellatif

As a promising candidate for the accident tolerant fuel (ATF) used in light water reactors (LWRs), the fuel performance of uranium silicide (U 3Si 2) at LWR conditions needs to be well-understood. However, existing experimental post-irradiation examination (PIE) data are limited to the research reactor conditions, which involve lower fuel temperature compared to LWR conditions. This lack of appropriate experimental data significantly affects the development of fuel performance codes that can precisely predict the microstructure evolution and property degradation at LWR conditions, and therefore evaluate the qualification of U 3Si 2 as an AFT for LWRs. Considering the high cost,more » long timescale, and restrictive access of the in-pile irradiation experiments, this study aims to utilize ion irradiation to simulate the inpile behavior of the U 3Si 2 fuel. Both in situ TEM ion irradiation and ex situ high-energy ATLAS ion irradiation experiments were employed to simulate different types of microstructure modifications in U 3Si 2. Multiple PIE techniques were used or will be used to quantitatively analyze the microstructure evolution induced by ion irradiation so as to provide valuable reference for the development of fuel performance code prior to the availability of the in-pile irradiation data.« less

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

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

Proof-of-Concept Demonstrations for Computation-Based Human Reliability Analysis. Modeling Operator Performance During Flooding Scenarios

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

Joe, Jeffrey Clark; Boring, Ronald Laurids; Herberger, Sarah Elizabeth Marie

The United States (U.S.) Department of Energy (DOE) Light Water Reactor Sustainability (LWRS) program has the overall objective to help sustain the existing commercial nuclear power plants (NPPs). To accomplish this program objective, there are multiple LWRS “pathways,” or research and development (R&D) focus areas. One LWRS focus area is called the Risk-Informed Safety Margin and Characterization (RISMC) pathway. Initial efforts under this pathway to combine probabilistic and plant multi-physics models to quantify safety margins and support business decisions also included HRA, but in a somewhat simplified manner. HRA experts at Idaho National Laboratory (INL) have been collaborating with othermore » experts to develop a computational HRA approach, called the Human Unimodel for Nuclear Technology to Enhance Reliability (HUNTER), for inclusion into the RISMC framework. The basic premise of this research is to leverage applicable computational techniques, namely simulation and modeling, to develop and then, using RAVEN as a controller, seamlessly integrate virtual operator models (HUNTER) with 1) the dynamic computational MOOSE runtime environment that includes a full-scope plant model, and 2) the RISMC framework PRA models already in use. The HUNTER computational HRA approach is a hybrid approach that leverages past work from cognitive psychology, human performance modeling, and HRA, but it is also a significant departure from existing static and even dynamic HRA methods. This report is divided into five chapters that cover the development of an external flooding event test case and associated statistical modeling considerations.« less

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.

Using the Human Systems Simulation Laboratory at Idaho National Laboratory for Safety Focused Research

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

Joe, Jeffrey .C; Boring, Ronald L.

Under the United States (U.S.) Department of Energy (DOE) Light Water Reactor Sustainability (LWRS) program, researchers at Idaho National Laboratory (INL) have been using the Human Systems Simulation Laboratory (HSSL) to conduct critical safety focused Human Factors research and development (R&D) for the nuclear industry. The LWRS program has the overall objective to develop the scientific basis to extend existing nuclear power plant (NPP) operating life beyond the current 60-year licensing period and to ensure their long-term reliability, productivity, safety, and security. One focus area for LWRS is the NPP main control room (MCR), because many of the instrumentation andmore » control (I&C) system technologies installed in the MCR, while highly reliable and safe, are now difficult to replace and are therefore limiting the operating life of the NPP. This paper describes how INL researchers use the HSSL to conduct Human Factors R&D on modernizing or upgrading these I&C systems in a step-wise manner, and how the HSSL has addressed a significant gap in how to upgrade systems and technologies that are built to last, and therefore require careful integration of analog and new advanced digital technologies.« 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

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).

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.

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

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.

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.

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.

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.

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.

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.

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.

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.

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.

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.

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

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).

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

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.

A REVIEW OF HUMAN-SYSTEM INTERFACE DESIGN ISSUES OBSERVED DURING ANALOG-TO-DIGITAL AND DIGITAL-TO-DIGITAL MIGRATIONS IN U.S. NUCLEAR POWER PLANTS

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

Kovesdi, C.; Joe, J.

The United States (U.S.) Department of Energy (DOE) Light Water Reactor Sustainability (LWRS) program is developing a scientific basis through targeted research and development (R&D) to support the U.S. nuclear power plant (NPP) fleet in extending their existing licensing period and ensuring their long-term reliability, productivity, safety, and security. Over the last several years, human factors engineering (HFE) professionals at the Idaho National Laboratory (INL) have supported the LWRS Advanced Instrumentation, Information, and Control (II&C) System Technologies pathway across several U.S. commercial NPPs in analog-to-digital migrations (i.e., turbine control systems) and digital-to-digital migrations (i.e., Safety Parameter Display System). These effortsmore » have included in-depth human factors evaluation of proposed human-system interface (HSI) design concepts against established U.S. Nuclear Regulatory Commission (NRC) design guidelines from NUREG-0700, Rev 2 to inform subsequent HSI design prior to transitioning into Verification and Validation. This paper discusses some of the overarching design issues observed from these past HFE evaluations. In addition, this work presents some observed challenges such as common tradeoffs utilities are likely to face when introducing new HSI technologies into NPP hybrid control rooms. The primary purpose of this work is to distill these observed design issues into general HSI design guidance that industry can use in early stages of HSI design.« less

A Research Roadmap for Computation-Based Human Reliability Analysis

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

Boring, Ronald; Mandelli, Diego; Joe, Jeffrey

2015-08-01

The United States (U.S.) Department of Energy (DOE) is sponsoring research through the Light Water Reactor Sustainability (LWRS) program to extend the life of the currently operating fleet of commercial nuclear power plants. The Risk Informed Safety Margin Characterization (RISMC) research pathway within LWRS looks at ways to maintain and improve the safety margins of these plants. The RISMC pathway includes significant developments in the area of thermalhydraulics code modeling and the development of tools to facilitate dynamic probabilistic risk assessment (PRA). PRA is primarily concerned with the risk of hardware systems at the plant; yet, hardware reliability is oftenmore » secondary in overall risk significance to human errors that can trigger or compound undesirable events at the plant. This report highlights ongoing efforts to develop a computation-based approach to human reliability analysis (HRA). This computation-based approach differs from existing static and dynamic HRA approaches in that it: (i) interfaces with a dynamic computation engine that includes a full scope plant model, and (ii) interfaces with a PRA software toolset. The computation-based HRA approach presented in this report is called the Human Unimodels for Nuclear Technology to Enhance Reliability (HUNTER) and incorporates in a hybrid fashion elements of existing HRA methods to interface with new computational tools developed under the RISMC pathway. The goal of this research effort is to model human performance more accurately than existing approaches, thereby minimizing modeling uncertainty found in current plant risk models.« less

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

Environmental Effect on Evolutionary Cyclic Plasticity Material Parameters of 316 Stainless Steel: An Experimental & Material Modeling Approach

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

Mohanty, Subhasish; Soppet, William K.; Majumdar, Saurin

2014-09-20

This report provides an update on an earlier assessment of environmentally assisted fatigue for light water reactor (LWR) materials under extended service conditions. This report is a deliverable under the work package for environmentally assisted fatigue in the Light Water Reactor Sustainability (LWRS) program. The overall objective of this LWRS project is to assess the degradation by environmentally assisted cracking/fatigue of LWR materials such as various alloy base metals and their welds used in reactor coolant system piping. This effort is to support the Department of Energy LWRS program for developing tools to understand the aging/failure mechanism and to predictmore » the remaining life of LWR components for anticipated 60-80 year operation.« less

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

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).

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.

Migration of Older to New Digital Control Systems in Nuclear Power Plant Main Control Rooms

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

Kovesdi, Casey Robert; Joe, Jeffrey Clark

The United States (U.S.) Department of Energy (DOE) Office of Nuclear Energy (NE) has the primary mission to advance nuclear power by resolving socio-technical issues through research and development (R&D). One DOE-NE activity supporting this mission is the Light Water Reactor Sustainability (LWRS) program. LWRS has the overall objective to sustain the operation of existing commercial nuclear power plants (NPPs) through conducting R&D across multiple “pathways,” or R&D focus areas. The Advanced Instrumentation, Information, and Control (II&C) Systems Technologies pathway conducts targeted R&D to address aging and reliability concerns with the legacy instrumentation and control (I&C) and related information systemsmore » in operating U.S. NPPs. This work involves (1) ensuring that legacy analog II&C systems are not life-limiting issues for the LWR fleet, and (2) implementing digital II&C technology in a manner that enables broad innovation and business improvement in the NPP operating model. Under the LWRS Advanced II&C pathway, Human Factors experts at Idaho National Laboratory (INL) have been conducting R&D in support of NPP main control room (MCR) modernization activities. Work in prior years has focused on migrating analog I&C systems to new digital I&C systems (). In fiscal year 2016 (FY16), one new focus area for this research is migrating older digital I&C systems to new and advanced digital I&C systems. This report summarizes a plan for conducting a digital-to-digital migration of a legacy digital I&C system to a new digital I&C system in support of control room modernization activities.« less

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).

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.

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).

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.

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.

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.;

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.

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.

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

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

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.

Gaseous swelling of U 3 Si 2 during steady-state LWR operation: A rate theory investigation

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

Miao, Yinbin; Gamble, Kyle A.; Andersson, David

Rate theory simulations of fission gas behavior in U 3Si 2 are reported for light water reactor (LWR) steady-state operation scenarios. We developed a model of U 3Si 2 and implemented into the GRASS-SST code based on available research reactor post-irradiation examination (PIE) data, and density functional theory (DFT) calculations of key material properties. Simplified peripheral models were also introduced to capture the fuel-cladding interaction. The simulations identified three regimes of U 3Si 2 swelling behavior between 390 K and 1190 K. Under typical steady-state LWR operating conditions where U 3Si 2 temperature is expected to be below 1000 K,more » intragranular bubbles are dominant and fission gas is retained in those bubbles. The consequent gaseous swelling is low and associated degradation in the fuel thermal conductivity is also limited. Those predictions of U 3Si 2 performance during steady-state operations in LWRs suggest that this fuel material is an appropriate LWR candidate fuel material. Fission gas behavior models established based on this work are being coupled to the thermo-mechanical simulation of the fuel behavior using the BISON fuel performance multi-dimensional finite element code.« less

Gaseous swelling of U 3 Si 2 during steady-state LWR operation: A rate theory investigation

DOE PAGES

Miao, Yinbin; Gamble, Kyle A.; Andersson, David; ...

2017-07-25

Rate theory simulations of fission gas behavior in U 3Si 2 are reported for light water reactor (LWR) steady-state operation scenarios. We developed a model of U 3Si 2 and implemented into the GRASS-SST code based on available research reactor post-irradiation examination (PIE) data, and density functional theory (DFT) calculations of key material properties. Simplified peripheral models were also introduced to capture the fuel-cladding interaction. The simulations identified three regimes of U 3Si 2 swelling behavior between 390 K and 1190 K. Under typical steady-state LWR operating conditions where U 3Si 2 temperature is expected to be below 1000 K,more » intragranular bubbles are dominant and fission gas is retained in those bubbles. The consequent gaseous swelling is low and associated degradation in the fuel thermal conductivity is also limited. Those predictions of U 3Si 2 performance during steady-state operations in LWRs suggest that this fuel material is an appropriate LWR candidate fuel material. Fission gas behavior models established based on this work are being coupled to the thermo-mechanical simulation of the fuel behavior using the BISON fuel performance multi-dimensional finite element code.« 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

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 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.

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

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

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.

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

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.

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.

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.

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

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.

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

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.

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.

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.

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.

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

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.

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.

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

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%).

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.

Overview of NRC Proactive Management of Materials Degradation (PMMD) Program

NASA Astrophysics Data System (ADS)

Carpenter, C. E. Gene; Hull, Amy; Oberson, Greg

Materials degradation phenomena, if not appropriately managed, have the potential to adversely impact the design functionality and safety margins of nuclear power plant (NPP) systems, structures and components (SSCs). Therefore, the U.S. Nuclear Regulatory Commission (NRC) has initiated an over-the-horizon multi-year research Proactive Management of Materials Degradation (PMMD) Research Program, which is presently evaluating longer time frames (i.e., 80 or more years) and including passive long-lived SSCs beyond the primary piping and core internals, such as concrete containment and cable insulation. This will allow the NRC to (1) identify significant knowledge gaps and new forms of degradation; (2) capture current knowledge base; and, (3) prioritize materials degradation research needs and directions for future efforts. This effort is being accomplished in collaboration with the U.S. Department of Energy's (DOE) LWR Sustainability (LWRS) program. This presentation will discuss the activities to date, including results, and the path forward.

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.

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.

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.

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.

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.

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.

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.

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.

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.

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.

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.

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

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

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

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.

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.

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.

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.

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.

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

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.

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.

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.

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)

Yang, Ying

Radiation-induced segregation (RIS) has been frequently reported in structural materials such as austenitic, ferritic, and ferritic-martensitic stainless steels (SS) that have been widely used in light water reactors (LWRs). RIS has been linked to secondary degradation effects in SS including irradiation-induced stress corrosion cracking (IASCC). Earlier studies on thermal segregation in Fe-based alloys found that metalloids elements such as P, S, Si, Ge, Sn, etc., embrittle the materials when enrichment was observed at grain boundaries (GBs). RIS of Fe-Cr-Ni-based austenitic steels has been modeled in the U.S. 2015 fiscal year (FY2015), which identified the pre-enrichment due to thermal segregation canmore » have an important role on the subsequent RIS. The goal of this work is to develop thermal segregation models for alloying elements in steels for future integration with RIS modeling.« less

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.

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.

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

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

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.

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.

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.

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.

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

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.

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

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

Cyber security evaluation of II&C technologies

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

Thomas, Ken

The Light Water Reactor Sustainability (LWRS) Program is a research and development program sponsored by the Department of Energy, which is conducted in close collaboration with industry to provide the technical foundations for licensing and managing the long-term, safe and economical operation of current nuclear power plants The LWRS Program serves to help the US nuclear industry adopt new technologies and engineering solutions that facilitate the continued safe operation of the plants and extension of the current operating licenses. Within the LWRS Program, the Advanced Instrumentation, Information, and Control (II&C) Systems Technologies Pathway conducts targeted research and development (R&D) tomore » address aging and reliability concerns with the legacy instrumentation and control and related information systems of the U.S. operating light water reactor (LWR) fleet. The II&C Pathway is conducted by Idaho National Laboratory (INL). Cyber security is a common concern among nuclear utilities and other nuclear industry stakeholders regarding the digital technologies that are being developed under this program. This concern extends to the point of calling into question whether these types of technologies could ever be deployed in nuclear plants given the possibility that the information in them can be compromised and the technologies themselves can potentially be exploited to serve as attack vectors for adversaries. To this end, a cyber security evaluation has been conducted of these technologies to determine whether they constitute a threat beyond what the nuclear plants already manage within their regulatory-required cyber security programs. Specifically, the evaluation is based on NEI 08-09, which is the industry’s template for cyber security programs and evaluations, accepted by the Nuclear Regulatory Commission (NRC) as responsive to the requirements of the nuclear power plant cyber security regulation found in 10 CFR 73.54. The evaluation was conducted by a cyber security team with expertise in nuclear utility cyber security programs and experience in conducting these evaluations. The evaluation has determined that, for the most part, cyber security will not be a limiting factor in the application of these technologies to nuclear power plant applications.« 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.

Proposed Activities to Address Regulatory Gaps and Challenges for Licensing Advanced Reactors Using Seismic Isolation

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

Coleman, Justin Leigh; Kammerer, Annie M.; Whittaker, Andrew S.

Over the last decade, particularly since implementation of the certified design regulatory approaches outlined in 10 CFR 52, “Licenses, Certifications, and Approvals for Nuclear Power Plants,” interest has been increasing in the use of seismic isolation (SI) technology to support seismic safety in nuclear facilities. In 2009, the United States (U.S.) Nuclear Regulatory Commission (NRC) initiated research activities to develop new guidance targeted at isolated facilities because SI is being considered for nuclear power plants in the U.S. One product of that research, which was developed around a risk-informed regulatory approach, is a draft NRC NUREG series (NUREG/CR) report thatmore » investigates and discusses considerations for use of SI in otherwise traditionally founded large light water reactors (LWRs). A coordinated effort led to new provisions for SI of LWRs in the American Society of Civil Engineers standard ASCE/SEI 4-16, “Seismic Analysis of Safety Related Nuclear Structures.” The risk-informed design philosophy that underpinned development of the technical basis for these documents led to a set of proposed performance objectives and acceptance criteria intended to serve as the foundation for future NRC guidance on the use of SI and related technology. Although the guidance provided in the draft SI NUREG/CR report and ASCE/SEI 4 16 provides a sound basis for further development of nuclear power plant designs incorporating SI, these initial documents were focused on surface-founded or near-surface-founded LWRs and were, necessarily, limited in scope. For example, there is limited information in both the draft NUREG/CR report and ASCE/SEI 4-16 related to nonlinear analysis of soil-structure systems for deeply-embedded reactors, the isolation of components, and the use of vertical isolation systems. Also not included in the draft SI NUREG/CR report are special considerations for licensing of isolated facilities using the certified design approach in 10 CFR 52 and a detailed discussion of seismic probabilistic risk assessments for isolated facilities.« 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.

Transuranic inventory reduction in repository by partitioning and transmutation

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

Kang, C.H.; Kazimi, M.S.

1992-01-01

The promise of a new reprocessing technology and the issuance of Environmental Protection Agency (EPA) and U.S. Nuclear Regulatory Commission regulations concerning a geologic repository rekindle the interest in partitioning and transmutation of transuranic (TRU) elements from discharged reactor fuel as a high level waste management option. This paper investigates the TRU repository inventory reduction capability of the proposed advanced liquid metal reactors (ALMRs) and integral fast reactors (IFRs) as well as the plutonium recycled light water reactors (LWRs).

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).

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.

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.

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.

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

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.

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

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

Metrics for the technical performance evaluation of light water reactor accident-tolerant fuel

DOE PAGES

Bragg-Sitton, Shannon M.; Todosow, Michael; Montgomery, Robert; ...

2017-03-26

The safe, reliable, and economic operation of the nation’s nuclear power reactor fleet has always been a top priority for the nuclear industry. Continual improvement of technology, including advanced materials and nuclear fuels, remains central to the industry’s success. Enhancing the accident tolerance of light water reactors (LWRs) became a topic of serious discussion following the 2011 Great East Japan Earthquake, resulting tsunami, and subsequent damage to the Fukushima Daiichi nuclear power plant complex. The overall goal for the development of accident-tolerant fuel (ATF) for LWRs is to identify alternative fuel system technologies to further enhance the safety, competitiveness, andmore » economics of commercial nuclear power. Designed for use in the current fleet of commercial LWRs or in reactor concepts with design certifications (GEN-III+), fuels with enhanced accident tolerance would endure loss of active cooling in the reactor core for a considerably longer period of time than the current fuel system while maintaining or improving performance during normal operations. The complex multiphysics behavior of LWR nuclear fuel in the integrated reactor system makes defining specific material or design improvements difficult; as such, establishing desirable performance attributes is critical in guiding the design and development of fuels and cladding with enhanced accident tolerance. Research and development of ATF in the United States is conducted under the U.S. Department of Energy (DOE) Fuel Cycle Research and Development Advanced Fuels Campaign. The DOE is sponsoring multiple teams to develop ATF concepts within multiple national laboratories, universities, and the nuclear industry. Concepts under investigation offer both evolutionary and revolutionary changes to the current nuclear fuel system. This study summarizes the technical evaluation methodology proposed in the United States to aid in the optimization and prioritization of candidate ATF designs.« 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

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.

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

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

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.

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.

Rate Theory Modeling and Simulation of Silicide Fuel at LWR Conditions

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

Miao, Yinbin; Ye, Bei; Hofman, Gerard

As a promising candidate for the accident tolerant fuel (ATF) used in light water reactors (LWRs), the fuel performance of uranium silicide (U 3Si 2) at LWR conditions needs to be well understood. In this report, rate theory model was developed based on existing experimental data and density functional theory (DFT) calculations so as to predict the fission gas behavior in U 3Si 2 at LWR conditions. The fission gas behavior of U 3Si 2 can be divided into three temperature regimes. During steady-state operation, the majority of the fission gas stays in intragranular bubbles, whereas the dominance of intergranularmore » bubbles and fission gas release only occurs beyond 1000 K. The steady-state rate theory model was also used as reference to establish a gaseous swelling correlation of U 3Si 2 for the BISON code. Meanwhile, the overpressurized bubble model was also developed so that the fission gas behavior at LOCA can be simulated. LOCA simulation showed that intragranular bubbles are still dominant after a 70 second LOCA, resulting in a controllable gaseous swelling. The fission gas behavior of U 3Si 2 at LWR conditions is benign according to the rate theory prediction at both steady-state and LOCA conditions, which provides important references to the qualification of U 3Si 2 as a LWR fuel material with excellent fuel performance and enhanced accident tolerance.« less

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°).

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.

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

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.

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.

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.

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.

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.

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.

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.

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.

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

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

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.

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.

Computer Based Procedures for Field Workers - FY16 Research Activities

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

Oxstrand, Johanna; Bly, Aaron

The Computer-Based Procedure (CBP) research effort is a part of the Light-Water Reactor Sustainability (LWRS) Program, which provides the technical foundations for licensing and managing the long-term, safe, and economical operation of current nuclear power plants. One of the primary missions of the LWRS program is to help the U.S. nuclear industry adopt new technologies and engineering solutions that facilitate the continued safe operation of the plants and extension of the current operating licenses. One area that could yield tremendous savings in increased efficiency and safety is in improving procedure use. A CBP provides the opportunity to incorporate context-driven jobmore » aids, such as drawings, photos, and just-in-time training. The presentation of information in CBPs can be much more flexible and tailored to the task, actual plant condition, and operation mode. The dynamic presentation of the procedure will guide the user down the path of relevant steps, thus minimizing time spent by the field worker to evaluate plant conditions and decisions related to the applicability of each step. This dynamic presentation of the procedure also minimizes the risk of conducting steps out of order and/or incorrectly assessed applicability of steps. This report provides a summary of the main research activities conducted in the Computer-Based Procedures for Field Workers effort since 2012. The main focus of the report is on the research activities conducted in fiscal year 2016. The activities discussed are the Nuclear Electronic Work Packages – Enterprise Requirements initiative, the development of a design guidance for CBPs (which compiles all insights gained through the years of CBP research), the facilitation of vendor studies at the Idaho National Laboratory (INL) Advanced Test Reactor (ATR), a pilot study for how to enhance the plant design modification work process, the collection of feedback from a field evaluation study at Plant Vogtle, and path forward to commercialize INL’s CBP system.« less

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.

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

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.

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).

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.

A HUMAN FACTORS ENGINEERING PROCESS TO SUPPORT HUMAN-SYSTEM INTERFACE DESIGN IN CONTROL ROOM MODERNIZATION

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

Kovesdi, C.; Joe, J.; Boring, R.

The primary objective of the United States (U.S.) Department of Energy (DOE) Light Water Reactor Sustainability (LWRS) program is to sustain operation of the existing commercial nuclear power plants (NPPs) through a multi-pathway approach in conducting research and development (R&D). The Advanced Instrumentation, Information, and Control (II&C) System Technologies pathway conducts targeted R&D to address aging and reliability concerns with legacy instrumentation and control (I&C) and other information systems in existing U.S. NPPs. Control room modernization is an important part following this pathway, and human factors experts at Idaho National Laboratory (INL) have been involved in conducting R&D to supportmore » migration of new digital main control room (MCR) technologies from legacy analog and legacy digital I&C. This paper describes a human factors engineering (HFE) process that supports human-system interface (HSI) design in MCR modernization activities, particularly with migration of old digital to new digital I&C. The process described in this work is an expansion from the LWRS Report INL/EXT-16-38576, and is a requirements-driven approach that aligns with NUREG-0711 requirements. The work described builds upon the existing literature by adding more detail around key tasks and decisions to make when transitioning from HSI Design into Verification and Validation (V&V). The overall objective of this process is to inform HSI design and elicit specific, measurable, and achievable human factors criteria for new digital technologies. Upon following this process, utilities should have greater confidence with transitioning from HSI design into V&V.« less

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.

System analysis with improved thermo-mechanical fuel rod models for modeling current and advanced LWR materials in accident scenarios

NASA Astrophysics Data System (ADS)

Porter, Ian Edward

A nuclear reactor systems code has the ability to model the system response in an accident scenario based on known initial conditions at the onset of the transient. However, there has been a tendency for these codes to lack the detailed thermo-mechanical fuel rod response models needed for accurate prediction of fuel rod failure. This proposed work will couple today's most widely used steady-state (FRAPCON) and transient (FRAPTRAN) fuel rod models with a systems code TRACE for best-estimate modeling of system response in accident scenarios such as a loss of coolant accident (LOCA). In doing so, code modifications will be made to model gamma heating in LWRs during steady-state and accident conditions and to improve fuel rod thermal/mechanical analysis by allowing axial nodalization of burnup-dependent phenomena such as swelling, cladding creep and oxidation. With the ability to model both burnup-dependent parameters and transient fuel rod response, a fuel dispersal study will be conducted using a hypothetical accident scenario under both PWR and BWR conditions to determine the amount of fuel dispersed under varying conditions. Due to the fuel fragmentation size and internal rod pressure both being dependent on burnup, this analysis will be conducted at beginning, middle and end of cycle to examine the effects that cycle time can play on fuel rod failure and dispersal. Current fuel rod and system codes used by the Nuclear Regulatory Commission (NRC) are compilations of legacy codes with only commonly used light water reactor materials, Uranium Dioxide (UO2), Mixed Oxide (U/PuO 2) and zirconium alloys. However, the events at Fukushima Daiichi and Three Mile Island accident have shown the need for exploration into advanced materials possessing improved accident tolerance. This work looks to further modify the NRC codes to include silicon carbide (SiC), an advanced cladding material proposed by current DOE funded research on accident tolerant fuels (ATF). Several additional fuels will also be analyzed, including uranium nitride (UN), uranium carbide (UC) and uranium silicide (U3Si2). Focusing on the system response in an accident scenario, an emphasis is placed on the fracture mechanics of the ceramic cladding by design the fuel rods to eliminate pellet cladding mechanical interaction (PCMI). The time to failure and how much of the fuel in the reactor fails with an advanced fuel design will be analyzed and compared to the current UO2/Zircaloy design using a full scale reactor model.

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.

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.

The Complete Burning of Weapons Grade Plutonium and Highly Enriched Uranium with (Laser Inertial Fusion-Fission Energy) LIFE Engine

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

Farmer, J C; Diaz de la Rubia, T; Moses, E

2008-12-23

The National Ignition Facility (NIF) project, a laser-based Inertial Confinement Fusion (ICF) experiment designed to achieve thermonuclear fusion ignition and burn in the laboratory, is under construction at the Lawrence Livermore National Laboratory (LLNL) and will be completed in April of 2009. Experiments designed to accomplish the NIF's goal will commence in late FY2010 utilizing laser energies of 1 to 1.3 MJ. Fusion yields of the order of 10 to 20 MJ are expected soon thereafter. Laser initiated fusion-fission (LIFE) engines have now been designed to produce nuclear power from natural or depleted uranium without isotopic enrichment, and from spentmore » nuclear fuel from light water reactors without chemical separation into weapons-attractive actinide streams. A point-source of high-energy neutrons produced by laser-generated, thermonuclear fusion within a target is used to achieve ultra-deep burn-up of the fertile or fissile fuel in a sub-critical fission blanket. Fertile fuels including depleted uranium (DU), natural uranium (NatU), spent nuclear fuel (SNF), and thorium (Th) can be used. Fissile fuels such as low-enrichment uranium (LEU), excess weapons plutonium (WG-Pu), and excess highly-enriched uranium (HEU) may be used as well. Based upon preliminary analyses, it is believed that LIFE could help meet worldwide electricity needs in a safe and sustainable manner, while drastically shrinking the nation's and world's stockpile of spent nuclear fuel and excess weapons materials. LIFE takes advantage of the significant advances in laser-based inertial confinement fusion that are taking place at the NIF at LLNL where it is expected that thermonuclear ignition will be achieved in the 2010-2011 timeframe. Starting from as little as 300 to 500 MW of fusion power, a single LIFE engine will be able to generate 2000 to 3000 MWt in steady state for periods of years to decades, depending on the nuclear fuel and engine configuration. Because the fission blanket in a fusion-fission hybrid system is subcritical, a LIFE engine can burn any fertile or fissile nuclear material, including unenriched natural or depleted U and SNF, and can extract a very high percentage of the energy content of its fuel resulting in greatly enhanced energy generation per metric ton of nuclear fuel, as well as nuclear waste forms with vastly reduced concentrations of long-lived actinides. LIFE engines could thus provide the ability to generate vast amounts of electricity while greatly reducing the actinide content of any existing or future nuclear waste and extending the availability of low cost nuclear fuels for several thousand years. LIFE also provides an attractive pathway for burning excess weapons Pu to over 99% FIMA (fission of initial metal atoms) without the need for fabricating or reprocessing mixed oxide fuels (MOX). Because of all of these advantages, LIFE engines offer a pathway toward sustainable and safe nuclear power that significantly mitigates nuclear proliferation concerns and minimizes nuclear waste. An important aspect of a LIFE engine is the fact that there is no need to extract the fission fuel from the fission blanket before it is burned to the desired final level. Except for fuel inspection and maintenance process times, the nuclear fuel is always within the core of the reactor and no weapons-attractive materials are available outside at any point in time. However, an important consideration when discussing proliferation concerns associated with any nuclear fuel cycle is the ease with which reactor fuel can be converted to weapons usable materials, not just when it is extracted as waste, but at any point in the fuel cycle. Although the nuclear fuel remains in the core of the engine until ultra deep actinide burn up is achieved, soon after start up of the engine, once the system breeds up to full power, several tons of fissile material is present in the fission blanket. However, this fissile material is widely dispersed in millions of fuel pebbles, which can be tagged as individual accountable items, and thus made difficult to divert in large quantities. This report discusses the application of the LIFE concept to nonproliferation issues, initially looking at the LIFE (Laser Inertial Fusion-Fission Energy) engine as a means of completely burning WG Pu and HEU. By combining a neutron-rich inertial fusion point source with energy-rich fission, the once-through closed fuel-cycle LIFE concept has the following characteristics: it is capable of efficiently burning excess weapons or separated civilian plutonium and highly enriched uranium; the fission blanket is sub-critical at all times (keff < 0.95); because LIFE can operate well beyond the point at which light water reactors (LWRs) need to be refueled due to burn-up of fissile material and the resulting drop in system reactivity, fuel burn-up of 99% or more appears feasible. The objective of this work is to develop LIFE technology for burning of WG-Pu and HEU.« less

User guidelines and best practices for CASL VUQ analysis using Dakota.

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

Adams, Brian M.; Swiler, Laura Painton; Hooper, Russell

2014-03-01

Sandia's Dakota software (available at http://dakota.sandia.gov) supports science and engineering transformation through advanced exploration of simulations. Specifically it manages and analyzes ensembles of simulations to provide broader and deeper perspective for analysts and decision makers. This enables them to enhance understanding of risk, improve products, and assess simulation credibility. This manual offers Consortium for Advanced Simulation of Light Water Reactors (LWRs) (CASL) partners a guide to conducting Dakota-based VUQ studies for CASL problems. It motivates various classes of Dakota methods and includes examples of their use on representative application problems. On reading, a CASL analyst should understand why and howmore » to apply Dakota to a simulation problem. This SAND report constitutes the product of CASL milestone L3:VUQ.V&V.P8.01 and is also being released as a CASL unlimited release report with number CASL-U-2014-0038-000.« less

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.

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.

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.

Early implementation of SiC cladding fuel performance models in BISON

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

Powers, Jeffrey J.

2015-09-18

SiC-based ceramic matrix composites (CMCs) [5–8] are being developed and evaluated internationally as potential LWR cladding options. These development activities include interests within both the DOE-NE LWR Sustainability (LWRS) Program and the DOE-NE Advanced Fuels Campaign. The LWRS Program considers SiC ceramic matrix composites (CMCs) as offering potentially revolutionary gains as a cladding material, with possible benefits including more efficient normal operating conditions and higher safety margins under accident conditions [9]. Within the Advanced Fuels Campaign, SiC-based composites are a candidate ATF cladding material that could achieve several goals, such as reducing the rates of heat and hydrogen generation duemore » to lower cladding oxidation rates in HT steam [10]. This work focuses on the application of SiC cladding as an ATF cladding material in PWRs, but these work efforts also support the general development and assessment of SiC as an LWR cladding material in a much broader sense.« 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.

Bubble morphology in U 3Si 2 implanted by high-energy Xe ions at 300 °C

DOE PAGES

Miao, Yinbin; Harp, Jason; Mo, Kun; ...

2017-08-02

The microstructure modifications of a high-energy Xe implanted U 3Si 2, a promising accident tolerant fuel candidate, were characterized and are reported upon. The U 3Si 2 pellet was irradiated at Argonne Tandem Linac Accelerator System (ATLAS) by an 84 MeV Xe ion beam at 300 °C. The irradiated specimen was then investigated using a series of transmission electron microscopy (TEM) techniques. A dense distribution of bubbles were observed near the range of the 84 MeV Xe ions. Xe gas was also found to accumulate at multiple types of sinks, such as dislocations and grain boundaries. Bubbles aggregated at thosemore » sinks are slightly larger than intragranular bubbles in lattice. At 300 °C, the gaseous swelling strain is limited as all the bubbles are below 10 nm, implying the promising fission gas behavior of U 3Si 2 under normal operating conditions in light water reactors (LWRs).« less

Bubble morphology in U3Si2 implanted by high-energy Xe ions at 300 °C

NASA Astrophysics Data System (ADS)

Miao, Yinbin; Harp, Jason; Mo, Kun; Zhu, Shaofei; Yao, Tiankai; Lian, Jie; Yacout, Abdellatif M.

2017-11-01

The microstructure modifications of a high-energy Xe implanted U3Si2, a promising accident tolerant fuel candidate, were characterized and are reported upon. The U3Si2 pellet was irradiated at Argonne Tandem Linac Accelerator System (ATLAS) by an 84 MeV Xe ion beam at 300 °C. The irradiated specimen was then investigated using a series of transmission electron microscopy (TEM) techniques. A dense distribution of bubbles were observed near the range of the 84 MeV Xe ions. Xe gas was also found to accumulate at multiple types of sinks, such as dislocations and grain boundaries. Bubbles aggregated at those sinks are slightly larger than intragranular bubbles in lattice. At 300 °C, the gaseous swelling strain is limited as all the bubbles are below 10 nm, implying the promising fission gas behavior of U3Si2 under normal operating conditions in light water reactors (LWRs).

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

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

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

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

U.S. Department of Energy Accident Resistant SiC Clad Nuclear Fuel Development

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

George W. Griffith

2011-10-01

A significant effort is being placed on silicon carbide ceramic matrix composite (SiC CMC) nuclear fuel cladding by Light Water Reactor Sustainability (LWRS) Advanced Light Water Reactor Nuclear Fuels Pathway. The intent of this work is to invest in a high-risk, high-reward technology that can be introduced in a relatively short time. The LWRS goal is to demonstrate successful advanced fuels technology that suitable for commercial development to support nuclear relicensing. Ceramic matrix composites are an established non-nuclear technology that utilizes ceramic fibers embedded in a ceramic matrix. A thin interfacial layer between the fibers and the matrix allows formore » ductile behavior. The SiC CMC has relatively high strength at high reactor accident temperatures when compared to metallic cladding. SiC also has a very low chemical reactivity and doesn't react exothermically with the reactor cooling water. The radiation behavior of SiC has also been studied extensively as structural fusion system components. The SiC CMC technology is in the early stages of development and will need to mature before confidence in the developed designs can created. The advanced SiC CMC materials do offer the potential for greatly improved safety because of their high temperature strength, chemical stability and reduced hydrogen generation.« less

Seamless Digital Environment – Data Analytics Use Case Study

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

Oxstrand, Johanna

Multiple research efforts in the U.S Department of Energy Light Water Reactor Sustainability (LWRS) Program studies the need and design of an underlying architecture to support the increased amount and use of data in the nuclear power plant. More specifically the three LWRS research efforts; Digital Architecture for an Automated Plant, Automated Work Packages, Computer-Based Procedures for Field Workers, and the Online Monitoring efforts all have identified the need for a digital architecture and more importantly the need for a Seamless Digital Environment (SDE). A SDE provides a mean to access multiple applications, gather the data points needed, conduct themore » analysis requested, and present the result to the user with minimal or no effort by the user. During the 2016 annual Nuclear Information Technology Strategic Leadership (NITSL) group meeting the nuclear utilities identified the need for research focused on data analytics. The effort was to develop and evaluate use cases for data mining and analytics for employing information from plant sensors and database for use in developing improved business analytics. The goal of the study is to research potential approaches to building an analytics solution for equipment reliability, on a small scale, focusing on either a single piece of equipment or a single system. The analytics solution will likely consist of a data integration layer, predictive and machine learning layer and the user interface layer that will display the output of the analysis in a straight forward, easy to consume manner. This report describes the use case study initiated by NITSL and conducted in a collaboration between Idaho National Laboratory, Arizona Public Service – Palo Verde Nuclear Generating Station, and NextAxiom Inc.« less

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.

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.

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.

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.

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.

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

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.

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.

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EPA Pesticide Factsheets

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A HUMAN FACTORS META MODEL FOR U.S. NUCLEAR POWER PLANT CONTROL ROOM MODERNIZATION

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

Joe, Jeffrey C.

Over the last several years, the United States (U.S.) Department of Energy (DOE) has sponsored human factors research and development (R&D) and human factors engineering (HFE) activities through its Light Water Reactor Sustainability (LWRS) program to modernize the main control rooms (MCR) of commercial nuclear power plants (NPP). Idaho National Laboratory (INL), in partnership with numerous commercial nuclear utilities, has conducted some of this R&D to enable the life extension of NPPs (i.e., provide the technical basis for the long-term reliability, productivity, safety, and security of U.S. NPPs). From these activities performed to date, a human factors meta model formore » U.S. NPP control room modernization can now be formulated. This paper discusses this emergent HFE meta model for NPP control room modernization, with the goal of providing an integrated high level roadmap and guidance on how to perform human factors R&D and HFE for those in the U.S. nuclear industry that are engaging in the process of upgrading their MCRs.« less

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.

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.

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

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.

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

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.

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.

Length-weight relationship of eleven species of marine catfishes from the northern Arabian Sea coast of Pakistan

NASA Astrophysics Data System (ADS)

Farooq, Noureen; Qamar, Nazia; Rashid, Shahnaz; Panhwar, Sher Khan

2017-09-01

This study records length-weight relationships (LWRs) for eleven commercially important marine catfish species of the family Ariidae (sea catfishes) and Plotosidae (eel catfishes) from the northern Arabian Sea coast of Pakistan. The specimens were sampled from December 2014 to November 2015, using bottom trawls with various mesh sizes by commercial vessels. The species were Nemapteryx caelatus, Sciades sona, Arius gagora, Batrachocephalus mino, Netuma thalassina, N. bilineata, Osteogeneiosus militaris, Plicofollis dussumieri, P. tenuispinis, Plotosus limbatus, and P. lineatus. Of the eleven species, two species A. gagora and N. bilineata were recorded for the first time and LWRs for four species A. gagora, N. bilineata, S. sona, and B. mino still have no data in the FishBase database. In addition, new maximum length for each of the three species N. bilineata, O. militaris and B. mino was also found.

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.

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.

Stress Concentrations.

DTIC Science & Technology

1982-09-01

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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.

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

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

[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].

Infrasonic tremor observed at Kilauea Volcano, Hawaii'i

USGS Publications Warehouse

Garces, M.; Harris, A.; Hetzer, C.; Johnson, J.; Rowland, S.; Marchetti, E.; Okubo, P.

2003-01-01

Infrasonic array data collected at Ki??lauea Volcano, Hawai'i, during November 12-21, 2002 indicate that the active vents and lava tube system near the P'u 'O??'o?? vent complex emit almost continuous infrasound in the 0.310 Hz frequency band. The spectral content of these infrasonic signals matches well that of synchronous seismic tremor. In sites protected from wind noise, significant signal to noise ratios were recorded as far as ???13 km from the crater of Pu'u 'O??'o??. The infrasonic recordings suggest that one or more tremor sources may be close to the surface. In addition, these results demonstrate that adequate site and instrument selections for infrasonic arrays are essential in order to obtain consistent and reliable infrasonic detections. ?? 2003 by the American Geophysical Union.

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.

Shallow magma system of Kilauea volcano investigated using L-band synthetic aperture radar data

NASA Astrophysics Data System (ADS)

Fukushima, Y.; Sinnett, D. K.; Segall, P.

2009-12-01

L-band synthetic aperture radar (SAR) images on Kilauea volcano have been archived by Japanese JERS-1 (1992-1998) and ALOS (2006-) satellites. L-band interferometric SAR (InSAR) can measure displacements in a broader region compared to C-band, thanks to higher phase coherence on vegetated areas. We made InSAR analyses on Kilauea using the following L-band data sets: J1) two JERS-1 images, acquired on 20 Oct. 1992 and 1 Mar. 1993 from a descending orbit (RSP path 589) with off-nadir angle of 34.3 degrees, J2) three JERS-1 images, acquired between 8 Oct. 1993 and 3 Jul. 1997 from a descending orbit (RSP path 590) with off-nadir angle of 34.3 degrees, A1) 13 ALOS images, acquired between 24 Jun. 2006 and 14 Feb. 2009 from an ascending orbit with off-nadir angle 9.9 degrees, and A2) 11 ALOS images, acquired between 21 May 2006 and 26 Feb. 2009 from a descending orbit with off-nadir angle 9.9 degrees. One-second SRTM digital elevation data were used to remove the topographic phase. The interferogram of the data set J1 contains signals of 1) a maximum of about 30 cm of range decrease resulting from a dike intrusion in the Makaopuhi crater area, 2) about 10 cm of maximum range increase in the Pu`u `O`o crater area, and 3) a few cm of range increase along the East Rift Zone (ERZ) between the summit and Pu`u `O`o craters. An interferogram (8 Oct. 1993 - 3 Jul. 1997) of the data set J2 indicates 1) range increase (maximum 7 cm/yr) in both the summit and Pu`u `O`o areas, 2) range increase (maximum 5 cm/yr) along the ERZ between the summit and Makaopuhi crater, and 3) range decrease (maximum 6cm/yr) on the southern flank near the coast that is consistent with a seaward movement of the southern flank. A small baseline subset InSAR time-series analysis was performed using all the images of the data sets A1 and A2, assuming that the data acquisitions had been made in pure vertical direction. The analysis period includes the 2007 Father's day dike intrusion. A preliminary result indicates the followings. Pre-eruption period (9 months): 12 cm/yr of uplift in an area of a few km SW of the summit caldera and 3 cm/yr of subsidence along the ERZ between the summit and Napau craters. Co-eruption period (7 months): 15 cm of subsidence in the summit crater and a few tens of cm of uplift associated with the diking. Post-eruption period (17 months): more than 2 cm/yr of subsidence in the summit area and at least 1 cm/yr of subsidence in the Pu`u `O`o area, where the spatial extensions of the two subsiding areas are comparable. While the obtained subsidence signals can be attributed to lava compactions and to artifacts due to errors in the digital elevation model, our results may indicate a developed shallow magma reservoir under the Pu`u `O`o crater, and also smaller shallow reservoirs distributed along the ERZ between the summit and Pu`u `O`o.

A Comparison of ACQ, AIE and AEE-Based Polymers Loaded on Polyurethane Foams as Sensors for Explosives Detection.

PubMed

Chu, Zhiwei; Fan, Zhuxin; Zhang, Xiang; Tan, Xiaofeng; Li, Dongxu; Chen, Guohua; Zhao, Qinghua

2018-05-15

An aggregation-caused quenching (ACQ)-active polymer (PF), an aggregation-induced emission (AIE)-active polymer (PFTPE) and an aggregation-enhanced emission (AEE)-active polymer (PTTPE) were synthesized by tetraphenylethane (TPE), fluorene and thiophene moieties. Polyurethane (PU) foams modified by PF, PFTPE and PTTPE, namely PU-PF, PU-PFTPE and PU-PTTPE, using ultrasonication-assisted method have been prepared. A comparative study of PU-PF, PU-PFTPE and PU-PTTPE for detection explosives had been performed, and significant fluorescence quenching was observed with the introduction of PA solutions. The as-prepared PU-PF, PU-PFTPE and PU-PTTPE sensors exhibited a superior sensitivity for PA solutions with different concentrations. Remarkably, PU-PF gave a quenching efficiency of 96.2%, higher than 93.5% for PU-PFTPE and 86.7% for PU-PTTPE at a PA concentration of 180 µg·mL -1 in methanol, which was attributed to the effective energy transfer from the fluorophore (PF) to the nitro explosive (PA). This suggested that some ACQ polymers, applied to detect explosives, could afford better performances than AIE or AEE polymers through modification of structures and selection of adequate carriers. At the same time, these chemical sensors can be recycled many times.

A Comparison of ACQ, AIE and AEE-Based Polymers Loaded on Polyurethane Foams as Sensors for Explosives Detection

PubMed Central

Chu, Zhiwei; Fan, Zhuxin; Zhang, Xiang; Tan, Xiaofeng; Chen, Guohua; Zhao, Qinghua

2018-01-01

An aggregation-caused quenching (ACQ)-active polymer (PF), an aggregation-induced emission (AIE)-active polymer (PFTPE) and an aggregation-enhanced emission (AEE)-active polymer (PTTPE) were synthesized by tetraphenylethane (TPE), fluorene and thiophene moieties. Polyurethane (PU) foams modified by PF, PFTPE and PTTPE, namely PU-PF, PU-PFTPE and PU-PTTPE, using ultrasonication-assisted method have been prepared. A comparative study of PU-PF, PU-PFTPE and PU-PTTPE for detection explosives had been performed, and significant fluorescence quenching was observed with the introduction of PA solutions. The as-prepared PU-PF, PU-PFTPE and PU-PTTPE sensors exhibited a superior sensitivity for PA solutions with different concentrations. Remarkably, PU-PF gave a quenching efficiency of 96.2%, higher than 93.5% for PU-PFTPE and 86.7% for PU-PTTPE at a PA concentration of 180 µg·mL−1 in methanol, which was attributed to the effective energy transfer from the fluorophore (PF) to the nitro explosive (PA). This suggested that some ACQ polymers, applied to detect explosives, could afford better performances than AIE or AEE polymers through modification of structures and selection of adequate carriers. At the same time, these chemical sensors can be recycled many times. PMID:29762497

Pre-Licensing Evaluation of Legacy SFR Metallic Fuel Data

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

Yacout, A. M.; Billone, M. C.

2016-09-16

The US sodium cooled fast reactor (SFR) metallic fuel performance data that are of interest to advanced fast reactors applications, can be attributed mostly to the Integral Fast Reactor (IFR) program between 1984 and 1994. Metallic fuel data collected prior to the IFR program were associated with types of fuel that are not of interest to future advanced reactors deployment (e.g., previous U-Fissium alloy fuel). The IFR fuels data were collected from irradiation of U-Zr based fuel alloy, with and without Pu additions, and clad in different types of steels, including HT9, D9, and 316 stainless-steel. Different types of datamore » were generated during the program, and were based on the requirements associated with the DOE Advanced Liquid Metal Cooled Reactor (ALMR) program.« less

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.

U.S. EPA, Pesticide Product Label, , 03/27/1989

EPA Pesticide Factsheets

2011-04-19

... d _n, "un .,t ••• n. c ••• I·'I: U, •• ,00' .".,tr .djult.d to • co"" .. t 'Pu,. Dar"t thl .,,., ta h"'.t ,I" .. , c,.Ck •• n. C".,C'I un G., pl· 'It. "aun' cOIt •• nl'. ...

Photonuclear activation of pure isotopic mediums.

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

Grohman, Mark A.; Lukosi, Eric Daniel

2010-06-01

This work simulated the response of idealized isotopic U-235, U-238, Th-232, and Pu-239 mediums to photonuclear activation with various photon energies. These simulations were conducted using MCNPX version 2.6.0. It was found that photon energies between 14-16 MeV produce the highest response with respect to neutron production rates from all photonuclear reactions. In all cases, Pu-239 responds the highest, followed by U-238. Th-232 produces more overall neutrons at lower photon energies then U-235 when material thickness is above 3.943 centimeters. The time it takes each isotopic material to reach stable neutron production rates in time is directly proportional to themore » material thickness and stopping power of the medium, where thicker mediums take longer to reach stable neutron production rates and thinner media display a neutron production plateau effect, due to the lack of significant attenuation of the activating photons in the isotopic mediums. At this time, no neutron sensor system has time resolutions capable of verifying these simulations, but various indirect methods are possible and should be explored for verification of these results.« less

Lead Slowing-Down Spectrometry Time Spectral Analysis for Spent Fuel Assay: FY11 Status Report

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

Kulisek, Jonathan A.; Anderson, Kevin K.; Bowyer, Sonya M.

2011-09-30

Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration, of which PNNL is a part, to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertaintymore » considerably lower than the approximately 10% typical of today's confirmatory assay methods. This document is a progress report for FY2011 PNNL analysis and algorithm development. Progress made by PNNL in FY2011 continues to indicate the promise of LSDS analysis and algorithms applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model, which accounts for self-shielding effects using empirical basis vectors calculated from the singular value decomposition (SVD) of a matrix containing the true self-shielding functions of the used fuel assembly models. The potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space was demonstrated. Also, in FY2011, PNNL continued to develop an analytical model. Such efforts included the addition of six more non-fissile absorbers in the analytical shielding function and the non-uniformity of the neutron flux across the LSDS assay chamber. A hybrid analytical-empirical approach was developed to determine the mass of total Pu (sum of the masses of 239Pu, 240Pu, and 241Pu), which is an important quantity in safeguards. Results using this hybrid method were of approximately the same accuracy as the pure empirical approach. In addition, total Pu with much better accuracy with the hybrid approach than the pure analytical approach. In FY2012, PNNL will continue efforts to optimize its empirical model and minimize its reliance on calibration data. In addition, PNNL will continue to develop an analytical model, considering effects such as neutron-scattering in the fuel and cladding, as well as neutrons streaming through gaps between fuel pins in the fuel assembly.« less

Feasibility Study of Supercritical Light Water Cooled Reactors for Electric Power Production, Nuclear Energy Research Initiative Project 2001-001, Westinghouse Electric Co. Grant Number: DE-FG07-02SF22533, Final Report

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

Philip E. MacDonald

2005-01-01

The supercritical water-cooled reactor (SCWR) is one of the six reactor technologies selected for research and development under the Generation IV program. SCWRs are promising advanced nuclear systems because of their high thermal efficiency (i.e., about 45% versus about 33% efficiency for current Light Water Reactors [LWRs]) and considerable plant simplification. SCWRs are basically LWRs operating at higher pressure and temperatures with a direct once-through cycle. Operation above the critical pressure eliminates coolant boiling, so the coolant remains single-phase throughout the system. Thus, the need for a pressurizer, steam generators, steam separators, and dryers is eliminated. The main mission ofmore » the SCWR is generation of low-cost electricity. It is built upon two proven technologies: LWRs, which are the most commonly deployed power generating reactors in the world, and supercritical fossil-fired boilers, a large number of which are also in use around the world. The reference SCWR design for the U.S. program is a direct cycle system operating at 25.0 MPa, with core inlet and outlet temperatures of 280 and 500 C, respectively. The coolant density decreases from about 760 kg/m3 at the core inlet to about 90 kg/m3 at the core outlet. The inlet flow splits with about 10% of the inlet flow going down the space between the core barrel and the reactor pressure vessel (the downcomer) and about 90% of the inlet flow going to the plenum at the top of the rector pressure vessel, to then flow down through the core in special water rods to the inlet plenum. Here it mixes with the feedwater from the downcomer and flows upward to remove the heat in the fuel channels. This strategy is employed to provide good moderation at the top of the core. The coolant is heated to about 500 C and delivered to the turbine. The purpose of this NERI project was to assess the reference U.S. Generation IV SCWR design and explore alternatives to determine feasibility. The project was organized into three tasks: Task 1. Fuel-cycle Neutronic Analysis and Reactor Core Design Task 2. Fuel Cladding and Structural Material Corrosion and Stress Corrosion Cracking Task 3. Plant Engineering and Reactor Safety Analysis. moderator rods. materials.« 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

High- and low-Am RE inclusion phases in a U-Np-Pu-Am-Zr alloy

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

Janney, Dawn E.; Madden, James W.; O'Holleran, Thomas P.

2015-03-01

Structural, microstructural, and microchemical data were collected from rare-earth inclusions in an as-cast U-Pu-Zr alloy with ~3 at% Am, 2% Np, and 9% rare-earth elements (La, Ce, Pr, and Nd). Two RE phases with different concentrations of Am were identified. The composition of high-Am RE inclusions is ~2-5 at% La, 15-20 % Ce, 5-10% Pr, 25-45% Nd, 1% Np, 5-10% Pu, and 10-20% Am. Some areas also have O, although this does not appear to be an essential part of the high-Am RE phase. The inclusions have a face-centered cubic structure with a lattice parameter a ~ 0.54 nm. Themore » composition of the only low-Am RE inclusion studied in detail is ~~35-40 at% O, 40-45 % Nd, 1-2% Zr, 4-5% La, 9-10% Ce, and 6-7% Pr. This inclusion is an oxide with a crystal structure similar to the room-temperature structure of Nd 2O 3. Microstructural features suggest that oxidation occurred during casting, and that early crystallization of high-temperature oxides led to formation of two distinct RE phases.« less

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.

Search for hidden high-Z materials inside containers with the Muon Portal Project

NASA Astrophysics Data System (ADS)

La Rocca, P.; Antonuccio, V.; Bandieramonte, M.; Becciani, U.; Belluomo, F.; Belluso, M.; Billotta, S.; Blancato, A. A.; Bonanno, D.; Bonanno, G.; Costa, A.; Fallica, G.; Garozzo, S.; Indelicato, V.; Leonora, E.; Longhitano, F.; Longo, S.; Lo Presti, D.; Massimino, P.; Petta, C.; Pistagna, C.; Pugliatti, C.; Puglisi, M.; Randazzo, N.; Riggi, F.; Riggi, S.; Romeo, G.; Russo, G. V.; Santagati, G.; Valvo, G.; Vitello, F.; Zaia, A.; Zappalà, G.

2014-01-01

The Muon Portal is a recently born project that plans to build a large area muon detector for a noninvasive inspection of shipping containers in the ports, searching for the presence of potential fissile (U, Pu) threats. The technique employed by the project is the well-known muon tomography, based on cosmic muon scattering from high-Z materials. The design and operational parameters of the muon portal under construction will be described in this paper, together with preliminary simulation and test results.

A baseline assessment of forest composition, structure, and health in the Hawai‘i experimental tropical forests

Treesearch

Robert R. Pattison; Andrew N. Gray; Lori Tango

2015-01-01

The US Forest Service’s Forest Inventory and Analysis (FIA) Program of the Pacific Northwest (PNW) Research Station has been working in the Hawaiian islands since 2010. During this time they have installed a base grid of field plots across all of the Hawaiian Islands and an intensified sample of two experimental forests, the Laupāhoehoe and Pu‘u Wa‘awa‘a units of the...

Photo-fission Product Yield Measurements at Eγ=13 MeV on 235U, 238U, and 239Pu

NASA Astrophysics Data System (ADS)

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

2016-09-01

We have measured Fission Product Yields (FPYs) in photo-fission of 235U, 238U, and 239Pu at TUNL's High-Intensity Gamma-ray Source (HI γS) using mono-energetic photons of Eγ = 13 MeV. Details of the experimental setup and analysis procedures will be discussed. Yields for approximately 20 fission products were determined. They are compared to neutron-induced FPYs of the same actinides at the equivalent excitation energies of the compound nuclear systems. In the future photo-fission data will be taken at Eγ = 8 . 0 and 10.5 MeV to find out whether photo-fission exhibits the same so far unexplained dependence of certain FPYs on the energy of the incident probe, as recently observed in neutron-induced fission, for example, for the important fission product 147Nd. Work supported by the U. S. Dept. of Energy, under Grant No. DE-FG02-97ER41033, and by the NNSA, Stewardship Science Academic Alliances Program, Grant No. DE-NA0001838 and the Lawrence Livermore, National Security, LLC under Contract No. DE-AC52-07NA27344.

Isotopic fission-fragment distributions of 238U, 239Np, 240Pu, 244Cm, and 250Cf produced through inelastic scattering, transfer, and fusion reactions in inverse kinematics

NASA Astrophysics Data System (ADS)

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

2018-05-01

Transfer- and fusion-induced fission in inverse kinematics has proved to be a powerful tool to investigate nuclear fission, widening information on the fission fragments and access to unstable fissioning systems with respect to other experimental approaches. An experimental campaign is being carried out at GANIL with this technique since 2008. In these experiments, a beam of 238U, accelerated to 6.1 MeV/u, impinges on a 12C target. Fissioning systems from U to Cf are populated through inelastic scattering, transfer, and fusion reactions, with excitation energies that range from a few MeV up to 46 MeV. The use of inverse kinematics, the SPIDER telescope, and the VAMOS spectrometer allow the characterization of the fissioning system in terms of mass, nuclear charge, and excitation energy, and the isotopic identification of the full fragment distribution. This work reports on new data from the second experiment of the campaign on fission-fragment yields of the heavy actinides 238U, 239Np, 240Pu, 244Cm, and 250Cf, which are of interest from both fundamental and application points of view.

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

Xu, C.; Santschi, P; Roberts, K

Relatively recently, inorganic colloids have been invoked to reconcile the apparent contradictions between expectations based on classical dissolved-phase Pu transport and field observations of 'enhanced' Pu mobility (Kersting et al. Nature 1999, 397, 56-59). A new paradigm for Pu transport is mobilization and transport via biologically produced ligands. This study for the first time reports a new finding of Pu being transported, at sub-pM concentrations, by a cutin-like natural substance containing siderophore-like moieties and virtually all mobile Pu. Most likely, Pu is complexed by chelating groups derived from siderophores that are covalently bound to a backbone of cutin-derived soil degradationmore » products, thus revealing the history of initial exposure to Pu. Features such as amphiphilicity and small size make this macromolecule an ideal collector for actinides and other metals and a vector for their dispersal. Cross-linking to the hydrophobic domains (e.g., by polysaccharides) gives this macromolecule high mobility and a means of enhancing Pu transport. This finding provides a new mechanism for Pu transport through environmental systems that would not have been predicted by Pu transport models.« 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

Speciation and Bioavailability Measurements of Environmental Plutonium Using Diffusion in Thin Films.

PubMed

Cusnir, Ruslan; Steinmann, Philipp; Christl, Marcus; Bochud, François; Froidevaux, Pascal

2015-11-09

The biological uptake of plutonium (Pu) in aquatic ecosystems is of particular concern since it is an alpha-particle emitter with long half-life which can potentially contribute to the exposure of biota and humans. The diffusive gradients in thin films technique is introduced here for in-situ measurements of Pu bioavailability and speciation. A diffusion cell constructed for laboratory experiments with Pu and the newly developed protocol make it possible to simulate the environmental behavior of Pu in model solutions of various chemical compositions. Adjustment of the oxidation states to Pu(IV) and Pu(V) described in this protocol is essential in order to investigate the complex redox chemistry of plutonium in the environment. The calibration of this technique and the results obtained in the laboratory experiments enable to develop a specific DGT device for in-situ Pu measurements in freshwaters. Accelerator-based mass-spectrometry measurements of Pu accumulated by DGTs in a karst spring allowed determining the bioavailability of Pu in a mineral freshwater environment. Application of this protocol for Pu measurements using DGT devices has a large potential to improve our understanding of the speciation and the biological transfer of Pu in aquatic ecosystems.

Forensic investigation of plutonium metal: a case study of CRM 126

DOE PAGES

Byerly, Benjamin L.; Stanley, Floyd; Spencer, Khal; ...

2016-11-01

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.

Fertile-to-fissile and fission measurements for depleted uranium bombarded by 800-MeV protons

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

Russell, G.J.; Gilmore, J.S.; Robinson, H.

Axial distributions of fertile-to-fissile conversions (/sup 238/U to /sup 239/Pu) and fissions have been measured for a thick depleted uranium target bombarded by 800-MeV protons. The /sup 239/Pu production was determined by measuring the amount of /sup 239/Np produced. The axial distributions were integrated to get the total conversions and fissions occurring in the target. Preliminary experimental results give 3.81 +- 0.19 /sup 239/Np atoms produced per incident proton and 5.59 +- 0.56 fissions per incident proton. Corresponding calculated results are 3.46 +- 0.05 and 3.93 +- 0.06. The computations did not include the effects of high-energy fission competition withmore » evaporation. Measured axial disributions of /sup 237/U and eleven fission products produced in the target are reported. Preliminary experimental data give 0.95 +- 0.05 /sup 237/U atoms made per incident proton.« less

A comparison of the pharmacokinetic and pharmacodynamic properties of nitroglycerin according to the composition of the administration set: A preliminary study.

PubMed

Kim, Choon Ok; Song, Jeongyun; Min, Ji Young; Park, Su Jung; Lee, Hye Mi; Byon, Hyo-Jin

2018-03-01

There is a risk of drug sorption into an intravenous administration set composed of polyvinyl chloride (PVC), polyurethane (PU), or polyolefin (PO). This has implications on the dose of the active ingredient the patient receives, and thus therapeutic success. This study aimed to determine the plasma concentration of nitroglycerin and the effect of nitroglycerin on patients based on the composition of the administration set. Using a randomized, open-labeled, 3 × 3 crossover method, 9 volunteers were assigned to 3 groups. In period I, nitroglycerin (100 μg/mL) was infused via a PVC- (group A), PU- (group B), or PO-based (group C) administration set. In period II, PU- (group A), PO- (group B), and PVC-based (group C) administration sets were used, and in period III, PO- (group A), PVC- (group B), and PU-based (group C) administration sets were used. The rate of drug administration in all periods was 12 mL/hour for 30 minutes using an infusion pump. Blood samples were collected, and the plasma concentrations of nitroglycerin were analyzed using validated high-performance liquid chromatography coupled with tandem mass spectrometry. Blood pressure was determined using a sphygmomanometer applied to the other upper arm at an interval of 5 minutes. We observed that the mean plasma concentration of nitroglycerin over time when administered using a PO-based tube was higher than that when using a PU- or PVC-based tube. When the percent change of the mean arterial pressure from baseline at each time point was compared among groups, there were statistically significant differences between PU and PO or PVC at most points during nitroglycerin infusion. Our results showed higher nitroglycerin plasma concentration and lower arterial pressure when a PO-based administration set was used than when a PVC- or PU-based administration set was used. PO-based administration sets may be more appropriate for nitroglycerin administration compared to those composed of PVC or PU.

A comparison of the pharmacokinetic and pharmacodynamic properties of nitroglycerin according to the composition of the administration set

PubMed Central

Kim, Choon Ok; Song, Jeongyun; Min, Ji Young; Park, Su Jung; Lee, Hye Mi; Byon, Hyo-Jin

2018-01-01

Abstract Background: There is a risk of drug sorption into an intravenous administration set composed of polyvinyl chloride (PVC), polyurethane (PU), or polyolefin (PO). This has implications on the dose of the active ingredient the patient receives, and thus therapeutic success. This study aimed to determine the plasma concentration of nitroglycerin and the effect of nitroglycerin on patients based on the composition of the administration set. Methods: Using a randomized, open-labeled, 3 × 3 crossover method, 9 volunteers were assigned to 3 groups. In period I, nitroglycerin (100 μg/mL) was infused via a PVC- (group A), PU- (group B), or PO-based (group C) administration set. In period II, PU- (group A), PO- (group B), and PVC-based (group C) administration sets were used, and in period III, PO- (group A), PVC- (group B), and PU-based (group C) administration sets were used. The rate of drug administration in all periods was 12 mL/hour for 30 minutes using an infusion pump. Blood samples were collected, and the plasma concentrations of nitroglycerin were analyzed using validated high-performance liquid chromatography coupled with tandem mass spectrometry. Blood pressure was determined using a sphygmomanometer applied to the other upper arm at an interval of 5 minutes. Results: We observed that the mean plasma concentration of nitroglycerin over time when administered using a PO-based tube was higher than that when using a PU- or PVC-based tube. When the percent change of the mean arterial pressure from baseline at each time point was compared among groups, there were statistically significant differences between PU and PO or PVC at most points during nitroglycerin infusion. Conclusion: Our results showed higher nitroglycerin plasma concentration and lower arterial pressure when a PO-based administration set was used than when a PVC- or PU-based administration set was used. PO-based administration sets may be more appropriate for nitroglycerin administration compared to those composed of PVC or PU. PMID:29489681

Identifying Patterns in Implementation of Hospital Pressure Ulcer Prevention Programs: A Multisite Qualitative Study.

PubMed

Soban, Lynn M; Finley, Erin P; Miltner, Rebecca S

2016-01-01

To describe the presence or absence of key components of hospital pressure ulcer (PU) prevention programs in 6 acute care hospitals. Multisite comparative case study. Using purposeful selection based on PU rates (high vs low) and hospital size, 6 hospitals within the Veterans Health Administration health care system were invited to participate. Key informant interviews (n = 48) were conducted in each of the 6 participating hospitals among individuals playing key roles in PU prevention: senior nursing leadership (n = 9), nurse manager (n = 7), wound care specialist (n = 6), frontline RNs (n = 26). Qualitative data were collected during face-to-face, semistructured interviews. Interview protocols were tailored to each interviewee's role with a core set of common questions covering 3 major content areas: (1) practice environment (eg, policies and wound care specialists), (2) current prevention practices (eg, conduct of PU risk assessment and skin inspection), and (3) barriers to PU prevention. We conducted structured coding of 5 key components of PU prevention programs and cross-case analysis to identify patterns in operationalization and implementation of program components across hospitals based on facility size and PU rates (low vs high). All hospitals had implemented all PU prevention program components. Component operationalization varied considerably across hospitals. Wound care specialists were integral to the operationalization of the 4 other program components examined; however, staffing levels and work assignments of wound care specialists varied widely. Patterns emerged among hospitals with low and high PU rates with respect to wound care specialist staffing, data monitoring, and staff education. We found hospital-level variations in PU prevention programs. Wound care specialist staffing may represent a potential point of leverage in achieving other PU program components, particularly performance monitoring and staff education.

Confidence Intervals from Realizations of Simulated Nuclear Data

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

Younes, W.; Ratkiewicz, A.; Ressler, J. J.

2017-09-28

Various statistical techniques are discussed that can be used to assign a level of confidence in the prediction of models that depend on input data with known uncertainties and correlations. The particular techniques reviewed in this paper are: 1) random realizations of the input data using Monte-Carlo methods, 2) the construction of confidence intervals to assess the reliability of model predictions, and 3) resampling techniques to impose statistical constraints on the input data based on additional information. These techniques are illustrated with a calculation of the keff value, based on the 235U(n, f) and 239Pu (n, f) cross sections.

Assessment of Possible Cycle Lengths for Fully-Ceramic Micro-Encapsulated Fuel-Based Light Water Reactor Concepts

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

R. Sonat Sen; Michael A. Pope; Abderrafi M. Ougouag

2012-04-01

The tri-isotropic (TRISO) fuel developed for High Temperature reactors is known for its extraordinary fission product retention capabilities [1]. Recently, the possibility of extending the use of TRISO particle fuel to Light Water Reactor (LWR) technology, and perhaps other reactor concepts, has received significant attention [2]. The Deep Burn project [3] currently focuses on once-through burning of transuranic fissile and fissionable isotopes (TRU) in LWRs. The fuel form for this purpose is called Fully-Ceramic Micro-encapsulated (FCM) fuel, a concept that borrows the TRISO fuel particle design from high temperature reactor technology, but uses SiC as a matrix material rather thanmore » graphite. In addition, FCM fuel may also use a cladding made of a variety of possible material, again including SiC as an admissible choice. The FCM fuel used in the Deep Burn (DB) project showed promising results in terms of fission product retention at high burnup values and during high-temperature transients. In the case of DB applications, the fuel loading within a TRISO particle is constituted entirely of fissile or fissionable isotopes. Consequently, the fuel was shown to be capable of achieving reasonable burnup levels and cycle lengths, especially in the case of mixed cores (with coexisting DB and regular LWR UO2 fuels). In contrast, as shown below, the use of UO2-only FCM fuel in a LWR results in considerably shorter cycle length when compared to current-generation ordinary LWR designs. Indeed, the constraint of limited space availability for heavy metal loading within the TRISO particles of FCM fuel and the constraint of low (i.e., below 20 w/0) 235U enrichment combine to result in shorter cycle lengths compared to ordinary LWRs if typical LWR power densities are also assumed and if typical TRISO particle dimensions and UO2 kernels are specified. The primary focus of this summary is on using TRISO particles with up to 20 w/0 enriched uranium kernels loaded in Pressurized Water Reactor (PWR) assemblies. In addition to consideration of this 'naive' use of TRISO fuel in LWRs, several refined options are briefly examined and others are identified for further consideration including the use of advanced, high density fuel forms and larger kernel diameters and TRISO packing fractions. The combination of 800 {micro}m diameter kernels of 20% enriched UN and 50% TRISO packing fraction yielded reactivity sufficient to achieve comparable burnup to present-day PWR fuel.« less

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

NONE

Nuclear power has safely, reliably, and economically contributed almost 20% of electrical generation in the United States over the past two decades. It remains the single largest contributor (more than 60%) of non-greenhouse-gas-emitting electric power generation in the United States. Domestic demand for electrical energy is expected to grow by about 24% from 2013 to 2040 . At the same time, most of the currently operating nuclear power plants will begin reaching the end of their initial 20-year extension to their original 40-year operating license, for a total of 60 years of operation (the oldest commercial plants in the Unitedmore » States reached their 40th anniversary in 2009). Figure E-1 shows projected nuclear energy contribution to the domestic generating capacity for 40- and 60-year license periods. If current operating nuclear power plants do not operate beyond 60 years (and new nuclear plants are not built quickly enough to replace them), the total fraction of generated electrical energy from nuclear power will rapidly decline. That decline will be accelerated if plants are shut down before 60 years of operation. Decisions on extended operation ultimately rely on economic factors; however, economics can often be improved through technical advancements. The U.S. Department of Energy Office of Nuclear Energy's 2010 Research and Development Roadmap (2010 Nuclear Energy Roadmap) organizes its activities around four objectives that ensure nuclear energy remains a compelling and viable energy option for the United States. The four objectives are as follows: 1. Develop technologies and other solutions that can improve the reliability, sustain the safety, and extend the life of the current reactors; 2. Develop improvements in the affordability of new reactors to enable nuclear energy to help meet the Administration's energy security and climate change goals; 3. Develop sustainable nuclear fuel cycles; and 4. Understand and minimize the risks of nuclear proliferation and terrorism. The Light Water Reactor Sustainability (LWRS) Program is the primary programmatic activity that addresses Objective 1. This document summarizes the LWRS Program's plans. For the LWRS Program, sustainability is defined as the ability to maintain safe and economic operation of the existing fleet of nuclear power plants for a longer-than-initially-licensed lifetime. It has two facets with respect to long-term operations: (1) manage the aging of plant systems, structures, and components so that nuclear power plant lifetimes can be extended and the plants can continue to operate safely, efficiently, and economically; and (2) provide science-based solutions to the industry to implement technology to exceed the performance of the current labor-intensive business model.« less

A Roll, Fin, and Fin Controller Prediction Computer Program.

DTIC Science & Technology

1980-06-01

IERATI *EQ. 03 WRITE16920301 ROLL 365 365 3R1TE(G. 26311 ROLL 366 no 505 ImU - 1,NNU ROLL 36? 50S WRITE(G.2011 3U(I’U),OAWPU(1PU,SIGLCfINU) ROLL 360...ROLL DAMPING WILL BE ONE**/$ ROLL 642 2016 FORMAT (/jIX,*LONGCRESTEO SVECTRA AND COMPONENTS WILL SE PRINTED. ROLL 44S 2’) ROLL 444 2019 FORMAT (1/19

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

Guidelines for Implementation of an Advanced Outage Control Center to Improve Outage Coordination, Problem Resolution, and Outage Risk Management

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

St. Germain, Shawn W.; Farris, Ronald K.; Whaley, April M.

This research effort is a part of the Light-Water Reactor Sustainability (LWRS) Program, which is a research and development (R&D) program sponsored by Department of Energy (DOE) and performed in close collaboration with industry R&D programs that provide the technical foundations for licensing and managing the long-term, safe, and economical operation of current nuclear power plants. The LWRS program serves to help the U.S. nuclear industry adopt new technologies and engineering solutions that facilitate the continued safe operation of the plants and extension of the current operating licenses. The purpose of this research is to improve management of nuclear powermore » plant (NPP) outages through the development of an advanced outage control center (AOCC) that is specifically designed to maximize the usefulness of communication and collaboration technologies for outage coordination and problem resolution activities. This technical report for industry implementation outlines methods and considerations for the establishment of an AOCC. This report provides a process for implementation of a change management plan, evaluation of current outage processes, the selection of technology, and guidance for the implementation of the selected technology. Methods are presented for both adoption of technologies within an existing OCC and for a complete OCC replacement, including human factors considerations for OCC design and setup.« less

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

Neutron-induced fission cross section of 242Pu from 15 MeV to 20 MeV

NASA Astrophysics Data System (ADS)

Jovančević, N.; Salvador-Castineira, P.; Daraban, L.; Vidali, M.; Heyse, J.; Oberstedt, S.; Hambsch, F.-J.; Bonaldi, C.; Geerts, W.

2017-09-01

Accurate nuclear-data needs in the fast-neutron-energy region have been recently addressed for the development of next generation nuclear power plants (GEN-IV) by the OECD Nuclear Energy Agency (NEA). This sensitivity study has shown that of particular interest is the 242Pu(n,f) cross section for fast reactor systems. Measurements have been performed with quasi-monoenergetic neutrons in the energy range from 15 MeV to 20 MeV produced by the Van de Graaff accelerator of the JRC-Geel. A twin Frisch-grid ionization chamber has been used in a back-to-back configuration as fission fragment detector. The 242Pu(n,f) cross section has been normalized to 238U(n,f) cross section data. The results were compared with existing literature data and show acceptable agreement within 5%.

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

Scott, Bobby R.; Tokarskaya, Zoya B.; Zhuntova, Galina V.

This report summarizes 4 years of research achievements in this Office of Science (BER), U.S. Department of Energy (DOE) project. The research described was conducted by scientists and supporting staff at Lovelace Respiratory Research Institute (LRRI)/Lovelace Biomedical and Environmental Research Institute (LBERI) and the Southern Urals Biophysics Institute (SUBI). All project objectives and goals were achieved. A major focus was on obtaining improved cancer risk estimates for exposure via inhalation to plutonium (Pu) isotopes in the workplace (DOE radiation workers) and environment (public exposures to Pu-contaminated soil). A major finding was that low doses and dose rates of gamma raysmore » can significantly suppress cancer induction by alpha radiation from inhaled Pu isotopes. The suppression relates to stimulation of the body's natural defenses, including immunity against cancer cells and selective apoptosis which removes precancerous and other aberrant cells.« 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.

Actuators based on polyurethanes with different types of polyol

NASA Astrophysics Data System (ADS)

Lim, Hyun-Ok; Bark, Geong-Mi; Jo, Nam-Ju

2007-07-01

This study dealt with the electrostrictive responses of polyurethane (PU) actuators with different microphase separation structure, which was a promising candidate for a material used in polymer actuators. In order to construct PUs with different higher-order structure, we synthesized PUs with different diols; poly(neopentyl glycol adipate) (PNAD), poly(tetramethylene glycol) (PTMG), and poly(dimethyl siloxnae) (PDMS). Synthesized PU was characterized by FT-IR spectroscopy and GPC. Thermal analysis and mechanical properties of PU films were carried out with DSC and UTM, respectively. And PU actuator was formed in a monomorph type which made by carbon black electrodes on the both surfaces of PU film by spin coating method. Actuation behavior was mainly influenced on microphase separation structure and mechanical property of PU. In result, PU actuator with PNAD, polyester urethane, had the largest field-induced displacement.

Quantitative non-destructive assay of PuBe neutron sources

NASA Astrophysics Data System (ADS)

Lakosi, László; Bagi, János; Nguyen, Cong Tam

2006-02-01

PuBe neutron sources were assayed, using a combination of high resolution γ-spectrometry (HRGS) and neutron correlation technique. In a previous publication [J. Bagi, C. Tam Nguyen, L. Lakosi, Nucl. Instr. and Meth. B 222 (2004) 242] a passive neutron well-counter was reported with 3He tubes embedded in a polyamide (TERRAMID) moderator (lined inside with Cd) surrounding the sources to be measured. Gross and coincidence neutron counting was performed, and the Pu content of the sources was found out from isotope analysis and by adopting specific (α, n) reaction yields of the Pu isotopes and 241Am in Be, based on supplier's information and literature data. The method was further developed and refined. Evaluation algorithm was more precisely worked out. The contribution of secondary (correlated) neutrons to the total neutron output was derived from the coincidence (doubles) count rate and taken into account in assessing the Pu content. A new evaluation of former results was performed. Assay was extended to other PuBe sources, and new results were added. In order to attain higher detection efficiency, a more efficient moderator was also applied, with and without Cd shielding around the assay chamber. Calibration seems possible using neutron measurements only (without γ-spectrometry), based on a correlation between the Pu amount and the coincidence-to-total ratio. It is expected that the method could be used for Pu accountancy and safeguards verification as well as identification and assay of seized, found, or not documented PuBe neutron sources.

Lead Slowing-Down Spectrometry for Spent Fuel Assay: FY11 Status Report

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

Warren, Glen A.; Casella, Andrew M.; Haight, R. C.

2011-08-01

Executive Summary Developing a method for the accurate, direct, and independent assay of the fissile isotopes in bulk materials (such as used fuel) from next-generation domestic nuclear fuel cycles is a goal of the Office of Nuclear Energy, Fuel Cycle R&D, Material Protection and Control Technology (MPACT) Campaign. To meet this goal, MPACT supports a multi-institutional collaboration to study the feasibility of Lead Slowing Down Spectroscopy (LSDS). This technique is an active nondestructive assay method that has the potential to provide independent, direct measurement of Pu and U isotopic masses in used fuel with an uncertainty considerably lower than themore » approximately 10% typical of today’s confirmatory assay methods. This document is a progress report for FY2011 collaboration activities. Progress made by the collaboration in FY2011 continues to indicate the promise of LSDS techniques applied to used fuel. PNNL developed an empirical model based on calibration of the LSDS to responses generated from well-characterized used fuel. The empirical model demonstrated the potential for the direct and independent assay of the sum of the masses of 239Pu and 241Pu to within approximately 3% over a wide used fuel parameter space. Similar results were obtained using a perturbation approach developed by LANL. Benchmark measurements have been successfully conducted at LANL and at RPI using their respective LSDS instruments. The ISU and UNLV collaborative effort is focused on the fabrication and testing of prototype fission chambers lined with ultra-depleted 238U and 232Th, and uranium deposition on a stainless steel disc using spiked U3O8 from room temperature ionic liquid was successful, with improving thickness obtained. In FY2012, the collaboration plans a broad array of activities. PNNL will focus on optimizing its empirical model and minimizing its reliance on calibration data, as well continuing efforts on developing an analytical model. Additional measurements are planned at LANL and RPI. LANL measurements will include a Pu sample, which is expected to provide more counts at longer slowing-down times to help identify discrepancies between experimental data and MCNPX simulations. RPI measurements will include the assay of an entire fresh fuel assembly for the study of self-shielding effects as well as the ability to detect diversion by detecting a missing fuel pin in the fuel assembly. The development of threshold neutron sensors will continue, and UNLV will calibrate existing ultra-depleted uranium deposits at ISU.« less

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

PREVENTION OF POLYURETHANE OXIDATIVE DEGRADATION WITH PHENOLIC-ANTIOXIDANTS COVALENTLY ATTACHED TO THE HARD SEGMENTS: STRUCTURE FUNCTION RELATIONSHIPS

PubMed Central

Stachelek, Stanley J; Alferiev, Ivan; Ueda, Masako; Eckels, Edward C.; Gleason, Kevin T.; Levy, Robert J

2010-01-01

Oxidative degradation of the polyurethane elastomeric (PU) components greatly reduces the efficacy of PU containing cardiovascular devices. Covalently appending the phenol-based antioxidant, 4-substituted 2,6-di-tert-butylphenol (DBP), to PU hard segments effectively reduced oxidative degradation of the PU in vivo and in vitro in prior studies by our group. In these experiments we analyze the contribution of the tethering molecule to the antioxidant capabilities of the DBP modified PU. Bromoalkylation chemistry was used to link DBP to the hard segment of the polyether polyurethane, Tecothane, via our original linker (PU-DBP), or variants containing side chains with 1 (PU-C-DBP) or 3 (PU-3C-DBP) carbons. Two additional DBP variants were fabricated in which the DBP group was appended to the alkyl chain via an oxygen atom (PU-O-DBP) or an amide linkage in the middle of the tether (PU-NHCO-DBP). All DBP variant films and unmodified control films were subject to oxidative degradation via 15 day immersion in a solution of 20% H2O2 + 0.1 M CoCl2. At the end of the oxidation protocol films were analyzed for the presence of oxidation related endpoints via scanning electron microscopy, contact angle measurements and Fourier transformation infrared spectroscopy (FTIR). All DBP containing variants resisted oxidation damage significantly better than the unmodified control PU. SEM analysis of oxidized PU-C-DBP and PU-O-DBP showed evidence of surface cracking consistent with oxidative degradation of the PU surfaces. Similarly there was a trend in increased ether cross-linking, a marker for oxidative degradation, in PU-C-DBP and PU-NHCO-DBP films. Consistent with these FTIR results, both PU-C-DBP and PU-NHCO-DBP had significant reductions in measured surface hydrophobicity as a result of oxidation. These data show for the first time that the choice of linker molecule significantly affects the efficiency of the linked phenolic antioxidant. PMID:20306526

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.

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.

Fisher Consistency of AM-Estimates of the Autoregression Parameter Using Hard Rejection Filter Cleaners

DTIC Science & Technology

1987-02-04

U5tr,)! P(U 5-t Since U - F with F RS, we get (3.1). Case b: 0 S 5 k -a Now P([U~t]riM) = P(UZk-a) and P([ Ugt ]rM) = P(US-k-a) S P(US-(k-a)) which again...robustness for autoregressive processes." The Annals of Statistics, 12, 843-863. Mallows, C.L. (1980). "Some theory of nonlinear smoothen." The Annals of

Systematic study of probable projectile-target combinations for the synthesis of the superheavy nucleus 302120

NASA Astrophysics Data System (ADS)

Santhosh, K. P.; Safoora, V.

2016-08-01

Probable projectile-target combinations for the synthesis of the superheavy element 302120 have been studied taking the Coulomb and proximity potential as the interaction barrier. The probabilities of the compound nucleus formation PCN for the projectile-target combinations found in the cold reaction valley of 302120 are estimated. At energies near and above the Coulomb barrier, we have calculated the capture, fusion, and evaporation residue cross sections for the reactions of all probable projectile-target combinations so as to predict the most promising projectile-target combinations for the synthesis of the superheavy element 302120 in heavy-ion fusion reactions. The calculated fusion and evaporation cross sections for the more asymmetric ("hotter") projectile-target combination is found to be higher than the less asymmetric ("colder") combination. It can be seen from the nature of the quasifission barrier height, mass asymmetry, the probability of compound nucleus formation, survival probability, and excitation energy, the systems 44Ar+258No , 46Ar+256No , 48Ca+254Fm , 50Ca+252Fm , 54Ti+248Cf , and 58Cr+244Cm in deep region I of the cold reaction valley and the systems 62Fe+240Pu , 64Fe+238Pu , 68Ni+234U , 70Ni+232U , 72Ni+230U , and 74Zn+228Th in the other cold valleys are identified as the better projectile-target combinations for the synthesis of 302120. Our predictions on the synthesis of 302120 superheavy nuclei using the combinations 54Cr+248Cm , 58Fe+244Pu , 64Ni+238U , and 50Ti+249Cf are compared with available experimental data and other theoretical predictions.

Colloidal cutin-like substances cross-linked to siderophore decomposition products mobilizing plutonium from contaminated soils.

PubMed

Xu, C; Santschi, P H; Zhong, J Y; Hatcher, P G; Francis, A J; Dodge, C J; Roberts, K A; Hung, C C; Honeyman, B D

2008-11-15

Relatively recently, inorganic colloids have been invoked to reconcile the apparent contradictions between expectations based on classical dissolved-phase Pu transport and field observations of "enhanced" Pu mobility (Kersting et al. Nature 1999, 397, 56-59). A new paradigm for Pu transport is mobilization and transport via biologically produced ligands. This study for the first time reports a new finding of Pu being transported, at sub-pM concentrations, by a cutin-like natural substance containing siderophore-like moieties and virtually all mobile Pu. Most likely, Pu is complexed by chelating groups derived from siderophores that are covalently bound to a backbone of cutin-derived soil degradation products, thus revealing the history of initial exposure to Pu. Features such as amphiphilicity and small size make this macromolecule an ideal collector for actinides and other metals and a vector for their dispersal. Cross-linking to the hydrophobic domains (e.g., by polysaccharides) gives this macromolecule high mobility and a means of enhancing Pu transport. This finding provides a new mechanism for Pu transport through environmental systems that would not have been predicted by Pu transport models.

Determination of origin and intended use of plutonium metal using nuclear forensic techniques.

PubMed

Rim, Jung H; Kuhn, Kevin J; Tandon, Lav; Xu, Ning; Porterfield, Donivan R; Worley, Christopher G; Thomas, Mariam R; Spencer, Khalil J; Stanley, Floyd E; Lujan, Elmer J; Garduno, Katherine; Trellue, Holly R

2017-04-01

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% 240 Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modeling feedback and trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. Based on this investigation, the most likely intended use for these plutonium foils was 239 Pu fission foil targets for physics experiments, such as cross-section measurements, etc. Copyright © 2017 Elsevier B.V. All rights reserved.

Determination of origin and intended use of plutonium metal using nuclear forensic techniques

DOE PAGES

Rim, Jung H.; Kuhn, Kevin J.; Tandon, Lav; ...

2017-04-01

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