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At least 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Electronic and optical properties of plutonium metal and oxides from Reflection Electron Energy Loss Spectroscopy

Reflection Electron Energy Loss Spectra (REELS) have been acquired on plutonium δ-Pu-Ga alloys, α-Pu 2 O 3 and PuO 2 . The position of the peaks attributable to the Pu 6p excitation can be used as ‘fingerprint’ for these species. X-ray Photoelectron Spectroscopy has been used to aid interpretation of the REELS spectra. The band gap of PuO 2 was determined from the onset of the energy loss in the REELS spectrum. The REELS data have been evaluated within the dielectric response theory by means of the QUEELS-ε(k, w)-REELS software. In this work, the Energy Loss Function, dielectric function, refractive index and extinction coefficient for these materials have been determined in the ultraviolet and extreme ultraviolet range and are compared to previously reported results.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Plutonium mobilization from contaminated estuarine sediments, Esk Estuary (UK)

Since 1952, liquid radioactive effluent containing 238-242 Pu, 241 Am, 237 Np, 137 Cs, and 99 Tc has been released with authorization from the Sellafield nuclear complex (UK) into the Irish Sea. This represents the largest source of plutonium (Pu) discharged in all western Europe, with 276 kg having been released. In the Eastern Irish Sea, the majority of the transuranic activity has settled into an area of sediments (Mudpatch) located off the Cumbrian coast. Radionuclides from the Mudpatch have been re-dispersed via particulate transport in fine-grained estuarine and intertidal sediments to the North-East Irish Sea, including the intertidal saltmarsh located at the mouth of the Esk Estuary. Saltmarshes are highly dynamic systems which are vulnerable to external agents (sea level change, erosion, sediment supply, and freshwater inputs), and their stability remains uncertain under current sea level rise projections and possible increases in storm activity. In this work, we examined factors affecting Pu mobility in contaminated sediments collected from the Esk Estuary by conducting leaching experiments under both anoxic and oxic conditions. Here, leaching experiments were conducted over a 9-month period and were periodically sampled to determine solution phase Pu via multicollector-inductively coupled plasma-mass spectrometry (MC-ICP-MS), and to measure redox indicators (Eh, pH and extractable Fe(II)). Microbial community composition was also characterized in the sediments, and at the beginning and end of the anoxic/oxic experiments. Results show that: 1) Pu leaching is about three times greater in solutions leached under anoxic conditions compared to oxic conditions, 2) the sediment slurry microbial communities shift as conditions change from anoxic to oxic, 3) Pu leaching is enhanced in the shallow sediments (0–10 cm depth), and 4) the magnitude of Pu leached from sediments is not correlated with total Pu, indicating that the biogeochemistry of sediment-associated Pu is spatially heterogeneous. These findings provide constraints on the stability of redox sensitive Pu in biogeochemically dynamic/transient environments on a timescale of months and suggests that anoxic conditions can enhance Pu mobility in estuarine systems.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2018

Excess Lead-210 and Plutonium-239+240: Two suitable radiogenic soil erosion tracers for mountain grassland sites

Highlights: • First application of excess Lead-210 as soil tracer in alpine grasslands. • {sup 239+240}Pu/{sup 137}Cs ratios indicated 75% Chernobyl contribution to {sup 137}Cs inventory. • {sup 239+240}Pu is compared to more mature radioisotopic tracers (i.e. {sup 210}Pb{sub ex} and {sup 137}Cs). • {sup 210}Pb{sub ex}, {sup 137}Cs and {sup 239+240}Pu yielded comparable estimates of soil redistribution. The expected growing population and challenges associated with globalisation will increase local food and feed demands and enhance the pressure on local and regional upland soil resources. In light of these potential future developments it is necessary to define sustainable land use and tolerable soil loss rates with methods applicable and adapted to mountainous areas. Fallout-radionuclides (FRNs) are proven techniques to increase our knowledge about the status and resilience of agro-ecosystems. However, the use of the Caesium-137 ({sup 137}Cs) method is complicated in the European Alps due to its heterogeneous input and the timing of the Chernobyl fallout, which occurred during a few single rain events on partly snow covered ground. Other radioisotopic techniques have been proposed to overcome these limitations. The objective of this study is to evaluate the suitability of excess Lead-210 ({sup 210}Pb{sub ex}) and Plutonium-239+240 ({sup 239+240}Pu) as soil erosion tracers for three different grassland management types at the steep slopes (slope angles between 35 and 38°) located in the Central Swiss Alps. All three FRNs identified pastures as having the highest mean (± standard deviation) net soil loss of −6.7 ± 1.1, −9.8 ± 6.8 and −7.0 ± 5.2 Mg ha{sup -1} yr{sup -1} for {sup 137}Cs, {sup 210}Pb{sub ex} and {sup 239+240}Pu, respectively. A mean soil loss of −5.7 ± 1.5, −5.2 ± 1.5 and-5.6 ± 2.1 was assessed for hayfields and the lowest rates were established for pastures with dwarf-shrubs (−5.2 ± 2.5, −4.5 ± 2.5 and −3.3 ± 2.4 Mg ha{sup -1} yr{sup -1} for {sup 137}Cs, {sup 210}Pb{sub ex} and {sup 239+240}Pu, respectively). These rates, evaluated at sites with an elevated soil erosion risk exceed the respective soil production rates. Among the three FRN methods used, {sup 239+240}Pu appears as the most promising tracer in terms of measurement uncertainty and reduced small scale variability (CV of 13%). Despite a higher level of uncertainty, {sup 210}Pb{sub ex} produced comparable results, with a wide range of erosion rates sensitive to changes in grassland management. {sup 210}Pb{sub ex} can then be as well considered as a suitable soil tracer to investigate alpine agroecosystems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

The Impact of Gate Width Setting and Gate Utilization Factors on Plutonium Assay in Passive Correlated Neutron Counting

In the field of nuclear safeguards, passive neutron multiplicity counting (PNMC) is a method typically employed in non-destructive assay (NDA) of special nuclear material (SNM) for nonproliferation, verification and accountability purposes. PNMC is generally performed using a well-type thermal neutron counter and relies on the detection of correlated pairs or higher order multiplets of neutrons emitted by an assayed item. To assay SNM, a set of parameters for a given well-counter is required to link the measured multiplicity rates to the assayed item properties. Detection efficiency, die-away time, gate utilization factors (tightly connected to die-away time) as well as optimum gate width setting are among the key parameters. These parameters along with the underlying model assumptions directly affect the accuracy of the SNM assay. In this paper we examine the role of gate utilization factors and the single exponential die-away time assumption and their impact on the measurements for a range of plutonium materials. In addition, we examine the importance of item-optimized coincidence gate width setting as opposed to using a universal gate width value. Finally, the traditional PNMC based on multiplicity shift register electronics is extended to Feynman-type analysis and application of this approach to Pu mass assay is demonstrated.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2017

Passive assay of plutonium metal plates using a fast-neutron multiplicity counter

Here, we developed a fast-neutron multiplicity counter based on organic scintillators (EJ-309 liquid and stilbene). The system detects correlated photon and neutron multiplets emitted by fission reactions, within a gate time of tens of nanoseconds. The system was used at Idaho National Laboratory to assay a variety of plutonium metal plates. A coincidence counting strategy was used to quantify the 240 Pu effective mass of the samples. Coincident neutrons, detected within a 40-ns coincidence window, show a monotonic trend, increasing with the 240 Pu-effective mass (in this work, we tested the 0.005–0.5 kg range). After calibration, the system estimated the 240 Pu effective mass of an unknown sample ( 240 Pu eff >50 g) with an uncertainty lower than 1% in a 4-min assay time.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

On the equilibrium isotopic composition of the thorium–uranium–plutonium fuel cycle

The equilibrium isotopic compositions and the times to equilibrium in the process of thorium–uranium–plutonium oxide fuel recycling in VVER-type reactors using heavy water mixed with light water are estimated. It is demonstrated thEhfat such reactors have a capacity to operate with self-reproduction of active isotopes in the equilibrium mode.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

NNSS Soils Monitoring: Plutonium Valley (CAU366)

The U.S. Department of Energy (DOE) National Nuclear Security Administration (NNSA), Nevada Site Office (NSO), Environmental Restoration Soils Activity has authorized the Desert Research Institute (DRI) to conduct field assessments of potential sediment transport of contaminated soil from Corrective Action Unit (CAU) 366, Area 11 Plutonium Valley Dispersion Sites Contamination Area (CA) during precipitation runoff events.

(CAU)↗
DOE OSTI2015

Independent Review of Siesmic Performance Assessments for the Plutonium Facility PF-4

The Plutonium Facility, designated PF-4, is located in Technical Area 55 at the Los Alamos National Laboratory (LANL). The facility is a one-story rectangular structure above a complete basement; the building was constructed of cast-in-place reinforced concrete, with small interior frames of structural steel. The plan dimensions of the building are 265’×284’. The overall height of the building varies between 39’-0” at the north and south ends, and 40’-6” at the center ridge. The programmatic work performed in the building is vital to our national security and its functions and storage purposes are not replicated elsewhere in the United States Department of Energy (DOE).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Corrective Action Investigation Plan for Corrective Action Unit 414: Clean Slate III Plutonium Dispersion (TTR) Tonopah Test Range, Nevada, Revision 1

Corrective Action Unit (CAU) 414 is located on the Tonopah Test Range, which is approximately 130 miles northwest of Las Vegas, Nevada, and approximately 40 miles southeast of Tonopah, Nevada. The CAU 414 site consists of the release of radionuclides to the surface and shallow subsurface from the conduct of the Clean Slate III (CSIII) storage–transportation test conducted on June 9, 1963. CAU 414 includes one corrective action site (CAS), TA-23-03CS (Pu Contaminated Soil). The known releases at CAU 414 are the result of the atmospheric dispersal of contamination from the 1963 CSIII test. The CSIII test was a nonnuclear detonation of a nuclear device located inside a reinforced concrete bunker covered with 8 feet of soil. This test dispersed radionuclides, primarily uranium and plutonium, on the ground surface. The presence and nature of contamination at CAU 414 will be evaluated based on information collected from a corrective action investigation (CAI). The investigation is based on the data quality objectives (DQOs) developed on June 7, 2016, by representatives of the Nevada Division of Environmental Protection; the U.S. Air Force; and the U.S. Department of Energy (DOE), National Nuclear Security Administration Nevada Field Office. The DQO process was used to identify and define the type, amount, and quality of data needed to develop and evaluate appropriate corrective action alternatives for CAU 414.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Thermal Safety Analyses for the Production of Plutonium-238 at the High Flux Isotope Reactor

There has been a considerable effort over the previous few years to demonstrate and optimize the production of plutonium-238 ( 238 Pu) at the High Flux Isotope Reactor (HFIR). This effort has involved resources from multiple divisions and facilities at the Oak Ridge National Laboratory (ORNL) to demonstrate the fabrication, irradiation, and chemical processing of targets containing neptunium-237 ( 237 Np) dioxide (NpO 2 )/aluminum (Al) cermet pellets. A critical preliminary step to irradiation at the HFIR is to demonstrate the safety of the target under irradiation via documented experiment safety analyses. The steady-state thermal safety analyses of the target are simulated in a finite element model with the COMSOL Multiphysics code that determines, among other crucial parameters, the limiting maximum temperature in the target. Safety analysis efforts for this model discussed in the present report include: (1) initial modeling of single and reduced-length pellet capsules in order to generate an experimental knowledge base that incorporate initial non-linear contact heat transfer and fission gas equations, (2) modeling efforts for prototypical designs of partially loaded and fully loaded targets using limited available knowledge of fabrication and irradiation characteristics, and (3) the most recent and comprehensive modeling effort of a fully coupled thermo-mechanical approach over the entire fully loaded target domain incorporating burn-up dependent irradiation behavior and measured target and pellet properties, hereafter referred to as the production model. These models are used to conservatively determine several important steady-state parameters including target stresses and temperatures, the limiting condition of which is the maximum temperature with respect to the melting point. The single pellet model results provide a basis for the safety of the irradiations, followed by parametric analyses in the initial prototypical designs that were necessary due to the limiting fabrication and irradiation data available. The calculated parameters in the final production target model are the most accurate and comprehensive, while still conservative. Over 210 permutations in irradiation time and position were evaluated, and are supported by the most recent inputs and highest fidelity methodology. The results of these analyses show that the models presented in this report provide a robust and reliable basis for previous, current and future experiment safety analyses. In addition, they reveal an evolving knowledge of the steady-state behavior of the NpO 2 /Al pellets under irradiation for a variety of target encapsulations and potential conditions.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2019

ORNL automates key process in plutonium-238 production

Oak Ridge National Laboratory scientists have automated part of the process of producing plutonium-238, which is used by NASA to fuel deep space exploration. Resolving this key bottleneck will help boost annual production of the radioisotope towards NASA’s goal of 1.5 kilograms of Pu-238 per year by 2025.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2016

In-Situ Gamma-Ray Assay of the 235-F Plutonium Fuel Form Facility at the Savannah River Site - 16293

The Plutonium Fuel Form (PuFF) Facility is located in Building 235-F near the geographic center of the Savannah River Site. Between 1978 and 1984, the facility was used to produce approximately 165 kilograms of iridium-encapsulated Pu-238 spheres and pellets for use as radioisotope thermal generators, primarily for the space program. The facility is divided between two cell lines, the east cell line used to process powdered Pu-238 oxide raw material into fuel forms and the west cell line used to encapsulate the fuel forms in iridium. Scoping in-situ gamma-ray assays were performed in the PuFF Facility in 2006 and estimated that hundreds of grams of Pu-238 holdup were within the facility. Using this holdup estimate as a source term, SRS has performed a risk analysis that indicated a seismic event that induces a full-facility fire in 235-F could lead to a 28,800 rem dose to a co-located worker. Based on this risk assessment, SRS is taking steps to decontaminate the facility. One of the first steps taken has been to improve upon the quality of the in-situ gamma-ray assay data. Carts and collimators were specially designed to survey the equipment in the PuFF Facility. The cell interiors were assayed along with the furnaces and storage coolers that protrude beneath the cells. While the previous scoping work consisted of 32 measurements, the current series of measurements included nearly 400 measurements using both high-purity germanium and lanthanum bromide detectors. Data analysis for the current set of measurements was conducted with greater rigor as well. MCNP5 was used to evaluate a variety of possible physical distributions for the Pu-238 source term and estimate cross-talk between neighboring cells. Data analysis was performed using three gamma-rays emitted by Pu-238 (99.85 keV, 152.7 keV, and 766.4 keV) providing three independent estimates of the mass of Pu-238 holdup in each of the cells. This also allowed the application of matrix correction factors to adjust gamma-ray attenuation. The weighted mean of these three results was used as the best estimate of Pu-238 holdup in the PuFF facility. This work lowered the estimate of holdup in the PuFF facility by approximately 100 grams compared to the previous estimate, a 0.55's difference. The uncertainty in the Pu-238 holdup was also reduced substantially relative to the 2006 scoping assay. Further radiological measurements are planned for the near future including in-situ gamma-ray assays of wing cabinets in the east cell line maintenance area, the transfer tube between the two cell lines, and some of the furnaces and storage coolers. A germanium gamma imager, the GeGI, will also be used to map out the distribution of the Pu-238 source term in the PuFF Facility. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2017

The thermal neutron scattering law for hydrogen bound in plutonium dihydride and predicted critical mass for several configurations

The thermal neutron scattering law (TSL) for hydrogen bound in plutonium dihydride (H-PuH{sub 2}) is developed using first-principles density functional theory and lattice dynamics calculations. The GGA+U exchange correlation with spin-polarized magnetism is used to simulate the electronic structure of the material with a Hubbard U parameter that is selected to reproduce experimental lattice constant measurements. The partial phonon density of states from these calculations is used to develop a thermal neutron scattering law evaluation for H-PuH{sub 2} in the incoherent approximation. This thermal scattering law is used to predict the critical mass of {sup 239}PuH{sub 2} in various bare, reflected, and moderated spherical configurations with MC21 using ENDF/B-VII.1 cross sections. The H-PuH{sub 2} TSL is designed to be suitable for the analysis of bulk PuH{sub x} compositions with 0.0 < x ≤ 2.0. Water volume fractions from 0.0 to 0.95 are analyzed for the homogenized slurry. A small positive difference in k{sub eff} is observed for the water reflected configuration when comparing calculations using the {sup 1}H free-gas treatment instead of the H-PuH{sub 2} thermal scattering law.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Geochemical Simulations of Plutonium Redox Speciation at Increasing Ionic Strengths - 18567

In salt repositories like the Waste Isolation Pilot Plant (WIPP), reducing conditions are expected, supporting two aqueous species of plutonium: Pu(III) and Pu(IV). Of these states, Pu(III) is more soluble than Pu(IV). Because Pu behavior is uncertain in WIPP brines under reducing conditions, performance assessment calculations assume a 50/50 partitioning between the two, justified through calculations using dilute solutions. Recent experimental evidence suggests an increasing importance for Pu(III). To reexamine this assumption, we modeled Pu speciation in NaCl and dilute WIPP brine solutions equilibrated with a Pu solid, including PuO{sub 2} and Pu(OH){sub 3}. To maintain reducing conditions, sulfate and sulfide were added. Models were performed using PHREEQC and the Specific Ion Theory (SIT) database on dilutions ranging from 0.1 M to 3 M. Models were compared to calculations using the Pitzer database with PuO{sub 2} and with analogs Am(III) and Th(IV), all up to 11 M. Results indicate that under reducing conditions, Pu(III) concentrations increase with ionic strength and can be up to 80 fold higher than Pu(IV). While concentrations varied due to differences in solubility for each solid, Pu(IV) concentrations remained nearly constant in all solutions. Analogs showed similar trends, though Am(III) is 3 times more soluble than Pu(III) while Th(IV) is 6 times more soluble than Pu(IV). Pu(IV) concentrations using Pitzer calculations were similar to those with SIT. Our study indicates that assuming equivalent partitioning of Pu species may under-represent concentrations during a release. They also show that in PA calculations there is a need to consider redox state at high ionic strength rather than adopting an assumption of equal partitioning between the two charges. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

Engineering Controls for the Processing and Repackaging of Gloveboxes Contaminated with Plutonium - 19629

Gloveboxes used for processing plutonium (Pu)-238 at the US DOE Mound site in Miamisburg, Ohio, in support of the United States space mission were packaged in non-standard waste boxes and sent to the INL Site for temporary disposal. In addition to the gloveboxes, an assortment of smaller items, all with varying levels of Pu-238 contamination, were found in the non-standard waste boxes. The characteristics of Pu-238 make it especially difficult to contain and control contamination; alpha recoil phenomena and nanometer particle sizes lend to the contamination exhibiting near gas like characteristics. The Idaho Cleanup Project Core contractor, Fluor Idaho, LLC, engineered and deployed a waste processing containment with specialized ventilation and processes to characterize and disposition this waste. This paper summarizes the successes and lessons learned from processing Pu-238-contaminated waste. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Reduction of Plutonium in Acidic Solutions by Mesoporous Carbons

Batch contact experiments with several porous carbon materials showed that carbon solids spontaneously reduce the oxidation state of plutonium in 1-1.5 M acid solutions, without significant adsorption. The final oxidation state and rate of Pu reduction varies with the solution matrix, and also depends on the surface chemistry and surface area of the carbon. It was demonstrated that acidic Pu(VI) solutions can be reduced to Pu(III) by passing through a column of porous carbon particles, offering an easy alternative to electrolysis with a potentiostat.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗