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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Packaging Plan for Mark-18A Plutonium Oxide

Mark-18A (Mk-18A) targets were irradiated at the Savannah River Site and have been in wet storage at the site since the 1970s. The Mk-18A Target Material Recovery Program has been established to recover the 244 Pu and heavy curium (≥50% 246 Cm and 248 Cm) in the targets at the Savannah River National Laboratory (SRNL) and ship the materials to Oak Ridge National Laboratory’s (ORNL’s) Radiochemical Engineering Development Center for programmatic use. Two products will be recovered from the Mk- 18A targets for shipment from SRNL to ORNL: a plutonium oxide stream and an oxide material that will contain the americium, curium, and lanthanides. This document presents the plan for packaging of the plutonium oxide material for shipment and storage at ORNL.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2023

Report on the Analysis of Plutonium-238 Oxide, Campaign #P5PO

Oak Ridge National Laboratory (ORNL) is currently producing Plutonium-238 oxide for NASA space programs. Through the irradiation of NpO 2 pellets in the High Flux Isotope Reactor (HFIR), the production of Pu-238 oxide will be used for electrical power and heat on NASA spacecraft such as the Curiosity Mars Rover and the Voyager 1 and 2. The Transuranium Analytical Laboratory (TAL) leads the analytical effort for this project, which includes the dissolution of plutonium product oxide (PUP) and the analysis of the dissolved product solution using both radiological and inductively coupled plasma mass spectrometry (ICP-MS) techniques that are required to meet product specifications. The Transuranic Analytical Laboratory received three samples of Pu-238 oxide for analysis in January of 2022. This report documents the analytical protocols performed by the TAL along with the results produced from said analytical protocols. This report also includes a comparison with the general-purpose heat source (GPHS) specifications.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2022

Capability to Process and Characterize Uranium-Zirconium (U-Zr) and Uranium-Zirconium-Plutonium (U-Zr-Pu) Alloys

This work investigated co-reduction of anhydrous compounds of uranium, zirconium, and plutonium to produce uranium rich ternary nuclear fuel alloys. Metallothermic co-reduction is a novel method to produce all-metal nuclear fuels. Metal fuels offer thermal, fissility, compatibility, and security benefits over oxide fuels. Alloys of uranium–10% zirconium with plutonium contents of 0%, 2.5%, 5%, and 10% were produced, with yields of 60–85% of theoretical values in a traditional calciothermic bomb reduction apparatus. Microstructural analysis indicated transformation of uranium phase from gamma to beta and then alpha, in alternating lamellar plates typical of alpha phase uranium and delta phase uranium-zirconium, with zirconium and carbides at prior grain boundaries. Some of the analyses were inconclusive in their results and therefore require additional testing. Successful ternary co-reduction would simplify production of homogeneous feedstock and thereby streamline manufacture of homogeneous ternary metallic fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

APPLICATION OF INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY IN THE ANALYSIS OF PLUTONIUM CONTENT OF FAST CRITICAL ASSEMBLY FUEL DISPOSITION

Outline • Fast Critical Assembly (FCA) Plutonium Fuel Disposition • Brief campaign overview • Savannah River National Laboratory • Analytical capabilities and instrumentation • Typical FCA sample analysis process • Plutonium analysis by quadrupole-inductively coupled plasma-mass spectrometry (Q-ICP-MS) • Method description/development • Instrumentation • Data/control charts

Bonilla, Henry J. [Savannah River National Laborat↗
DOE OSTI2023

Plutonium Signatures in Molten-Salt Reactor Off-Gas Tank and Safeguards Considerations

Fluid-fueled molten-salt reactors (MSRs) are actively being developed by several companies, with plans to deploy them internationally. The current IAEA inspection tools are largely incompatible with the unique design features of liquid fuel MSRs (e.g., the complex fuel chemistry, circulating fuel inventory, bulk accountancy, and high radiation environment). For these reasons, safeguards for MSRs are seen as challenging and require the development of new techniques. This paper proposes one such technique through the observation of the reactor’s off-gas. Any reactor design using low-enriched uranium will build up plutonium as the fuel undergoes burnup. Plutonium has different fission product yields than uranium. Therefore, a shift in fission product production is expected with fuel evolution. The passive removal of certain gaseous fission products to the off-gas tank of an MSR provides a valuable opportunity for analysis without significant modifications to the design of the system. Uniquely, due to the gaseous nature of the isotopes, beta particle emissions are available for observation. The ratios of these fission product isotopes can, thus, be traced back to the relative amount and types of fissile isotopes in the core. This proposed technique represents an effective safeguards tool for bulk accountancy which, while avoiding being onerous, could be used in concert with other techniques to meet the IAEA’s timeliness goals for the detection of a diversion.

Dunkle, Nicholas (ORCID:000000027323011X)↗
NASA NTRS1972

Some neutron and gamma radiation characteristics of plutonium cermet fuel for isotopic power sources

Gamma and neutron measurements on various types of plutonium sources are presented in order to show the effects of O-17, O-18 F-19, Pu-236, age of the fuel, and size of the source on the gamma and neutron spectra. Analysis of the radiation measurements shows that fluorine is the main contributor to the neutron yields from present plutonium-molybdenum cermet fuel, while both fluorine and Pu-236 daughters contribute significantly to the gamma ray intensities.

Neff, R. A.↗
NASA NTRS1972

Plutonium-244 fission tracks - Evidence in a lunar rock 3.95 billion years old.

Tracks attributed to the spontaneous fission of plutonium-244 and of uranium-238 were detected in a large whitlockite crystal in the lunar breccia 14321 from the Fra Mauro formation. For a track-retention age of 3.95 b.y., the number of plutonium tracks relative to the number of uranium tracks is 0.51 plus or minus 0.15, provided that the rock was not heavily neutron-irradiated 3.95 b.y. ago.

Hutcheon, I. D.↗
DOE OSTI2025

Control Selection for the Neutralization Tank in the Aqueous Recovery System at the Savannah River Plutonium Processing Facility

The Aqueous Recovery System (ARS) at the Savannah River Plutonium Processing Facility (SRPPF) recovers and purifies plutonium (Pu) using aqueous chemistry techniques. The neutralization tanks in the ARS collect waste streams with various impurities and greatly reduced concentrations of Pu than are produced during aqueous processing. Criticality safety is primarily achieved in the ARS by using geometrically favorable process vessels. However, due to the geometry of neutralization tanks, each tank is administratively limited to no more than 450 g Pu, thus representing the transition from geometry to mass control. To ensure that this mass limit is not exceeded, an administrative control requires taking two samples of any solution to be sent to a neutralization tank. Normal operations are expected to result in less than 50 g Pu in a neutralization tank filled to its capacity of 250 L. Process upsets may cause an inadvertent transfer of up to 1000 g Pu to a neutralization tank, producing a system that is potentially not subcritical for all possible configurations of the tank. To ensure that a neutralization tank remains safety subcritical, passive engineered controls (e.g. changing tank geometry or adding fixed poisons), active engineered controls (e.g. interlocks), and administrative controls (e.g. soluble poisons and valve isolation) were considered and their viability evaluated. Ultimately, the team chose an administrative, dual-valve isolation strategy. This paper will thoroughly discuss the various control strategy options and why many of the options were not feasible for maintaining criticality safety.

Dressman, Phillip M. [Savannah River Nuclear Solut↗
DOE OSTI2025

Control Selection for the Neutralization Tank in the Aqueous Recovery System at the Savannah River Plutonium Processing Facility

The Aqueous Recovery System (ARS) at the Savannah River Plutonium Processing Facility (SRPPF) recovers and purifies plutonium (Pu) using aqueous chemistry techniques. The neutralization tanks in the ARS collect the waste streams, containing various impurities and greatly reduced concentrations of Pu, that are produced during aqueous processing. Criticality safety is primarily achieved in the ARS by using geometrically favorable process vessels. However, due to the geometry of neutralization tanks, each tank is administratively limited to no more than 450 g Pu, thus representing the transition from geometry to mass control. To ensure that this mass limit is not exceeded, an administrative control requires taking two samples of any solution to be sent to a neutralization tank. Normal operations are expected to result in less than 50 g Pu in a neutralization tank filled to its capacity of 250 L. Process upsets may cause an inadvertent transfer of up to 1000 g Pu to a neutralization tank, producing a system that is potentially not subcritical for all possible configurations of the tank. To ensure that a neutralization tank remains safety subcritical, passive engineered controls (e.g.changing tank geometry or adding fixed poisons), active engineered controls (e.g. interlocks), and administrative controls (e.g. soluble poisons and valve isolation) were considered and their viability evaluated. Ultimately, the team chose an administrative, dual-valve isolation strategy. This paper will thoroughly discuss the various control strategy options and why many of the options were not feasible for maintaining criticality safety.

Dressman, Phillip M. [Savannah River Nuclear Solut↗
DOE OSTI2022

A Machine Learning Method for the Forensics Attribution of Separated Plutonium

Plutonium (Pu) source attribution would be a powerful tool to support nuclear nonproliferation efforts. This capability to find the source of a Pu sample would act as a deterrent to smuggling efforts, and also help regulatory agencies verify declared nuclear activities. Work at Texas A&M University yielded a nuclear forensics methodology, which is capable of determining separated Pu’s reactor of origin, fuel burnup, and the time since irradiation (TSI)—three parameters of interest. The methodology used a set of ten intra-element isotopic ratios found in separated Pu, which was compared to a library of isotopic ratio values produced using neutronics simulations for reactors of interest. By calculating the probability that unknown Pu sample’s isotopic ratio set matched a set in the library, the methodology could predict the three parameters of interest of the sample. One shortcoming of this methodology was an inability to correctly attribute spoofed Pu, where Pu sourced from two different reactors or two different fuel burnup levels are mixed. A new methodology to rectify this vulnerability using machine learning (ML) technique is developed, instead of the maximum likelihood calculation previously used and the results are satisfactory. The ML approach leverages the existing simulated data for training the algorithm, but use them efficiently by only using intra-element isotope ratios that contribute to the attribution one of the three parameters at a time. Previously, all isotope ratios were used to attribute all three parameters together. The new methodology attributes the Pu parameters in three steps, one for each parameter, rather than resolving all of the three parameters simultaneously like the previous maximum likelihood approach. First, a support vector machine classifier with a set of seven isotopic ratios finds the reactor of origin and a set of regression models trained using gaussian process predicts the burnup with a different set of seven isotopes. Finally, TSI is calculated analytically using decay equations. Thus far, the new methodology is capable of attributing pure Pu samples and has been validated using experimental data. The next step will to be augment the classifier training data set with spoofed Pu data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
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 OSTI2025

Unique & challenging aspects of plutonium metal standards exchange program for actinide measurements

The Los Alamos National Laboratory exchange program is the only program of its kind for the distribution of plutonium (Pu) standards materials with a range of impurity contents to multiple laboratories for destructive measurements of elemental concentration. This paper discusses statistical methods used to address challenges in Pu metal exchange data by way of two case studies. Challenges include how to evaluate a data set when a large fraction of the values are minimum detection limits (MDLs), and how to determine potential outliers with limited in-formation on the true spread of the data.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Influence of ethylenediaminetetraacetic acid on the long-term oxidation state distribution of plutonium

Here, spectrophotometry was used to study the effect of EDTA on plutonium oxidation state distribution as a function of time, pH, and ligand-to-metal ratio (L/M) under anoxic conditions. Novel Pu(V)-EDTA absorption bands were identified at 571, 993, 1105, and 1150 nm with molar absorption coefficients of 15 ± 1, 6 ± 1, 10 ± 1, and 10 ± 1 cm –1 M –1 , respectively. Pu(V)-EDTA spectral changes occurred at L/M < 1, indicating only Pu V O 2 (EDTA) 3- formed with logK = 3.6 ± 0.3. Time-resolved experiments showed EDTA drastically increased the Pu(V/VI) reduction rate, which we propose is driven by amine lone-pair electron donation and the oxidative decarboxylation of EDTA. Oxidation of Pu(III)-EDTA to Pu(IV)-EDTA occurred on a slower time scale (110–237 days) than previously reported (<15 min) and is hypothesized to be radiolysis driven. Pu(V/VI)-EDTA and Pu(III)-EDTA both approached Pu(IV)-EDTA stabilization over time, yet Pu(V/VI)-EDTA solubility data was ≥ 1.0 log 10 units higher than predicted by Pu(IV)-EDTA solubility models, indicating that current thermodynamic models are incomplete. Ultimately, the data show EDTA preferentially stabilizes Pu(IV) over time regardless of initial oxidation state, but Pu(V)-EDTA can persist under environmentally-relevant conditions, emphasizing the need to continue investigating redox reactions, speciation, and behavior of these complexes to support the transuranic waste disposal and surface remediation/containment efforts.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Parabolic oxidation kinetics of a plutonium alloy at room temperature

Auger electron spectroscopy (AES) was used to characterize the oxide scale formed on an ~0.5 wt. % Ga plutonium metal alloy. Analysis of changes to the characteristic Auger transitions for Pu and O during sputter depth profiles were used in combination with previously measured sputter yields to determine the thickness of the oxide scale and provide insight into its chemistry. From this data, the parabolic kinetics for the Pu-Ga alloy were determined as a function of relative humidity, RH = 14–92%, and oxygen partial pressure, p(O 2 ) = 31–157 Torr, at 25°C. For each relative humidity investigated, the parabolic rate constant was found to be independent of oxygen partial pressure. Furthermore, power-law fits to the relative humidity effect on the rate constant was found to have a power of n = 1.265, indicating the diffusion species which rate-limits the reaction isn’t molecular water, which subsequent dissociates at the oxide-metal interface, or hydroxyl from dissociation at the gas-surface interface.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Morphological and chemical characteristics of oxide scales formed on δ-Phase plutonium metal alloys I: 3.5 at% ga

Focused ion-beam scanning electron microscopy (FIB-SEM) and three-dimensional (3D) microscopy were applied to characterize the subsurface morphological features of oxide scales formed on an ~3.5 at.% Ga plutonium (Pu) metal alloy. Using the FIB-SEM technique, a number of morphological features formed in the interior of the oxide scale from Pu metal's environmental exposure were observed and identified. Here, Auger electron spectroscopy (AES) was utilized to characterize the cross-sectional composition and chemistry of the oxide scale. The oxide scale formed during inert storage and operational environments has a characteristic internal scale structure that includes a relatively dense oxide layer with some lateral and transverse cracking. Generally, after subsequent exposure to dry air environment, the oxide scale retained most of the original structural and chemical characteristics. However, after aging in a moist air environment, while the oxide scale was found to maintain the chemical characteristics of the source oxide, the scale was found to be on average thinner and without the previously observed internal microcracking, likely the result of spallation of the source scale during exposure to the new environment.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Morphological and chemical characteristics of oxide scales formed on δ-phase plutonium metal alloys II: 2.0 at% Ga

The focused ion-beam scanning electron microscopy (FIB-SEM) and three-dimensional (3D) microscopy were applied to characterize the subsurface morphological features of oxide scales formed on an ~2.0 at. % Ga plutonium (Pu) metal alloy. Using the FIB-SEM technique, a number of morphological features formed in the interior of the oxide scale from Pu metal’s environmental exposure were observed and identified. Auger electron spectroscopy (AES) was utilized to characterize the cross-sectional composition and chemistry of the oxide scale. The oxide scale formed during inert storage and operational environments was found to be highly variable in thickness and morphology, presenting some regions with a thin (<400 nm), dense oxide layer and others with a thick (>2 µm) scale with substantial lateral cracking. After subsequent exposure to dry air environment, the oxide scale became thicker (~4 µm) and slightly more porous. The changes following aging in a moist air environment were observed to be more severe, with the formation of a highly porous internal structure containing significant lateral and transverse cracking. In comparison to the scale formed on an ~3.5 at. % Ga-Pu metal alloy, the oxide morphology of the lower gallium alloy investigated here exhibited greater variation in thickness and a noteworthy dependence on the presence of water vapor, particularly in terms of the internal porosity formed during growth of the oxide.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Improved plutonium and americium photon branching ratios from microcalorimeter gamma spectroscopy

Photon branching ratios are critical input data for activities such as nuclear materials protection and accounting because they allow material compositions to be extracted from measurements of gamma-ray intensities. Uncertainties in these branching ratios are often a limiting source of uncertainty in composition determination. Here, we use high statistics, high resolution - (60–70 eV full-width-at-half-maximum at 100 keV) gamma-ray spectra acquired using microcalorimeter sensors to substantially reduce the uncertainties for 11 plutonium ( 238 Pu, 239 Pu, 241 Pu) and 241 Am branching ratios important for material control and accountability and nuclear forensics in the energy range of 125 keV to 208 keV. Lastly, we show a reduction in uncertainty of over a factor of three for one branching ratio and a factor of 2–3 for four branching ratios.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗