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At least 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Closure Report for Corrective Action Unit 412: Clean Slate I Plutonium Dispersion (TTR) Tonopah Test Range, Nevada, Revision 0

This Closure Report (CR) presents information supporting the clean closure of Corrective Action Unit (CAU) 412: Clean Slate I Plutonium Dispersion (TTR), located on the Tonopah Test Range, Nevada. CAU 412 consists of a release of radionuclides to the surrounding soil from a storage–transportation test conducted on May 25, 1963. Corrective action investigation (CAI) activities were performed in April and May 2015, as set forth in the Streamlined Approach for Environmental Restoration (SAFER) Plan for Corrective Action Unit 412: Clean Slate I Plutonium Dispersion (TTR), Tonopah Test Range, Nevada; and in accordance with the Soils Activity Quality Assurance Plan. The purpose of the CAI was to fulfill data needs as defined during the data quality objectives process. The CAU 412 dataset of investigation results was evaluated based on a data quality assessment. This assessment demonstrated the dataset is complete and acceptable for use in fulfilling the data needs identified by the data quality objectives process. This CR provides documentation and justification for the clean closure of CAU 412 under the FFACO without further corrective action. This justification is based on historical knowledge of the site, previous site investigations, implementation of the 1997 interim corrective action, and the results of the CAI. The corrective action of clean closure was confirmed as appropriate for closure of CAU 412 based on achievement of the following closure objectives: Radiological contamination at the site is less than the final action level using the ground troops exposure scenario (i.e., the radiological dose is less than the final action level): Removable alpha contamination is less than the high contamination area criterion: No potential source material is present at the site, and any impacted soil associated with potential source material has been removed so that remaining soil contains contaminants at concentrations less than the final action levels: and There is sufficient information to characterize investigation and remediation waste for disposal.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Advanced Waste Management Concepts for Uranium and Plutonium Multi-Recycling - 18533

The multiple recycling of plutonium and uranium will play a major role in gradually achieving a fully closed nuclear fuel cycle in the future, once the first Generation IV fast reactors (FR) are deployed in the NPP fleet. To reach this objective, optimizations of current processes and technologies and, in some cases, the development of innovative concepts are required to meet the scientific, technical and economic challenges imposed by the treatment of spent fuels with an increasingly higher Pu content. Based on the significant past experience acquired by France in LWR and FR MOX fuel treatment, the CEA is running R and D studies to develop new efficient processes for Pu recycling and for FR MOX fuel fabrication. More compact and economically competitive processes, ensuring the safety/security of the facilities (particularly as regards criticality and proliferation resistance) have to be developed taking into account that the amounts of plutonium involved will be one order of magnitude higher than in UOX fuels. New concepts of head-end treatment, dissolution, and separation have been proposed. Consequently, effluent and waste management must be adapted to these processes and to the characteristics of fast reactor MOX fuels. New waste treatment processes are suggested: 1) Cladding waste and undissolved metallic particles could be treated simultaneously in a melting process. The molten metal could be decontaminated by a specific slag and the oxides recovered, in particular PuO{sub 2}, would be recycled at the frond-end of the process, 2) Fission Products and Actinides (FPA) containment glass will also be optimized to accommodate significant amounts of iron, nickel and chromium coming from hull corrosion, and / or decontamination slag coming from the metal melting process. 3) New peraluminous-type glass formulations are under development to accept increased amounts of FPA, as well as iron, nickel, and chromium. The first trials to evaluate the melting process have indicated that metallic compounds from the dissolution residues could be easily incorporated into a molten metal at levels of 1, 2 and 3 w%. (authors)

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

Dissolution of aerosol particles collected from nuclear facility plutonium production process

Here, a simple, robust analytical chemistry method has been developed to dissolve plutonium containing particles in a complex matrix. The aerosol particles collected on Marple cascade impactor substrates were shown to be dissolved completely with an acid mixture of 12 M HNO 3 and 0.1 M HF. A pressurized closed vessel acid digestion technique was utilized to heat the samples at 130 °C for 16 h to facilitate the digestion. The dissolution efficiency for plutonium particles was 99 %. The resulting particle digestate solution was suitable for trace elemental analysis and isotope composition determination, as well as radiochemistry measurements.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2015

Evaluating bis(2-ethylhexyl) methanediphosphonic acid (H 2 DEH[MDP]) based polymer ligand film (PLF) for plutonium and uranium extraction

This paper describes a new analyte extraction medium called polymer ligand film (PLF) that was developed to rapidly extract radionuclides. PLF is a polymer medium with ligands incorporated in its matrix that selectively and quickly extracts analytes. The main focus of the new technique is to shorten and simplify the procedure for chemically isolating radionuclides for determination through alpha spectroscopy. The PLF system was effective for plutonium and uranium extraction. The PLF was capable of co-extracting or selectively extracting plutonium over uranium depending on the PLF composition. As a result, the PLF and electrodeposited samples had similar alpha spectra resolutions.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Investigation of process history and underlying phenomena associated with the synthesis of plutonium oxides using Vector Quantizing Variational Autoencoder

Accurate, high throughput, and unbiased analysis of plutonium oxide particles is needed for analysis of the phenomenology associated with process parameters in their synthesis. Compared to qualitative and taxonomic descriptors, quantitative descriptors of particle morphology through scanning electron microscopy (SEM) have shown success in analyzing process parameters of uranium oxides. Among other candidates, a neural network called a Vector Quantizing Variational Autoencoder (VQ-VAE) has shown the ability to quantitatively describe particle morphology to attain >85% accuracy in identifying uranium oxide processing routes. We utilize a VQ-VAE to quantitatively describe plutonium dioxide (PuO 2 ) particles created in a designed experiment and investigate their phenomenology and prediction of their process parameters. PuO 2 was calcined from Pu(III) oxalates that were precipitated under varying synthetic conditions that related to concentrations, temperature, addition and digestion times, precipitant feed, and strike order; the surface morphology of the resulting PuO 2 powders were analyzed by SEM. A pipeline was developed to extract and quantify useful image representations for individual particles with the VQ-VAE, then further reduce the dimensionality of the feature space using a bottlenecking neural network fit to perform multiple classification tasks simultaneously. The reduced feature space could predict process parameters with greater than 80% accuracies for some parameters with a single particle. They also showed utility for grouping particles with similar surface morphology characteristics together. Both the clustering and classification results reveal valuable information regarding which chemical process parameters chiefly influence the PuO 2 particle morphologies: strike order and oxalic acid feedstock. Doing the same analysis with multiple particles was shown to improve the classification accuracy on each process parameter over the use of a single particle, with statistically significant results generally seen with as few as four particles in a sample.

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

Evidence of an oxidation induced phase transformation for a delta phase plutonium-gallium alloy

The oxidation of an ~1.5 at% Ga plutonium metal alloy in dry air as a function of time was studied using a combination of FIB-SEM, AES, and XRD. Analysis of SEM images of FIB cross-sections of the oxide allowed for direct measurement of the oxide thickness as well as determination of heterogeneity in the extent of the oxide. AES analysis performed on cross-sections of the oxide allowed for quantitative analysis of the atomic composition and semi-quantitative analysis of the chemical composition. Initial preparation of the sample was found to induce a martensitic transformation to α' - Pu with an average thickness of 233 nm. Electropolishing was found to be sufficient to fully remove the α' layer with creation of only a minimum oxide layer. Growth of the oxide in dry air was found to initially follow parabolic kinetics, with a parabolic rate constant orders of magnitude higher than expected for δ-Pu but in-line with values extrapolated to room temperature for α-Pu. Following complete oxidation of the initial α` layer, further regions of plutonium metal depleted in gallium were observed to form at the oxide / metal interface. However, gallium, as Ga 2 O 3 , was found to be enriched at the surface and present in the oxide in an amount comparable to the relative Ga:Pu ratio of the bulk metal alloy. Finally, the results presented here serve to bridge a diverse array of previous experimental and theoretical data and provide the first comprehensive view of the fate of the δ-stabilizer during formation of an oxide.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Development of small-scale plutonium electrorefining in molten CaCl 2

Molten salt extraction and electrorefining of plutonium were successfully conducted with only a 200-g initial charge. Due to this small scale, the electrorefining cell components were redesigned relative to conventional, multi-kg standards. The efficiency and yield of this small-scale process are comparable to those of larger-scale exemplars. Chemical analysis of the plutonium product and the anode heel is presented. Here, the product was 99.8% pure. The anode heel was able to be depleted beyond the expected freezing point without significant impurity carryover.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

Determination of total plutonium content in spent nuclear fuel assemblies with the differential die-away self-interrogation instrument

As a part of the Next Generation Safeguards Initiative Spent Fuel project, we simulate the response of the Differential Die-away Self-Interrogation (DDSI) instrument to determine total elemental plutonium content in an assayed spent nuclear fuel assembly (SFA). We apply recently developed concepts that relate total plutonium mass with SFA multiplication and passive neutron count rate. In this work, the multiplication of the SFA is determined from the die-away time in the early time domain of the Rossi-Alpha distributions measured directly by the DDSI instrument. Here, we utilize MCNP to test the method against 44 pressurized water reactor SFAs from a simulated spent fuel library with a wide dynamic range of characteristic parameters such as initial enrichment, burnup, and cooling time. Under ideal conditions, discounting possible errors of a real world measurement, a root mean square agreement between true and determined total Pu mass of 2.1% is achieved.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2015

Superconductivity in plutonium compounds

Although the family of plutonium-based superconductors is relatively small, consisting of four compounds all of which crystallize in the tetragonal HoCoGa 5 structure, these materials serve as an important bridge between the known Ce- and U-based heavy fermion superconductors and the high-temperature cuprate superconductors. Additionally, the partial localization of 5f electrons that characterizes the novel electronic properties of elemental plutonium appears to be central to the relatively high superconducting transition temperatures that are observed in PuCoGa 5 , PuRhGa 5 , PuCoIn 5 , and PuRhIn 5 .

36 MATERIALS SCIENCE↗
DOE OSTI2022

Experiments of water-moderated plutonium metal arrays: part I — description

In the mid-1970s and early 1980s, almost one hundred critical and approach-to-critical experiments using water-moderated plutonium metal arrays were performed at the Rocky Flats Critical Mass Laboratory. The experiments were performed in two programs: 2x2xN arrays conducted in the 1970s and 3x3x3 arrays conducted in the 1980s. Both sets of experiments used the same double-canned plutonium parts and were water moderated. The major differences between the two programs were the support structure and tank and the administrative limits on criticality. This paper summarizes the critical data and results of both sets of experiments. In conclusion, these experiments are then analyzed in a companion paper.

42 ENGINEERING↗
DOE OSTI2018

Automated Separation of Uranium and Plutonium from Environmental Swipe Samples for Multiple Collector Inductively Coupled Plasma Mass Spectrometry

A fully automated method for the separation of low-concentration uranium from plutonium in environmental swipe samples has been developed. The offline chromatography system features renewable 1 mL Eichrom TEVA and UTEVA column generation from bulk resin slurry. Discrete fractions of the separated actinides are delivered into user defined vials for future analysis. Clean room background levels were achieved outside of a cleanroom environment with this method. Purification of uranium and plutonium from various sample matrixes and at various concentrations was successful. Major and minor isotope ratios for both elements were measured via multiple collector inductively coupled plasma mass spectrometry and were in good agreement with certified reference values. Lastly, validation of the separation method was conducted on archived environmental samples and agreed with values previously reported using standard column chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Plutonium Speciation and Oxidation State Distributions in the Presence of Citrate

We explored the speciation and kinetics of the Pu(VI)-citrate and Pu(III)-citrate systems (pH m = 2.5–11.0, I = 0.1 M NaCl, T = 23 °C, O 2 (g) < 2 ppm) using ultraviolet–visible–near-infrared (UV–vis–NIR) spectrophotometry, solvent extraction, and PHREEQC modeling. Formation constants were determined for PuO 2 (HcitH)(aq) (log K° 1,1 = 1.09 ± 0.05) and PuO 2 (HcitH)(citH) 3– (log K° 1,2 = -0.20 ± 0.07), and evidence for (PuO 2 ) m (citH –k ) n (OH) x 2m(3+k)n–x was identified under alkaline conditions. Pu(VI) species were found to be less stable in the presence of citrate than in the absence of citrate (t ≤ 168 days); the rate of reduction increased with increasing pH. Further, the direct reduction of Pu(VI) to Pu(IV) was required to fit experimental data in the presence of citrate but did not improve the fit for Pu in the absence of citrate. We also observed increased Pu(III) stability in the presence of citrate (t ≤ 293 days), with higher concentrations of Pu(III) favored at lower pH. Finally, we provide evidence of a radiolysis-driven mechanism for the citrate-mediated reduction of plutonium that involves electron transfer from the oxidative breakdown of citrate. Our work highlights the need to investigate the redox effect of organic ligands on plutonium oxidation states under repository-relevant conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Oh, My Darling Clementine: A Detailed History and Data Repository of the Los Alamos Plutonium Fast Reactor

The Los Alamos Plutonium Fast Reactor, Clementine, provided the first fast neutron spectrum using a metallic plutonium fuel system and liquid mercury coolant. Clementine is often mentioned in the history of fast, metal-fueled, or metal-cooled designs, with little public information regarding the specifications or timeline. This paper contains a synopsis of each report regarding the development, operation, experimental results, failures, and subsequent disassembly of Clementine to explore this unique reactor within the context of modern advanced reactor development.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2023

Dose reconstruction for plutonium-239 intakes at the Rocky Flats Plant

Purpose: The Rocky Flats (RF) Plant was a weapons manufacturing facility that operated from the early 1950s to 1989. Its primary missions were the production of plutonium (Pu) pits for thermonuclear weapons and the processing of retired weapons for Pu recovery. The purpose of this study was to estimate radiation doses to a cohort of 4499 RF workers from an intake of 239 Pu, the primary plutonium isotope handled at the site. Materials and methods: The latest biokinetic models of the International Commission on Radiological Protection, or site-specific variations of those models, were used to estimate 239 Pu intakes for each worker based on model fits to bioassay data often coupled with lung measurements. Results: Urinary excretion and lung retention data for most 239 Pu intakes could be fit reasonably well by a mixture of Pu dioxide and moderately soluble material. For some workers, better fits were obtained by application of other absorption types including Type S, 239 Pu nitrate, or pure 239 Pu dioxide, or by assuming intake via a wound. The lungs typically received the highest tissue doses, with fifty-year committed equivalent doses in the range of 0.5–1 Sv for 275 workers, 1–5 Sv for 115 workers, and greater than 5 Sv for 12 workers. Conclusions: RF was a unique site regarding a large number of lung measurements available for determining the appropriate absorption types for inhaled material. Further, this provided higher confidence in reconstructed 239 Pu doses than is generally gained from urinary data alone.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2024

Distribution of plutonium and radium in the human heart

Since 1968, the United States Transuranium and Uranium Registries (USTUR) has studied the biokinetics and tissue dosimetry of uranium and transuranium elements in nuclear workers. As part of the USTUR collaboration with the Million Person Study of Low-Dose Health Effects, radiation dose to different parts of the human heart is being estimated for workers with documented intakes of 239 Pu or 226 Ra. The study may be expanded for workers with intakes of 238 U and other radionuclides. The distribution of radionuclides, expressed in terms of concentration (Bq per kg of tissue) serves as an important parameter for estimating radiation dose. Based on available organs from workers who donated their bodies or tissues for research, nine undissected hearts were selected: seven from USTUR registrants with plutonium exposure (males) and two individuals with radium intakes (female and male). For the plutonium workers, estimated 239 Pu systemic deposition ranged from <74 Bq to 1765 Bq. Estimated 226 Ra ‘initial systemic intakes’ were 10.1 MBq and 14.8 kBq for the female patient and male worker, respectively. Organ dissection was based on a heart model published by Borrego et al (2019 J. Radiol. Prot. 39 950–65). This model includes nine cardiac substructures: aorta, left main coronary artery, left atrium, left anterior descending artery, left circumflex artery, left ventricle, right atrium, right coronary artery, and right ventricle. In addition, heart valves, fat attached to epicardium, fluids, and a coronary bypass graft were collected resulting in 111 samples that are currently undergoing radiochemical analyses and mass-spectrometric measurements. The 239 Pu and 226 Ra evaluations are not completed. The results of this study are intended to support radiation worker health studies by improving associated dosimetric and epidemiological models.

USTUR↗
DOE OSTI2017

THE MAYAK WORKER DOSIMETRY SYSTEM (MWDS-2013) FOR INTERNALLY DEPOSITED PLUTONIUM: AN OVERVIEW

The Mayak Worker Dosimetry System (MWDS-2013) is a system for interpreting measurement data from Mayak workers from both internal and external sources. This paper is concerned with the calculation of annual organ doses for Mayak workers exposed to plutonium aerosols, where the measurement data consists mainly of activity of plutonium in urine samples. The system utilises the latest biokinetic and dosimetric models, and unlike its predecessors, takes explicit account of uncertainties in both the measurement data and model parameters. The aim of this paper is to describe the complete MWDS-2013 system (including model parameter values and their uncertainties) and the methodology used (including all the relevant equations) and the assumptions made. Where necessary, supplementary papers which justify specific assumptions are cited.

Bayesian analysis' retrospective dosimetry↗
DOE OSTI2023

People are like plutonium

An analogy is drawn between the study of human behavior and the study of plutonium to demonstrate that soft and hard sciences are more similar than different, making the distinction moot and unproductive. The studies of human behavior and plutonium follow a common scientific research cycle that aligns with Thomas Kuhn’s views of scientific change. This common research cycle provides evidence that the thought processes and methodologies required for success are congruent in the soft and hard sciences. The primary implication from this analogy is that scientists in all disciplines should eradicate the distinction between soft and hard sciences. Focusing on similarities rather than differences among researchers from different disciplines is necessary to enhance collective intelligence and the type of transdisciplinary collaboration required to tackle difficult sociotechnical problems. CCS Concepts: • Social and professional topics • User characteristics • Cultural characteristics.

96 KNOWLEDGE MANAGEMENT AND PRESERVATION↗
DOE OSTI2012

Los Alamos National Laboratory and Lawrence Livermore National Laboratory Plutonium Sustainment Monthly Program Report September 2012

In September of 2012 the Plutonium Sustainment program at LANL completed or addressed the following high-level activities: 1) Completed assembly, inspection, packing, and approvals for Pollux. Completed shipment to DAF in early October in accordance with the Gemini Core Team’s schedule. 2) Delivered the draft Program Implementation Plan and revised repeatedly. 3) Met with Kansas City Plant staff to “kick-off” the non-nuclear pit-component production mission. All MRT L2 Milestones 4195-4198 or the relevant PBIs associated with Plutonium Sustainment have been met and evidence packages submitted. The year-end budget/performance indices were 0.96 (S.P.I.) and 1.00 (C.P.I.). Table 1 identifies all Baseline Change Requests (BCRs) that were initiated, in process, or completed during the month. The earned value metrics overall for LANL are within acceptable thresholds, so no high-level recovery plan is required. Note that the planned (budget) and earned value for September includes planned carryover holdbacks (no allocation) with no associated FY12 costs. This has a minor (positive) impact on S.P.I. and a significant (positive) impact on the C.P.I. For Pu Sustainment overall, the C.P.I. in September neglecting the $10.75M holdback is 0.90. Likewise, the C.P.I. for FY12 is 1.004. With the facility infrastructure element removed, the C.P.I. in September becomes 0.92. Likewise, the C.P.I. for FY12 is 0.992. Again neglecting the holdback, the S.P.I. numbers for Pu Sustainment overall are 0.94 (Sept) and 0.96 (FY12) and with the facility infrastructure element removed 0.95 (Sept) and 0.95 (FY12).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗