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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

A Calibration to Predict the Concentrations of Impurities in Plutonium Oxide by Prompt Gamma Analysis Revision 2

This report documents the new PG calibration regression equation. These calibration equations incorporate new data that have become available since revision 1 of “A Calibration to Predict the Concentrations of Impurities in Plutonium Oxide by Prompt Gamma Analysis” was issued [3] The calibration equations are based on a weighted least squares (WLS) approach for the regression. The WLS method gives each data point its proper amount of influence over the parameter estimates. This gives two big advantages, more precise parameter estimates and better and more defensible estimates of uncertainties. The WLS approach makes sense both statistically and experimentally because the variances increase with concentration, and there are physical reasons that the higher measurements are less reliable and should be less influential. The new magnesium calibration includes a correction for sodium and separate calibration equation for items with and without chlorine. These additional calibration equations allow for better predictions and smaller uncertainties for sodium in materials with and without chlorine. Chlorine and sodium have separate equations for RICH materials. Again, these equations give better predictions and smaller uncertainties chlorine and sodium for RICH materials.

Instrumentation Related to Nuclear Science & Techn↗
DOE OSTI2025

Plutonium Oxidation State Distribution in the Presence of WIPP-Relevant Organics and Iron Corrosion Products

The oxidation state and solubility of plutonium (Pu) in high ionic strength synthetic WIPP (Waste Isolation Pilot Plant) brines as a function of pC H+ in the presence and absence of WIPP-relevant organic ligands (EDTA [Ethylenediaminetetraacetic acid], oxalate, citrate, acetate) and iron corrosion products (magnetite and metallic iron) at 𝑇 = 23 ± 2 ∘C was thoroughly studied by long-term batch solubility experiments (between approximately 800-1,100 days) from an undersaturation approach. The oxidation state of Pu in the WIPP environment has been a topic of interest since the initial Compliance Certification Application (CCA). This study aims to investigate the solubility of Pu under the expected WIPP conditions and to determine the oxidation state of the solid phase that will control the solubility. One of the most important results of this study is that the Pu oxidation state was analyzed both from the surface area of the corrosion products and in the precipitated solid. The analysis of the Pu oxidation state on the surface of the iron mineral from the ongoing undersaturated experiments is more relevant to the performance assessment of nuclear waste disposal than short term batch (plutonium-iron phase) experiments. The X-ray Absorption Near-Edge Spectroscopy (XANES) analysis showed that Pu oxidation state is different on the metal surface and in the precipitated solid. Pu(III) is the dominant oxidation state in the metallic iron (Fe 0 ) system in the presence and absence of organics. Pu(IV) is the dominant oxidation state in the magnetite system in the presence and absence of organics. Also, organics stabilize Pu(IV) in the magnetite system. Analysis of Pu in the precipitated solid by Extended X-ray Absorption Fine Structure (EXAFS) analysis showed that Pu formed an inner-sphere complex with iron with minor amounts of PuO 2 present. X-ray diffraction (XRD) results indicate that metallic iron and magnetite did not oxidize in three years in the alkaline and high ionic strength system. Under these conditions (8 < pC H+ < 10 at T = (22 ± 2) °C under nitrogen atmosphere, the solubility of Pu changes by up to three orders of magnitude (10 -5 and 10 -8 M). The spread in solubility is highest at pC H+ = 9. Pu(III) and Pu(IV) showed different solubility behavior in the synthetic WIPP brine. A summary of the data collected in this report will be submitted to Sandia National Laboratories as part of a parameter update report which will outline the changes to the OXSTAT parameter for the 2026 Compliance Recertification Application (CRA-2026). The experiments performed were done according to the U.S. Department of Energy (DOE) approved Test Plan entitled “Effects of Radiolysis, Organic Complexation, and Redox Conditions on the Speciation and Oxidation State Distribution of Pu(III/IV)” (LCO-ACP-25). All data reported were obtained under the Los Alamos National Laboratory-Carlsbad Office (LANL-CO) Quality Assurance Program, which is compliant with the DOE Carlsbad Field Office, Quality Assurance Program Document (CBFO/QAPD).

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

Plutonium Oxide Containment and the Potential for Water-Borne Transport as a Consequence of ARIES Oxide Processing Operations

The question of oxide containment during processing and storage has become a primary concern when considering the continued operability of the Plutonium Facility (PF-4) at Los Alamos National Laboratory (LANL). An Evaluation of the Safety of the Situation (ESS), “Potential for Criticality in a Glovebox Due to a Fire” (TA55-ESS-14-002-R2, since revised to R3) first issued in May, 2014 summarizes these concerns: “The safety issue of fire water potentially entering a glovebox is: the potential for the water to accumulate in the bottom of a glovebox and result in an inadvertent criticality due to the presence of fissionable materials in the glovebox locations and the increased reflection and moderation of neutrons from the fire water accumulation.” As a result, the existing documented safety analysis (DSA) was judged inadequate and, while it explicitly considered the potential for criticality resulting from water intrusion into gloveboxes, criticality safety evaluation documents (CSEDs) for the affected locations did not evaluate the potential for fire water intrusion into a glovebox.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Savannah River Site HB-Line Plutonium Oxide Production Process Simulation Model - 17458

The AFS II/Plutonium Oxide Production process is in its initial operational phase at the Savannah River Site's (SRS) HB-Line. The process is new for the facility where it is being performed, but the facility itself has been in use on and off for over 50 years. Beginning this process inside the facility has resulted in multiple process delays, due to both equipment issues and process restrictions. In order to better understand the process and to identify ways to improve facility performance, Savannah River Nuclear Solutions (SRNS), in conjuncture with Newport News Shipbuilding (NNS), developed the HB-Line Process Simulation Model. This tool completely replicates the operations that comprise the HB-Line process and simulates all of the constraints associated with the process. The model realistically accounts for the number of personnel required for a process step, the time required for a process step to occur, rules related to the parallel operation of process steps, and realistic equipment and operational delay data. The result is a tool that allows SRNS to test different scenarios for improving the process throughput, while realistically accounting for potential process delays and restrictions. The tool is currently in use and has allowed SRNS to present to their customer, the National Nuclear Security Administration (NNSA), estimated production capabilities over wide-ranging timetables and assumptions. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Potential hydrogen and oxygen partial pressures in legacy plutonium oxide packages at Oak Ridge

An approach to estimate the maximum hydrogen and oxygen partial pressures within sealed containers is described and applied to a set of packages containing high-purity plutonium dioxide. The approach uses experimentally determined maximum hydrogen and oxygen partial pressures and scales the experimentally determined pressures to the relevant packaged material properties. The important material properties are the specific wattage and specific surface area (SSA). Important results from the experimental determination of maximum partial pressures are (1) the ratio of hydrogen to oxygen is stoichiometric, and (2) the maximum pressures increase with increasing initial rates of production. The material properties that influence the rates are the material specific wattage and the SSA. The unusual properties of these materials, high specific wattage and high SSA, result in higher predicted maximum pressures than typical plutonium dioxide in storage. The pressures are well within the deflagration range for mixtures of hydrogen and oxygen.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Stability of plutonium oxide nanoparticles in the presence of montmorillonite and implications for colloid facilitated transport

The physical and chemical stability of PuO 2 nanoparticles (intrinsic colloids) in groundwater will control their transport and may affect the performance of high-level radioactive waste repositories. In this study, we examined the chemical stability of two types of PuO 2 nanoparticles at both 25 and 80 °C. The “alkaline” PuO 2 nanoparticles were prepared by neutralizing an acidic Pu(IV) solution with dilute NaOH to pH ~9.5. The “acidic” PuO 2 nanoparticles were precipitated from 0.1 M nitric acid by heating a Pu(IV) solution at 60–80 °C for 30 min. The chemical stability of these PuO 2 nanoparticles was tested in the presence of montmorillonite, a common mineral in the environment and potentially relevant backfill material in some nuclear waste repository designs. The “alkaline” PuO 2 nanoparticles were found to be unstable over a timescale of months at both 25 and 80 °C, with elevated temperature enhancing their dissolution rates and sorption to montmorillonite. PuO 2 nanoparticle dissolution rates decreased with increasing Pu concentration, consistent with solution saturation. The “acidic” PuO 2 nanoparticles appeared to remain stable for much longer than the “alkaline” PuO2 nanoparticles. The “alkaline” PuO 2 nanoparticle dissolution rate constants were as high as 10 -11.9±0.4 mol m -2 s -1 and 10 -11.2±0.2 mol m -2 s -1 at 25 and 80 °C, respectively, while the “acidic” PuO 2 nanoparticle dissolution rate at 80 °C was 10 -13.5 mol m -2 s -1 . Based on transmission electron microscopy, the “alkaline” and “acidic” PuO 2 nanoparticles were of similar size (2.5–4.5 and 2–3 nm nanoparticles, respectively). However, the “acidic” PuO 2 nanoparticles formed more ordered nanoparticle aggregates. Our results suggest that the specific conditions experienced during PuO 2 nanoparticle formation could significantly affect the stability of PuO 2 in the presence of competing sorption processes and, in turn, the relative importance of intrinsic versus pseudocolloid transport in the environment.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

MIS Shelf-Life Final Report for Plutonium Oxide Item CAN92 (SSR147) from Rocky Flats Analytical Laboratory Operations

A plutonium/uranium oxide material from the Material Identification and Surveillance (MIS) Program inventory has been studied to determine the gas generation and corrosion behavior in a storage environment. Sample CAN92 represents plutonium/uranium oxides stored in 3013 containers. The material originated in the analytical laboratory at Rocky Flats. This study followed over time the gas pressure and composition of a sample with nominally 0.5 wt% water in a sealed container with an internal volume scaled to 1/400th of the volume of a 3013 container. Gas compositions had been measured periodically over 5 ½ years. The maximum observed gas pressure from gas generation was 117 kPa. The increase over the initial pressure of 77.5 kPa was largely due to the generation of nitrogen and carbon dioxide with minor amounts of hydrogen and nitrous oxide. The internal components of SSR147 were inspected 6.5 years after it was removed from the array. The inside surfaces of the inner bucket exposed to the original sample for 1,937 days had an etched appearance and general corrosion. No pitting was observed on the inner bucket that held the sample.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗