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29 records · Page 2
All sourcesNASA NTRSDOE OSTI
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 OSTI2025

Actinide 5f Occupations: The Case of PuO 2

In actinide chemistry, the formal number of open-shell 5f electrons, n open , is a well-defined quantity with an integer value. The effective 5f occupation, n f , additionally takes donation and back-donation into account, generally has a non-integer value, and has varying numerical definitions. The present study explores the important distinction between n f and n open in actinide chemistry with the example of PuO2, by using electronic structure methods with a relativistic Hamiltonian in combination with experimental Pu M 5 -edge high-energy-resolution X-ray absorption and emission spectroscopic data. The total donation to the metal in PuO 2 is between 3.1 and 2.4 electrons, depending on the type of calculation, most of which is to the Pu 6d and 5f shells. The donation into 5f is sensitive to the approximations in the electronic structure model but likely amounts to 1.6/0.8 electrons when the diffuse regions of the 5f shell are included/excluded. Valence band resonant inelastic X-ray scattering experiments demonstrate that Pu 5f electron density is present in the valence band; thus, there is a clear experimental signature of covalent bonding in PuO 2 . Pu M 5 -edge and M 3 -edge high-energy-resolution X-ray absorption near-edge structures for Pu 3+ and Pu 4+ in an aqueous solution are compared to PuO 2 , showing that Pu in PuO 2 has an nf closer to Pu 4+ (aq).

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

Numerical Simulation of Container Breach and Airborne Release of Solids Due to Mechanical Insults

Throughout U.S. Department of Energy (DOE) complexes, safety engineers employ the five-factor formula to calculate the source term (ST) that includes parameters of airborne release fraction (ARF), respirable fraction (RF) and damage ratio (DR). Limited experimental data on fragmentation of solids, such as ceramic pellets (i.e., PuO2), and container breach due to mechanical insults (i.e., drop and forklift impact), can be supplemented by modeling and simulation using high fidelity computational tools to estimate these parameters. This paper presents the use of Sandia National Laboratories' SIERRA solid mechanics (SM) finite element code to investigate the behavior of the widely utilized waste container (such as 7A Drum) subject to a range of free fall impact and puncture scenarios. The resulting behavior of the container is assessed, and the estimates are presented for bounding DRs from calculated breach areas for the various accident conditions considered. This paper also describes a novel multiscale constitutive model recently implemented in SIERRA/SM that simulates the fracture of brittle materials such as PuO 2 and determines ARF during the fracture process. Furthermore, comparisons are made between model predictions and simple bench-top experiments.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2020

Variation in plutonium dioxide sputter yields for 1–5 keV Ar+ ions

An oxide layer with a known thickness and chemistry was grown on delta stabilized Pu and sputtered with 1–5 keV Ar+ ions over a range of incident ion angle between 22° and 72°. From the time required to remove the oxide layer, sputter yields of PuO2 were calculated. The sputter yields appear to increase with higher Ar+ ion beam energy in the range of 1–5 keV at an incident sputter ion angle of 42° and were found to increase with a decreasing angle of incidence up to 62°. The degree of oxide reduction induced during the sputter process was found to vary with the incident sputter ion angle.

Donald, Scott B.↗
DOE OSTI2025

Analysis of Radioactive Waste and Contamination using 3D Position-Sensitive CdZnTe Detectors

INTRODUCTION The US has surplus plutonium. This material will be diluted in gloveboxes at SRS [Ref 1 and 2]. This process will create holdup. Holdup is material in an unexpected or unwanted location. Because this holdup material is primarily PuO2, it must be accounted for (measured). This measurement is typically done using a liquid-nitrogen cooled, HPGe detector. To enable more rapid processing, advanced holdup technologies are being explored [Ref 3 and 4]. METHODS For the surplus plutonium dilute and dispose program, the traditional detector system could slow down the optimal operational tempo of the program. A multiple-detector system, providing complete glovebox coverage, based on CdZnTe crystals, 3D-positioning electronics, and a coded aperture mask, is in the process of being developed by ORNL and SRNL [Ref 4].

Whiteside, Tad [Savannah River National Laboratory↗
NASA NTRS1972

The response of a 0.03-cm silicon detector to a mixed neutron and gamma field as a function of shield material and thickness

The neutron and gamma radiation from a MHW-RTG was used to evaluate the total response of a shielded 0.3-mm silicon detector. The generator employs a 2200 W(th) PuO2 heat source concept known as the HELIPAK. The total integrated neutron and gamma ray fluxes at 100 cm away from the source along the radial direction were 1.67 x 1,000 n/sq cm/s and 1.49 x 10,000 gamma sq cm/s, respectively. Experimental values of the response function of the shielded silicon detector were used to determine the total counting rates due to photons at bias energies ranging from 50 to 200 keV. For neutrons, analytically computed response functions were used to determine the total counting rates at the same bias energies. It was found that for an aluminum shield the neutrons are not significant, regardless of the thickness of the shield. However, the magnitude of the total counting rate due to neutrons increases with increased atomic number of the shield and becomes comparable to the counting rate due to photons for a platinum shield thickness of 5 cm.

Taherzadeh, M.↗
NASA NTRS1976

The SNAP 27 gamma radiation spectrum obtained with a Ge/Li/ detector

The pulse height distribution, obtained experimentally using a Ge(Li) detector, was employed to determine the photon emission rate characteristic of a PuO2 fuel source known as the SNAP 27 heat source. The selfshielding parameters of the photon emitter, the efficiency of the detector and the geometry of the experiment were utilized to determine the unscattered photon emission rate of the source and the unscattered flux spectrum at a certain specified distance from the source. For the scattered part of the flux spectrum a Monte Carlo technique was employed so that the total flux spectrum could be determined at any point in the radiation field. As a result of this work, a technique was developed to obtain the unfolded radiation spectrum of the SNAP 27 heat source.

Taherzadeh, M.↗
NASA NTRS2007

Development of Advanced Stirling Radioisotope Generator for Space Exploration

Under the joint sponsorship of the Department of Energy and NASA, a radioisotope power system utilizing Stirling power conversion technology is being developed for potential future space missions. The higher conversion efficiency of the Stirling cycle compared with that of Radioisotope Thermoelectric Generators (RTGs) used in previous missions (Viking, Pioneer, Voyager, Galileo, Ulysses, Cassini, and New Horizons) offers the advantage of a four-fold reduction in PuO2 fuel, thereby saving cost and reducing radiation exposure to support personnel. With the advancement of state-of-the-art Stirling technology development under the NASA Research Announcement (NRA) project, the Stirling Radioisotope Generator program has evolved to incorporate the advanced Stirling convertor (ASC), provided by Sunpower, into an engineering unit. Due to the reduced envelope and lighter mass of the ASC compared to the previous Stirling convertor, the specific power of the flight generator is projected to increase from 3.5 to 7 We/kg, along with a 25 percent reduction in generator length. Modifications are being made to the ASC design to incorporate features for thermal, mechanical, and electrical integration with the engineering unit. These include the heat collector for hot end interface, cold-side flange for waste heat removal and structural attachment, and piston position sensor for ASC control and power factor correction. A single-fault tolerant, active power factor correction controller is used to synchronize the Stirling convertors, condition the electrical power from AC to DC, and to control the ASCs to maintain operation within temperature and piston stroke limits. Development activities at Sunpower and NASA Glenn Research Center (GRC) are also being conducted on the ASC to demonstrate the capability for long life, high reliability, and flight qualification needed for use in future missions.

Chan, Jack↗
DOE OSTI2020

Review of the General-Purpose Heat Source Module Reduction and Monitoring Processing at INL

A thorough review of the Module Reduction and Monitoring (MRM) process was conducted to evaluate the efficacy of processing. The degree of reduction was calculated using the mass balance of oxygen contained in carbon monoxide (CO) and carbon dioxide (CO 2 ) removed from all fuel processed between January 2014 through August 2019. The plutonia was slightly reduced from O/Pu ratio of 2.0 to a range of 1.991 to 1.999. The review evaluated publications generated when MRM processing was developed and performed at the Mound Laboratory. A similar degree of reduction was measured at Mound in the 1982 paper authored by Ernie Johnson as well as MRM processing of IHS-60 and some Cassini-era fuel. The original 1982 paper documenting the reduction process reported a mass balance reduction to 1.9931 yet reported a total reduction to ~1.98 (Johnson 1990). The IHS-60 and Cassini reductions were calculated at 1.995 and 1.997 using the number of moles of CO and CO 2 removed as published in a clad pressurization investigation report (Merten, et all 1995). MRM process changes are recommended to improve the accuracy of the CO partial pressure calcualtion.

42 ENGINEERING↗
DOE OSTI2022

Potential safety impacts associated with production of gaseous PuF 6 due to reactions between 3013-compliant PuO 2 with Novec TM 1230 at temperature

A part of the NNSA/SRNS Surplus Plutonium Disposition (SPD) project is a planned expansion of an existing facility with capabilities to handle, process, package, and characterize large amounts of plutonium oxide materials for permanent disposition at WIPP. The facility design for this future processing capability will include glovebox operations, HEPA filters, and exhaust/ventilation systems. An NNSA review of the facility support systems included comments on the potential residual reactivity of previously-stabilized PuO 2 , and on the possibility of chemical interactions between stabilized PuO 2 and a new fire suppressant (Novec TM 1230), a replacement for chlorinated/brominated compounds such as HALON TM , to be employed in the event of a room/glovebox fire where PuO 2 will be processed.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗