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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 523 records · Page 29
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Production of High Specific Activity 72 Se/ 72 As, 117m Sn and 203 Pb for Research and Clinical Applications: Effective target design, recycling of target material and radioisotope separation

This grant involved four objectives for producing high specific activity radionuclides using reactor and accelerator technologies that would find use in medical, industrial and research applications. This grant continued a collaboration between the scientists at the University of Washington (UW), the University of Missouri (MU) and Brookhaven National Laboratory (BNL) and addresses the need for high specific activity radionuclides, both reactor- and accelerator-produced, and for the training and education of radiochemists in isotope production, separations and precursor syntheses. All three institutions were involved in the projects, but to different degrees. The chemistry graduate students (Ph.D. program at MU) may have participated in an internship at one of the other institutions for training and project translation/facilitation.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

Mark-18A Loading Capacity and Dilute Acid Rinse of DGA Resin

Savannah River National Laboratory is developing a separations flowsheet for the recovery of valuable elements from irradiated 242 Pu targets. The primary impetus for this effort is to recover the rich amount of 244 Pu contained in the targets, however, the targets also contain other valuable isotopes such as heavy Cm and 241,243 Am. DGA Resin, developed by Eichrom Technologies Inc., was selected to recover these materials from the 7 – 9 M HNO 3 matrix raffinate of the anion exchange process used to separate Pu. The resin has a high affinity for trivalent actinides and rare earth elements (REEs) in moderate to strong nitric acid. After loading the resin, the extracted materials (including Cm and Am) are to be recovered as oxides in a two-step process by thermally drying and reducing the mass and volume of the resin in the process column followed by calcination of the resultant residue. It is desirable to reduce the amount of residual HNO 3 in the resin bed prior to these furnace operations, but the reduced acid concentration is known to lower the distribution coefficients of the components of interest to the extractant. The purpose of this study was to validate the loading capacity of the resin and determine losses to be expected from rinsing the loaded resin with dilute HNO 3 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Specification of FIPD Fission Gas Chemistry Data

The current FIPD library contains two main sets of fission gas chemistry data. The first set is data collected during the Integral Fast Reactor (IFR) program from 1984 to 1994, using a gas mass spectrometry system located in the Analytical Laboratory (AL) at Argonne National Laboratory-West (Argonne-West). Throughout this period, numerous fission gas release and chemistry datasets were gathered from a variety of metallic fuel pins. The fission gas was sampled by the Gas Assay, Sample and Recharge (GASR) System in the Hot Fuel Examination Facility (HFEF) and transferred to the AL to perform gas composition and isotopic abundance analysis. The second set is data collected after the IFR program. The fission gas samples were also collected by the GASR system at the HFEF, but analyzed using a similar gas mass spectrometer located in Pacific Northwest National Laboratory (PNNL). Many fuel pins irradiated in Experimental Breeder Reactor II (EBR-II) and the Fast Flux Test Facility (FFTF) were measured, including the fuel pins for the MFF series of experiments, designed to qualify metal fuel for use as driver fuel in the FFTF and X496 experiment. For either set of data, fission gas was sampled with the gas sampling line in GASR using sample bottles after the capsule/element volume has been determined and the system is still full of radioactive gas. The sample bottles were then transferred to the sample packaging cylinder or an approved storage location pending transfer to the AL or prepared for shipment to another laboratory (such as PNNL) for analysis of the collected gas as directed on the GASR data form, other approved form. The receiving laboratories (AL or PNNL) required their Analytical Service Request form to be completed prior to sample transfer. Typical sample transfer processes were initiated at HFEF by the principal or process engineer. The laboratories performing the analyses (AL or PNNL) use the sample bottle numbers as well as a sample number produced by the respective laboratory. HFEF and the responsible experimenter tracked the sample using the analysis number, the gas bottle number, and the fuel pin number.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Flammability and dispersion of tritium in confined release scenarios

Ignition of a flammable tritium-air mixture is the most probable means to produce the water form (T 2 O or HTO), which is more easily absorbed by living tissue and is hence ~10,000 times more hazardous to human health when uptake occurs compared to the gaseous form (T 2 or HT; per Mishima and Steele, 2002). Tritium-air mixtures with T 2 concentrations below 4 mol% are considered sub-flammable and will not readily convert to the more hazardous water form. It is therefore desirable from a safety perspective to understand the dispersion behavior of tritium under different release conditions, especially since tritium is often stored in quantities and pressures much lower than is typical for normal hydrogen. The formation of a flammable layer at the ceiling is a scenario of particular concern because the rate of dispersion to nonflammable conditions is slowest in this configuration, which maximizes the time window over which the flammable tritium may encounter an ignition source. This report describes the processes of buoyant rise and dispersion of tritium. Accumulation of flammable concentrations of tritium next to the ceiling is a common safety concern for hydrogen, but this situation can only occur if dispersion rates are slow with respect to rates of release and rise. Theory and simulations demonstrate that buoyancy does not cause regions with flammable concentrations to form within buildings from sources that have previously been mixed to sub-flammable concentrations. A simulated series of tritium release events with their associated dispersion behavior are reported herein; these simulations apply computational fluid dynamics to rooms with three different ceiling heights and a variety of tritium release rates. Safety related quantities from these simulations are reported, including the mass and volume of tritium occurring in a flammable mixture, the presence or absence of a flammable layer at the ceiling, and the time required for dispersion to nonflammable conditions after the end of the tritium release event. These safety metrics are influenced by the magnitude and rate of the tritium release with respect to the air volume in the room and also the momentum of the plume or jet with respect to the ceiling height. Several screening criteria are recommended to assess whether a specific tritium release scenario is likely to form a flammable layer at the ceiling. The methods and results in this modeling study have applicability to explosion safety analysis for other buoyant flammable gases, including the lighter isotopes of hydrogen.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

ICP-MS For Analysis of Lithium Isotopic Ratios in Materials Highly Enriched in 7Li - CRADA 626 (Abstract)

The purpose of this project is to develop analytical methods that can be deployed for analysis of lithium isotope enrichment products. One method involves rapid, high-throughput, relatively low precision analysis for direct monitoring of enrichment processes. A second method involves slower, but more precise analysis of final products of the enrichment process. We will use commercially available analytical equipment (quadrupole base inductively coupled plasma mass spectrometry and multi-collector magnetic sector inductively coupled plasma mass spectrometry) so that the analytical methods developed can be applied broadly.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Solid-state transformation of uranyl peroxide materials through high-level irradiation

The solid-state transformation of sodium uranyl triperoxide (Na 4 (UO 2 )(O 2 ) 3 ∙9H 2 O, NaUT) to sodium uranyl tricarbonate (Na 4 (UO 2 )(CO 3 ) 3 ) by radiolysis has been observed for the first time. The exposure of NaUT to 3 MGy gamma irradiation resulted in partial breakdown of the peroxides forming a mixed peroxide and carbonate species. The effects of He ion irradiation on NaUT was also investigated up to 225 MGy using both hydrated argon and dry argon. The complete conversion to the uranyl tricarbonate phase by 56 MGy using hydrated argon, while dry argon did not fully convert showing the importance of water in the system. He-ion irradiated NaUT samples all convert to the tricarbonate phase with time in air post radiation exposure. This transition was monitored via Raman spectroscopy, infrared spectroscopy (IR), and powder X-ray diffraction (PXRD) to further confirm the identity of the final product as the sodium uranyl tricarbonate, čejkaite. This transformation outlines a mechanism for the mobility of uranyl in natural environments and in the Hanford tanks.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Utilizing HYSPLIT for Emergency Response Modeling at SRS

The threat of a disaster happening at the Savannah River Site (SRS) is low, but not zero. When an emergency arises, emergency responders utilize a variety of tools to detect, track, and mitigate the disaster. HYSPLIT is a community atmospheric dispersion model that is highly configurable and has been used operationally to simulate particle, chemical, and radionuclide releases. We have developed a preliminary user interface (UI) that configures HYSPLIT to run for a variety of Emergency Action Level (EAL) scenarios at SRS. Using a hypothetical EAL scenario of an accidental release of Pu-238 in H-area and K-area onsite, an analysis was done to show how a preliminary UI framework allows HYSPLIT to be run on a terminal without the need form an active network connection. The study was successful in multiple aspects. For the preliminary UI, users were able to input certain characteristics of the hypothetical EAL such as hours of emission (how long was Pu-238 being released), curies of release, release start time (when does the model run start), and type of radionuclide directly into the terminal. For HYSPLIT, the model was successful in being able to take the UI input, calculate the results from the inputs and output multiple figures of both total volumetric airborne concentrations and surface deposition. We used the Pu-238 Derived Intervention Level (DIL) deposition thresholds for produce, dairy, and beef for visualization of the surface deposition, showing how a release would impact ingestion pathways.

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DOE OSTI2024

Assessment of Current MACCS Capabilities for Modeling Atmospheric Physical and Chemical Transformations

The physical and chemical transformation during atmospheric transport of radionuclides released into the environment has the possibility of impacting consequence modeling results. Accordingly, this report identifies physical and chemical transformations that may occur following release of chemically reactive radioactive species, how those transformations may affect modeling of consequences of release to the atmosphere and identifies current capabilities – in both MACCS and other state-of-practice atmospheric transport and dispersions models– to model those transformations. It was found that the inclusion of physical and chemical transformations is currently very limited in current state-of-practice codes for atmospheric dispersion of radionuclides. State-of-practice atmospheric dispersion codes appear to be typically limited to simulating either physical-chemical transformations or radioactive transformations, but not both. A state-of-practice atmospheric dispersion code capable of performing parallel physical, chemical, and radioactive transformation was not identified. A few atmospheric dispersion codes capable of modeling physical and chemical transport of specific species such as tritium or uranium hexafluoride were identified. Consequently, there is currently no information available that clearly suggests updates to the MACCS code are needed to bring it up to state-of-practice. However, investigations concluded that the MACCS computational framework can currently accommodate multiple physical/chemical forms in one simulation. Additionally, with some major assumptions, the computational framework in MACCS can accommodate parallel physical-chemical and radioactive transformations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

M3SF-24LL010302052-Comprehensive Analysis of Radionuclide Interaction with Hydrothermally Altered Repository Materials

This progress report (Level 3 Milestone Number M3SF-24LL010302052) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline Work Package Number SF-24LL01030205. The research is focused on actinide and radionuclide sequestration in hydrothermally altered repository materials. In FY24, we completed a rigorous analysis of Se sorption to iron oxide phases using our L-SCIE sorption database. This effort explicitly accounts for surface titration behavior of oxide surfaces that was the subject of a recently published manuscript (Han et al., 2023). With this in mind, our Se sorption analysis now yields a more robust workflow for developing self-consistent surface complexation modeling approaches that can be adapted to specific SCM conceptual and numerical approaches (i.e. non-electrostatic, diffuse layer, triple layer models). In late FY24, we plan to publish the results of our comprehensive surface complexation modeling of Se(IV) and Se(VI) sorption to iron oxide mineral phases and provide a path forward to developing robust radionuclide sorption models for use in performance assessment. In FY24, we also submitted a manuscript summarizing our approach to integrating radionuclide sorption and coprecipitation phenomena and evaluation of radionuclide partitioning values across a range of radionuclides relevant to performance assessment. We demonstrated our approach in detail using Se sorption and coprecipitation with iron oxide minerals as a test case. This manuscript was recently accepted for publication in Applied Geochemistry (Balboni et al., Accepted). We also continued experiments to identify radionuclide interaction with hydrothermally altered crystalline repository and backfill materials. Recent research performed at Los Alamos National Laboratory (LANL) and Sandia National Laboratory (SNL) has provided key insights regarding the hydrothermal alteration behavior of bentonite backfill in the presence of repository materials (steel, concrete, etc.). We are now examining how mineral alteration affects retardation behavior of a suite of radionuclides of interest to repository performance assessment. These experiments also allow us to test the predictive ability of our component additivity approach to surface complexation and ion exchange. Our guiding hypothesis is that a robust surface complexation/ion exchange model and associated database, developed using our L-SCIE approach, can effectively predict changes in radionuclide sorption behavior resulting from the hydrothermal alteration of mineralogy in a repository near field. A short update of results to date is presented below.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Investigation of Anion-Exchange Method for Purification of Fission-Produced 99 Mo

The LEU-Modified Cintichem (LMC) process is a small-scale (50- to 100-mL) method for purifying fission-produced 99 Mo. Traditionally, the process utilizes custom-made glassware and requires significant manual operations with hot cell manipulators. As an alternative to the LMC process, there is great interest in developing a 99 Mo purification method that could be automated to minimize remote handling while achieving the same purity specifications for the 99 Mo product. This report explores an ion-exchange approach to purifying fission-produced 99 Mo and discusses the decontamination factors for various fission products that are present after initial recovery of Mo on a titania column from a sulfate-based and uranium-containing solution.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2025

New charged-particle transport computational capability: the SIT code An L-4 milestone

We have developed a new high-fidelity code for direct transport of charged particles using the simple integral transport method. The code can be coupled to the outputs of any hydrodynamical simulation code in 1-D, 2-D or 3-D. In this report we summarize the formalism involved in treating complex transport problems. We present physical examples wherein we have used the code to calculate the transport of alpha particles. Future work is planned to study the sensitivity of hydrodynamical mix to charged-particle radiochemistry and reaction-in-flight neutrons for the complex inertial confinement fusion problems encountered at NIF and at the Z-machine.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Test Plan for DOE-GENIORS Dyanamic Irradiation Tests

Dynamic irradiation tests will be performed within the DOE-GENIORS collaboration, to be finished by the end of March 2021. These tests will be performed using three different setups, one at INL, one at CEA, and one at CIEMAT. The cis-mTDDGA/PTD chemical system will be used, applying both "extraction" (cis-mTDDGA - n-dodecane/HNO3) and "stripping" (cis-mTDDGA - n-dodecane/PTD - HNO3) conditions. This test plan provides the details and parameters to be used to perform irradiation at the INL using the INL Radiolysis Test Loop.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Assessment of Naturally Occurring Radioactive Material (NORM) in Illicit Drugs Using High-Resolution Gamma Spectroscopy

This report documents results assessing the presence of Naturally Occurring Radioactive Material (NORM) in illicit drugs using high-resolution gamma spectroscopy. Specifically, high-purity germanium (HPGe) measurements were conducted at the Drug Enforcement Administration (DEA) South Central Laboratory on 11 samples (referred to as exhibits) including cocaine, fentanyl, heroin, ketamine, LSD, marijuana, methamphetamines, psilocybin mushrooms, and synthetic cannabinoids.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Development of Solid Isotope Harvesting Methods in Preparation for FRIB (Final Report)

In a collaborative effort between Hunter College (HC), Lawrence Livermore National Laboratory (LLNL), and Michigan State University (MSU), we aimed to investigate the recovery of 88 Zr produced as the secondary beam at the National Superconducting Cyclotron Laboratory (NSCL) from solid collectors via solid isotope harvesting. We developed separation schemes to isolate Zr from sub-gram-scale collectors composed of various materials including carbon, aluminum, copper, tungsten, and gold. The solid harvesting endstation was constructed and then used as part of a dedicated beamtime at the NSCL using 88 Zr beam. After irradiation, the 88 Zr was radiochemically separated from each of the collector materials and the recovery efficiencies from each was assessed. The results of this work provide a path forward for harvesting hydrolysable metals at FRIB as a complementary approach to aqueous isotope harvesting.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Impact of Radiolysis on Iodine Speciation in a Variety of Matrices

This report details the work conducted in fiscal year 2023 with the aim of providing a better understanding of the speciation of iodine in support of domestic 99 Mo production Shine who uses a sulfate matrix in their process. Laboratory experiments to study the behavior of iodine speciation were conducted using spectroscopic methods including UV-vis and Raman as well as electrochemical studies. Radiolysis occurring in solution presents a unique challenge that is largely unaddressed with thermodynamic modeling, therefore a kinetic model was developed to address these issues. The focus of the studies conducted this year used surrogate radiolytic conditions induced by hydrogen peroxide for comparison to radiolytic conditions from direct gamma irradiation and neat acid solutions. For each case a model incorporating the kinetics was used to predict iodine speciation in the defined conditions where the output was directly compared to the experimental conditions. Further modeling was conducted incorporating the process conditions that are specific to Shine with incorporation of radiolysis and gas sparging.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

Predicting Radiation-Induced Plutonium Redox Chemistry using Multiscale Modeling Methods

Over the the last 70 years plutonium (Pu) has been integral in the development of several technologies that have changed the world, yet our fundamental understanding of its chemistry is still far from complete. This is a testament to this element?s unique and complex properties, such as its ability to coexist as multiple oxidation states in aqueous solution. Careful manipulation of plutonium oxidation states is essential in the study and utilization of its rich chemistry. To achieve this level of control, a comprehensive mechanistic understanding of radiation-induced plutonium redox chemistry is critical due to the unavoidable exposure of plutonium to ionizing radiation fields, both inherent and from in-process applications. For this reason, we have developed an experimentally evaluated multi-scale computer model for the prediction of gamma radiation-induced Pu(IV) redox chemistry in concentrated nitric acid solutions (1.0, 3.0, and 6.0 M).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Evaluations for neutron-induced activation cross sections for Y and Zr isotopes

Activation cross sections are an important input for evaluating results of radiochemical analyses, both for basic science and programmatic applications. We present an update on cross sections for a select set of Y and Zr target isotopes, including several isomers. This effort will focus on a methodology to obtain uncertainty quantified systematic trends for reaction model parameters and propagate them to cross sections. We discuss our results in the context of previous calculations.

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