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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 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Establishing Isotopic Measurement Capabilities using Laser-Induced Breakdown Spectroscopy for the Molten Salt Reactor Campaign

Proof-of-principle H isotope ratios of aqueous aerosol systems and liquid droplets on filter paper have been measured using laser-induced breakdown spectroscopy (LIBS) with root mean square error of prediction values down to 1.9%. Molten salt reactors (MSRs) will consist of a complex chemical and radiological system consistently producing new fission products as the reactor operates. Some of these fission products and/or their daughter species will leave the salt in the reactor off-gas. Monitoring the composition of the off-gas, as well as the salt itself, is important for monitoring reactor performance, including burnup, corrosion, and the concentration of impurities. Tritium is of concern for MSRs because it will be produced from the irradiation of key salt constituents, including Li and Be. LIBS offers an avenue for in situ salt and off-gas monitoring by firing a laser onto or into the sample stream to generate a plasma. The plasma light can be monitored to measure an elemental fingerprint of the sample. Extending this analysis to include isotopic ratios offers a critical expansion of the in situ monitoring capabilities being developed. This study demonstrates the expansion of Oak Ridge National Laboratory’s LIBS capabilities to monitor isotopes and shows how simple calibrations may provide rapid semiquantitative models.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

Evaluating Optical Techniques to Characterize Solid State Samples for the Pu-238 Supply Program

This report documents steps that have been taken to establish advanced characterization capabilities for solid-state samples to support the 238 Pu Supply Program. The program has already invested significantly in spectroscopy and online monitoring development for liquid processes. Many of the data, analytical methods, and equipment could also be leveraged for the analysis of Np/Pu oxides and Np pellets to help classify material properties and link them to operations. The techniques described in this work include diffuse reflectance spectroscopy (DRS), Raman spectroscopy, and laser-induced breakdown spectroscopy (LIBS). Each technique is sensitive to various chemical and/or elemental species and can provide complimentary information to more standard methods such as powder x-ray diffraction and scanning electron microscopy. These options are remotely deployable via fiber-optic cables. DRS and Raman spectroscopy are already approved for glove box and hot cell work, but LIBS requires US Department of Energy approval for incorporation. Raman spectroscopy does require laser shielding, which means that DRS is the easiest method to implement. However, each technique provides complimentary data, and the most robust sample characterization could be achieved when all three, among other methods, are harnessed together. This report documents some of the progress made testing these capabilities, some of the challenges, and next steps to optimize the technology and integration strategies.

07 ISOTOPE AND RADIATION SOURCES↗
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

Development of 211 At production at Crocker Nuclear Laboratory (Final Technical Report)

The focus of this effort was the development of the capability to produce and recover 211 At via the process 209 Bi(α, 2n) 211 At at the cyclotron at the Crocker Nuclear Laboratory at UC Davis. This effort required the design and fabrication of an internal production target, the development of a separation and processing area, and upgrades to the cyclotron to increase its reliability. There was a significant delay due to the pandemic lockdown, but ultimately we were able to produce and recover 211 At at the tens of µCi level using a wet chemistry method. Results of the project were presented at conference, but publication of a refereed article has been delayed by some discrepancies in understanding the calibration of total 211 At produced. We plan to repeat the production using internal funding, but first we want to revise our recovery to use a different technique, developed at the Texas A& M Cyclotron Institute.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Yield Calculations for Holmium-166M Production in the High Flux Isotope Reactor

This study is being completed in response to an assessment and commitment tracking system (ACTS) item that was opened during the production of 166m Ho. To satisfy the ACTS action item, cross section data of 166m Ho has been evaluated. Future 166m Ho production campaigns will employ the latest cross section data.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

Sum-of-Fractions Methodology for Actinides in Water- and Polyethylene-Moderated and -Reflected Systems

Sum-of-fractions is a method intended to make sure a subcritical margin for aqueous solutions and slurries of fissionable isotopes exists. The method indicates that a system is subcritical if the sum of the ratios of the mass of each isotope (in a mixture) to its individual minimum subcritical mass limit is less than or equal to one. Historically, the basis of the sum-of-fractions has been derived from allowances given in the American National Standards Institute (ANSI)/ American Nuclear Society (ANS)-8.15-1981. However, the allowance was removed in ANSI/ANS-8.15-2014 due to a lack of technical basis. A methodology was developed to assess the validity of using the sum-of-fractions for water- or polyethylene-moderated systems for the following nuclides: 232 U, 233 U, 234 U, 235 U, 237 Np, 236 Pu, 238 Pu, 239 Pu, 240 Pu, 241 Pu, 242 Pu, 241 Am, 242 m Am, 243 Am, 242 Cm, 243 Cm, 244 Cm, 245 Cm, 246 Cm, 247 Cm, 249 Cf, and 251 Cf. The methodology uses available benchmark data for mixtures of 233 U, 235 U, and 239 Pu to establish the calculational margin, and a mass limit reduction to establish the margin of subcriticality. Water- or polyethylene-moderated and -reflected mixtures containing the nuclides are evaluated with the code system, SCALE 6.2.4. Including the calculational margin, subcritical mass limits for each nuclide were computed for optimally water- or polyethylene-moderated and fully reflected systems. These masses were used to create nuclide mixtures in which the sum of the mass to subcritical mass limit ratios is one. The various nuclide mixtures were modeled over a range of moderation and demonstrate the keff does not exceed the calculational margin. For additional assurance of subcriticality, a significant mass reduction is applied to each computed minimum critical mass of the nuclides without adequate benchmark data consistent with the method in ANSI/ANS-8.15-2014.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

Micro-Quantification of Helium-3 and Helium-4 in TPBAR Components

This report documents the method development for measuring helium isotopes in micrometer-sized samples of tritium producing burnable absorption rod (TPBAR) components. Helium isotopes were measured as a tracer for tritium, which decays to 3 He with a half-life of 12.33 years. Getter and cladding materials from the TPBARs were analyzed, as they are designed to trap tritium. Therefore, constraining the diffusivity of tritium through these materials is of key importance. To first establish the reliability of the noble gas mass spectrometer, a reference gas with a relative 4 He/ 3 He ratio of 1000 was pre-mixed. This standard was measured several times to ensure measurements were reproducible. Unirradiated and irradiated getter and cladding samples of TPBARs were cut into 1-100 µm 3 cubes and analyzed for 3 He and 4 He content. The unirradiated materials had helium content equal to or less than that of the measured instrument background. Irradiated cladding also had instrument background levels of helium while irradiated getters had elevated levels of 3 He, interpreted to be the decay product of tritium. No diffusion of 4 He was observed in any of these materials, however, indicating that the 3 He detected in the irradiated getter was produced in situ after tritium diffusion and decay. These findings validate this method as a way to trace tritium diffusion in reactor materials.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

Chlorine Isotope Separations using Thermal Diffusion

As of the close of 2023 a thermal diffusion isotope separations (TDIS) apparatus was constructed, successful shakedown testing was achieved and enrichments of isotopic concentrations relative to natural abundance 35/37 Cl were collected. Further, the model for these enrichment experiments drove the timing for sampling and other critical, extrapolated functions that are discussed herein. Our decision to move forward in 2024 with the installation of a larger set of separation tubes and associated equipment was based on the successful development of the predictive model. The Chlorine Isotopes Project Team at PNNL is prepared to claim that the installation and hence its separative power is restricted only by the spatial limitations of the laboratory, and this at present appears to be the limiting feature to first pass high enriched 37 Cl.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2022

Improving Zr cross sections: 90 Zr(n, y) [Slides]

This presentation covers key take-aways such as the first of 4 isotopes (90,91,92,94) to be measured. 91 Zr is currently being measured at GELINA. Once all measurements are done a join evaluation with SAMMY will be undertaken. Further, there will be production of new evaluated resonance parameters and covariances. New data will be used to improve evaluation information, benefitting transport calculations of reactors, waste storage, etc.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2022

ORNL Contributions to the ENDF/B-VIII.1 Library [Slides]

For uranium and plutonium isotopes, evaluation work is converging to a stable configuration with an overall satisfactory benchmark performance (more information on the validation tests after CSEWG). Strontium evaluation was included in the repository library and successfully tested by processing codes relative to an alternative quantification of the external function. Cerium covariance matrices were updated to address review comments on the magnitude of the uncertainty. For future uncertainty quantification, theoretical observables should be properly decoupled from current measured guidelines. Tests to correctly include LP (from resonance parameters) fitted to measured energy-averaged data are in progress. Current ENDF files contains experimental LP data.

07 ISOTOPE AND RADIATION SOURCES↗
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 OSTI2024

FRAM In-Depth [Slides]

FRAM is an isotopic analysis code nominally designed for plutonium and uranium. It can also analyze other materials such as spent fuel (off all ages), medical isotopes.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

Mark-18A Cold Runs

The Savannah River National Laboratory (SRNL) is tasked by the National Nuclear Security Administration (NNSA) to recover highly valued isotopes from irradiated Mark-18A (Mk-18A) targets. The Savannah River Site (SRS) has sixty-five Mk-18A targets available for the recovery of the high valued materials. The sixty-five Mk-18A targets are currently stored in the L-Area Basin and will be removed one at a time and individually transported to SRNL. Upon receipt at SRNL, the Mk-18A target material will be removed from the confinement, dissolved, chemically separated, and calcined to a stable oxide. The flowsheet is designed to recover the plutonium as well as the trivalent actinides. The remaining unrecovered material will be discarded to the high activity drain (HAD) system in SRNL. A specially designed cask was procured for transport of the targets from L-Area to SRNL. Once received at SRNL, the targets will be loaded into the back of Cell 7 and resized as they enter the cell. The resized targets (1/4 lengths) will then be processed one at a time through the following processes: caustic dissolution and filtration; acidic dissolution and filtration, Reillex anion exchange, diglycolamide (DGA) cation exchange; and DGA calcination. This processing will result in two product streams. The first is an aqueous plutonium solution which will be removed from the shielded cells and taken to a glovebox for further purification and conversion to an oxide. The second is a calcined oxide containing the Am and Cm as well as other lanthanide fission products which will be removed from the shielded cells using a bagless transfer system. Both materials will be packaged for shipment to Oak Ridge National Laboratory (ORNL). All equipment to carry out this process was designed, procured or fabricated, and installed in a mock-up facility (716-4A) at SRS to allow for simulation testing in a non-radioactive area. This equipment was then dismantled and transferred from 716-4A to 773-A and installed in the SRNL Shielded Cells. After installation in the shielded cells facility testing was performed using water followed by surrogates and cold chemicals. Issues were identified during these evaluations, including equipment issues as well as technical challenges. Many of the issues were rectified during performance of the cold runs, and the remaining have a resolution identified. Table ES-1 provides a summary of all issues identified during the cold run operations, as well as the status and identified resolutions to outstanding issues.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2021

Production Facility Simulations for Annular LEU Targets

Eden Radioisotopes, LLC is designing a new molybdenum-99 (Mo-99) production facility based on a TRIGA-sized reactor with a core composed of low enriched uranium (LEU) targets. Reactor production is designed to exceed U.S. demand for Mo-99 using the fission processes. The nominal operational power is 1.8MW (less than 2.0MW, to satisfy the “non-power” reactor requirement) and desired irradiation scenarios include 7, 14, or 21 days of the irradiation for each target element. Safety limits for reactor operating margins are associated with such physical phenomena as fission gas release, fuel swelling, and stress cracking. As shown in the literature, one of the critical parameters defining safety margins for metallic uranium fuel is swelling. In its turn the fuel operational temperature is the main parameter impacting the swelling rate. This report documents the results of consecutive studies of reactor criticality, fission energy depositions, and cooling conditions for the target. The maximum temperature calculated for the LEU targets allows us to choose appropriate modeling approximation of the swelling. All obtained results refer to the preliminary targets and core designs provided by Eden. A criticality analysis was performed, and the results are listed mainly to cross-check Eden’s safety report and assume maximal neutron field disturbance for maximal reactivity. A brief description of the metallic uranium swelling model is provided in the Appendix.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Irradiation of Mo-100 Targets and Testing Fe(ll)CI 2 Precipitation for Tc-99 Removal

The production of molybdenum-99 (Mo-99) is a critical step in the generation of technetium-99m (Tc-99m), a radioisotope widely used in medical imaging. NorthStar Medical Radioisotopes, LLC is planning to produce the important medical radioisotope Mo-99 through a photonuclear reaction on molybdenum-100 (Mo-100). Accelerator production of Mo-99 using enriched Mo-100 targets yields undesirable isotopes, such as niobium-95 (Nb-95) and zirconium-95 (Zr-95). Previous studies reported that Nb and Zr isotopes can be effectively removed from Mo-99 products through coprecipitation with Fe(III). To enable the potential utilization of the first milking of Tc-99m from a Mo-99/Tc-99m generator, it is desirable to remove long-lived Tc-99. This can be accomplished by substituting Fe(III) with Fe(II) during the precipitation step, without affecting the removal of Zr and Nb isotopes. Previous experiments demonstrated up to 99+% removal of Tc using this method. It was also observed that the presence of hydrogen peroxide significantly impacts Tc removal. This was evident in the processing of enriched Mo-100 targets, where only 25% of Tc was removed. To further investigate this, another irradiation of enriched Mo-100 disks was conducted, followed by Tc-99 removal using Fe(II). Prior to irradiation, experimental conditions for Tc removal were optimized through several test runs using Mo-100 disks spiked with Tc-99. The results of these tests are discussed in this report.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Recovery of Enriched Mo-100 from Low Specific Activity Mo-99/Tc-99m Generator Waste Streams

This study assessed two potential techniques for the extraction of pure Mo-100 target material from Mo-99/Tc-99m waste streams: 1) an established solvent-extraction method tailored for Mo-99 spent solution recycling, and 2) a low-temperature molten salt electrochemical process. By making minor modifications to the conventional solvent extraction method, particularly to accommodate the altered solubility limits arising from elevated Na+ concentrations in the waste, we achieved quantitative Mo recoveries. Although the electrochemical technique offers advantages in scalability and processing simplicity, it proved ineffective in recovering Mo from a NaOH-KOH salt melt.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

Equivalency Factors and Mixed Isotope Subcritical Limits [Slides]

Equivalency factors (EF) are coefficients used to express the reactivity of a quantity of a given isotope in terms of an equivalent amount of another isotope’s reactivity. EFs are often used to conservatively determine if a given mixed-isotope system is within previously established limits. These EFs are calculated by taking ratios of established subcritical limits, also called the Rule of Fractions.

07 ISOTOPE AND RADIATION SOURCES↗