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At least 361 records · Page 20

Safeguards Technology Development Program: FY 2024 Mid-Year Report

This project has 2 major thrusts and 2 minor tasks – One of the major ones is a scoping study for improving uranium isotopics by analyzing higher energy, lower yield U-235 gamma emissions. The second major one benefits past projects such as auto-enrichment, and peak-based analysis routines previously added to GADRAS-DRF [1]. The two minor tasks involve an in-person or remote GADRAS-DRF training for the IAEA, and characterizing detectors of interest.

07 ISOTOPE AND RADIATION SOURCES↗

Design of Hypothetical Processes for the Production of 131 I and 99 Mo from Activation Targets

For over six decades, medical isotope production has been a high-priority focus of many research reactors across the globe. The majority of these isotopes were produced using highly-enriched uranium (HEU) or low enriched uranium (LEU) – delivering millions of doses of diagnostic and therapeutic isotopes. As a consequence of this production, however, six decades of isotope production has resulted in massive quantities of spent uranium material worldwide with no known disposition pathway creating growing proliferation concerns. Supported by the National Nuclear Security Administration’s (NNSA) Material Management and Minimization (M3) program, there has been increased focus in the production of high-priority isotopes without special nuclear materials or without uranium altogether. Isotope production via activation can potentially fulfill regional isotope demands – particularly in under-developed regions without access to isotope supply chains. The benefits of this approach would be a reduction in uranium proliferation risks, less special nuclear material wastes, and reduced risk of supply disruption in the likely event that major isotope producers will again go off-line as has happened in recent years due to a number of factors.

07 ISOTOPE AND RADIATION SOURCES↗

Comparison of the sensitivity of 236 U measurements in environmental samples by MC-ICP-MS and ATONA based high precision U TIMS measurements

The ATONA project is focused upon exploring the improvements in uranium isotope ratio measurements by thermal ionization mass spectrometry (TIMS) provided by a new, capacitor-based, amplifier technology. These “ATONA” Faraday amplifiers (Isotopx Ltd, UK) promise accurate, low-noise measurements of very small signals (< 1 femto-amp) in a traditional Faraday cup, which was only previously possible using an ion counter. This report outlines a series of experiments that were performed to assess the performance of the system in samples that test our rapid analysis procedures, and then compare the results against other mass spectrometry techniques currently available for environmental analyses. The following major goals were achieved: (1) illustrated the importance of 236 U measurements for the screening and analysis of environmental samples; (2) improved sensitivity for 236 U, and then identified 236 U in the 4350B standard at ultra-trace levels (3) Provided comparison of the 236 U sensitivity to multi-collector inductively coupled mass spectrometry techniques (4) Illustrated high TRL for the ATONA based measurement technique. This completes the reporting requirements for task 4 in the project LCP and highlights the utility of the system to make highly sensitive 236 U measurements in programmatically relevant sample matrices and at relevant uranium concentrations.

07 ISOTOPE AND RADIATION SOURCES↗

GADRAS-DRF Enhancements for Safeguards – Custom Peak Fitting to Enhance Model Fitting and Isotopics

One major software update was accomplished within the Gamma Detector Response and Analysis Software-Detector Response Function (GADRAS-DRF) package. This update allows users to adjust individual peak fits for use in subsequent analysis processes within GADRAS-DRF. A graphical user interface (GUI) was implemented so users can see the effect of their fit adjustments on the spectrum. This new feature will enhance the capability of the previously funded auto-enrichment and peak-based 1D model fit feature that was implemented in FY23 (Fiscal Year). Isotopic analysis was performed using M400 data obtained from uranium standards and the isotopic assessment is given with and without manual peak adjustments.

07 ISOTOPE AND RADIATION SOURCES↗

Theranostic Radiopnictogens: 71 As, 72 As, and 119 Sb (Final Technical Report)

This project has developed new methods for the cyclotron production of medically relevant radionuclides 71 As and 119 Sb. Arsenic and antimony are chemically homologous elements (group 5A, also known as the pnictogens) that have radionuclides that are of considerable interest within nuclear medicine. Such radiopnictogens include the potentially therapeutic radionuclides 119 Sb (t 1/2 = 38 h) that decays with the emission of 24.5 low energy, high potency electrons per decay with little concomitant photon radiation and 77 As (t 1/2 = 39 h) that decays with average beta energy of 230 keV and diagnostic nuclides 71 As (t 1/2 = 65 h, 28% β+) and 72 As (t 1/2 = 26 h, 80% β+) for positron emission tomography (PET). This work has had major success developing new methods for the cyclotron production and radiochemical isolation of 71 As, supporting parallel developments for 119 Sb, and assessing the chemical similarities between these two homologous radionuclides. This project brought into collaboration two universities with complimentary skill sets, proficiencies, expertise, and facilities: the University of Wisconsin (UWisc) and the University of Missouri (Mizzou). Professors Ellison and Engle have experience in the small cyclotron production and radiochemical isolation of radionuclides, including 72 As and 119 Sb. Their recently developed metallurgic methods for fabricating cyclotron targets have great potential to expand and allow for the biomedical cyclotron production of long- lived, lower positron energy 71 As. Professors Hennkens and Jurisson have significant experience in the reactor production, radiochemical isolation, and biological functionalization of radioarsenic. Recent development of trithiol-based chelator molecules for functionalizing radioarsenic provide a platform for the investigation of the fundamental challenges of the promising low-energy-electron emitter, 119 Sb. Through their positions within their respective University’s graduate schools, the PIs and Co-Is effectively trained of graduate students and postdoctoral researchers in nuclear and radiochemistry, sub-specialties specifically identified in the Department of Energy (DOE) Office of Science Isotope Program long-range plan. Annual laboratory research visits for students between UWisc and Mizzou provided essential broad-field experience and scientific networking that is critical for maintaining their path along the training pipeline to productive careers in isotope production. This research collaboration has provided significant benefits to the DOE University Isotope Network and radionuclide-using researchers around the country.

07 ISOTOPE AND RADIATION SOURCES↗

Report on New and Upgraded National User Facilities in Basic Energy Sciences

On December 1, 2023, the Director of the of the Office of Science (SC) charged all the Department of Energy Office of Science Federal Advisory Committees to respond to look toward the scientific horizon and identify what new or upgraded facilities will best serve the SC community needs in the next ten years (2024-2034). This report by the Basic Energy Sciences Advisory Committee (BESAC) assess facilities for the Basic Energy Sciences (BES) program.

07 ISOTOPE AND RADIATION SOURCES↗

“Production of High Specific Activity 155 Tb, 161 Tb and 203 Pb for Research and Clinical Applications: Effective Target Design, Target Material Recycling and Radioisotope Separation”

Radioisotopes are essential for the development and application of radiopharmaceuticals that target specific diseases, such as cancer, offering unique potential for precision medicine. The growing demand for theranostic radioisotopes underscores their critical role in personalized medicine, where they enhance diagnostic imaging, minimize patient radiation exposure, and improve targeted tissue uptake, particularly in receptor- and antigen-directed therapies. The theranostic pair terbium-155 (diagnostic) and terbium-161 (therapeutic) holds significant promise for advancing individualized, targeted, and dosimetry-driven radiotherapies. However, the United States currently lacks routine and reliable production of these isotopes. This project made significant progress toward addressing this supply issue by developing production and separation methods for terbium-155 and terbium-161 while also training the next generation of the nuclear and radiochemistry workforce. This grant also strengthened collaboration between scientists at the University of Washington, the University of Missouri and Brookhaven National Laboratory. The research effort focused on evaluating target preparation methods, optimizing irradiation parameters, and refining isolation processes. In addition, the project provided extensive hands-on training to graduate students and postdoctoral fellows, equipping them with expertise in radioisotope production technologies and fostering the growth of the nuclear science workforce.

07 ISOTOPE AND RADIATION SOURCES↗

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↗

Investigating Similarity Differences for Light-water-Moderated and Polyethylene-Moderated Systems

Oak Ridge National Laboratory has performed validation studies in support of Pacific Northwest National Laboratory’s analysis of the Sum-of-Fractions method. Work in a companion paper examines the validation methods and results for various mixtures of fissile isotopes in various concentrations moderated and reflected by water and polyethylene. Those results indicate a greater coverage of critical experiments for validating water moderated and reflected systems versus those moderated and reflected with polyethylene.

07 ISOTOPE AND RADIATION SOURCES↗

Consistent $\overline{ν}$ evaluation for minor Pu isotopes with CGMF

This report follows up on the evaluation work done in 2023 where we developed a procedure and performed the first consistent evaluation of the average prompt neutron multiplicity for minor Pu isotopes, including 238,240-242 Pu, using CGMF. Details on the necessary updates to the release version of CGMF, the experimental data and experimental uncertainty quantification that went into the evaluation, and this first evaluation effort are documented in and will not be repeated in this report. Instead, we discuss here the further investigations into the CGMF model space to improve the evaluation results from FY23. Additionally, we note that these evaluation results have been transformed into the ENDF format for mean values and covariances, and validation with critical assemblies has been performed; that work is documented elsewhere. In this short report, we discuss the updated evaluation efforts performed during FY24 in Sec. 2, show results from CGMF for other prompt fission observables in Sec. 3, and then briefly conclude in Sec. 4.

07 ISOTOPE AND RADIATION SOURCES↗

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

The intent of this project was to determine appropriate methodologies for analysis of lithium isotopes for 1) quasi-online monitoring of isotope separations, and 2) high-precision characterization of end-products, including lithium fluoride and lithium-beryllium fluoride (FLiBe). Traditionally, isotopic analysis requires the use of expensive, sophisticated instrumentation with often relatively long analytical timelines. We determined that the use of cheaper, smaller, and easier-to-operate instruments are sufficient for rapid analysis of lithium isotopes to monitor isotope separation efficiencies. In addition, we found that the analytical precision afforded by these lower-cost instruments is comparable to the more sophisticated (i.e., more expensive) instrumentation when the isotopic composition of lithium becomes highly depleted in 6Li. This finding will ultimately help lower costs of manufacturing of depleted lithium that is required for operation of certain designs of Generation IV nuclear reactors.

07 ISOTOPE AND RADIATION SOURCES↗

A Robust Assessment of High-Precision Plutonium Isotopic Analysis by Thermal Ionization Mass Spectrometry [Slides]

TIMS at SRNL • SRNL consolidated analytical laboratories and services into one area – loss of TIMS capability during relocation. • SRNL installed a new Thermo Scientific TRITON Plus TIMS in our Category II Nuclear Facility to re-establish the lab’s TIMS capabilities in Feb. 2024. • Allows for handling, preparation, purification, and analysis of high-level radiological materials within a single location • Pu and U isotopic composition and assay measurement qualification have been priority since installation. • Once the instrument has been qualified, this capability will support internal and external customers.

07 ISOTOPE AND RADIATION SOURCES↗

Characterization of the Multi-Coincident Bismuth Germanate Oxide Spectrometer at the Nuclear Counting Facility

A multi-detector γ-ray spectroscopy system including 3 high-purity germanium (HPGe) detectors has been developed at the Nuclear Counting Facility at Lawrence Livermore National Laboratory. This system operates not only in conventional singles γ-ray detection mode but also incorporates features like coincidence and anti-coincidence techniques. These advanced detection modes can significantly enhance the system’s sensitivity, making it a powerful tool for isotope identification and quantification, especially for complex samples with high background and overlapping peaks. In this re port, we present a comprehensive performance characterization of the Multi-Coincident Bismuth Oxide Spectrometer (MCBOS) using a variety of sample types, including 60 Co, 48 Sc, and mixed fission product samples. Each sample provides unique tests for the MCBOS capabilities. Additionally, a GEANT4 model of the MCBOS has been generated to aid with the characterization of the system.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radiation Dose Modeling for Niowave’s Accelerator Driven Uranium Target Assembly 3

Molybdenum-99 is a high-value radionuclide commonly used for medical purposes within the United States. The National Nuclear Security Administration (NNSA) seeks to reliably produce the radioisotope 99 Mo without the use of highly enriched uranium. NNSA’s Office of Material Management and Minimization (M3) provides funding and government laboratory expertise to private companies to expedite the production process domestically and currently funds designs that use low-enriched uranium or other 99 Mo production pathways. Several production designs are being explored across the industry, including uranium fission and photonuclear conversion of 100 Mo targets. Niowave Inc. seeks to produce 99 Mo via a high-energy electron accelerator that strikes a lead-bismuth eutectic target that ultimately produces a consistent neutron flux. The neutron flux then interacts in a subcritical reactor core configuration to produce fission in low-enriched or natural uranium targets. These fissionable targets are then processed to extract 99 Mo. The purpose of this work is to estimate the neutron and photon dose response across Niowave’s proposed facility for worker safety during operation. Owing to the size of the proposed Niowave facility and necessary shielding, unbiased Monte Carlo radiation transport is impractical, and variance reduction methods are required. This work focuses on the weight window variance reduction method to produce high confidence dose response results within a Monte Carlo radiation transport code. Specifically, an adjoint-informed weight window methodology was created to improve the dose response estimates for accelerator-driven subcritical reactor designs. This adjoint-informed methodology was implemented for Niowave’s proposed design and improved dose results at far-field locations across the facility. Acceptable dose rate contours for the proposed facility were generated across the facility and are presented in this work.

07 ISOTOPE AND RADIATION SOURCES↗

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↗

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↗

Feasibility of Isotopically Tailored Low Activation Materials

Materials employed in future fusion reactors and advanced fission reactors are susceptible to activation and transmutation due to fast neutron flux, which drives the need for Low Activation Materials for survivability, maintenance, and long-term disposal considerations. This paper investigates the feasibility of using ORNL’s planned enrichment technologies to produce isotopically enriched or depleted materials for use in future reactor construction. We focus on identifying isotopes of interest and performing estimates of the required scale of enrichment to impact future design and operation.

07 ISOTOPE AND RADIATION SOURCES↗