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Improved Cross Sections From Group T-2 For 11 B, 151 Eu, 153 Eu, and 165 Ho

Group T-2 has recently completed neutron-induced cross-section evaluations for 11 B, 151 Eu, 153 Eu, and 165 Ho. Evaluations for the latter three isotopes are described in Ref. 1. We have prepared cross-section tables based on the new evaluations for use in C-Division deterministic and Monte Carlo codes. Before describing how to access the new data for your calculations, we will compare some characteristics of the new data with previously available data. ZAID identifiers for the new and old data are listed in Table I, along with the source of the old data.

07 ISOTOPE AND RADIATION SOURCES↗

Radiolysis and radionuclide production in a flowing-water target during fast 40 Ca 20+ irradiation

Here, a flowing-water target was irradiated with a 140 MeV/u, 8 nA 40Ca20+ beam to test the feasibility of isotope harvesting at the upcoming Facility for Rare Isotope Beams. Among other radionuclides, 2.6(2)E-6 48Cr and 5.6(5)E-6 28 Mg nuclei were formed for every impingent 40Ca and were collected through ion exchange. Radiolysis-induced molecular hydrogen evolved from the target at an initial rate of 0.91(9) H2 molecules per 100 eV of beam energy deposited. No radiation-accelerated corrosion of the target material was determined.

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Low Count and Background Radionuclides Analysis - 20488

The US Department of Energy (DOE) is often faced with the need to evaluate radionuclides at low concentrations. When site sample data are likely to be close to threshold activity concentrations of interest, then the means by which the radiochemical analysis is performed and reported is critical. This situation can occur when differentiating from zero (presence/absence) for radionuclides that do not occur naturally, close comparison with environmental background for naturally occurring radionuclides, close comparison with a risk- or dose-based threshold concentrations of interest, or even comparisons across studies. There are several analytical issues that are of concern, but the two that appear to cause incorrect decisions to be made most often involve establishing detection limits and subtracting ambient background conditions in the laboratory. These issues are not critical when radionuclide activity concentrations are large relative to thresholds of concern, but they seem to be poorly understood when it matters. When the comparisons are important and are likely to be close to a threshold of interest, then the general contract with the analytical laboratories needs to be changed so that the right or appropriate data are obtained. The concern is that important decisions are made incorrectly more often as greater scrutiny is placed on DoE's radionuclide cleanup or monitoring decisions by the public and other stakeholders. Examples are presented of problems that have been observed for different projects, both within and outside the realm of DOE and NRC remediation and radioactive waste disposal problems, and solutions are offered that should lead to better data from which important decisions need to be made. The first example is from Los Alamos National Laboratory (LANL) and involves radionuclide concentrations in soil and rock beneath LANL's Material Disposal Area (MDA) G. An initial review of the data led to a conclusion that americium and plutonium are a long way present beneath MDA G. A more thorough review of the data that accounted properly for ambient background and the detection limits that had been established led to the opposite conclusion. Another example is from the Nevada National Security Site where tritium results from one of the wells were unexpectedly high. Proper understanding and analysis of ambient background led to the conclusion that the increased concentrations were not so obvious, and that a different contract with the analytical laboratory was needed to provide more appropriate data to support a better determination. Other examples are used from regulatory review of projects in Nevada, where background levels and secular equilibrium for naturally occurring radionuclides are not established correctly because of analytical issues. The same basic issues have also been found to create difficulties analyzing historical data from the West Valley Demonstration Project. There is evidence in the data that the apparent lack of secular equilibrium where it is expected to exist is related to ambient background subtraction or other analytical issues. A final example is presented for analysis of Tc-99 in samples of depleted uranium. In this case, two different studies that were performed only three months apart provide quite different results. The US Environmental Protection Agency (EPA) established the data quality objectives (DQO) process in the mid-1980's to establish decision performance criteria for data collection. EPA guidance (EPA G-4, for example) clearly distinguishes between DQOs and measurement performance objectives (MQOs) that should be addressed for laboratory analysis of samples. The language of DQOs and MQOs has become confused over time it seems, and the subsequent effects seem to include a lack of attention to decision performance and a routine approach to measurement quality. In order to better address radionuclide sample analysis when the concentrations are close to thresholds of concern, which might be zero for some radionuclides, background for others, and risk-based thresholds for yet others, it is important that routine laboratory analysis methods are adjusted, and that the project team and the laboratory work closely together to ensure that the data meets the MQO requirements of laboratory analysis and reporting of results, and that the MQOs effectively support project-specific DQOs. This basic approach will be applied in Los Alamos in the coming year to the collection of moisture data from underneath MDA T that will be analyzed for americium and neptunium isotopes. Proper understanding of the radiochemistry methods and reporting, and of appropriate statistical methods is critical to the success of such projects, ensuring that the right decisions are made. (authors)

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Recent 238 Pu Production Activities at Idaho National Laboratory

The Plutonium-238 ( 238 Pu) Production program at Idaho National Laboratory (INL) is actively qualifying irradiation targets containing 237 Np for the Advanced Test Reactor (ATR) to produce 238 Pu for future National Aeronautics and Space Administration missions. INL qualified and loaded seven targets in the ATR’s south flux trap for cycle 169A, which occurred in Spring 2021. The irradiation qualification program has expanded to additional ATR irradiation positions after two baseline production targets in three positions validated significant production of 238 Pu. The validation model was followed by the PFS-1 experimental test in the ATR Critical Facility that verified 238 Pu production cross sections. This paper outlines the progress and status of the 238 Pu production program at INL. The qualification effort, safety analysis, hardware status, and future activities for qualification of an updated target design for use in the ATR are discussed.

07 ISOTOPE AND RADIATION SOURCES↗

Biogenic uranium isotope fractionation [Slides]

Presentation Outline: Background and relevance; Project objectives; Tasks and timeline; Current Activities (Task 1: Controlled culture growth, Task 2: Enzymatic reduction of uranium oxides, Task 3: Cellular location of uranium reduction and precipitation); Future work; Achievements

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

Following several successful prompt $\overline{ν}$ evaluations using $\tt{CGMF}$, including consistent evaluations for minor Pu isotopes, we detail in this report our efforts to perform a consistent $\overline{ν}$ evaluation for minor U isotopes during FY25. Although we have not yet produced a finalized evaluation, we present the progress that we have made towards such an evaluation for 232,233,234,236,237,239 U prompt $\overline{ν}$. Our milestone explicitly calls out evaluations for 233 U, 234 U, and 236 U, however, to better constrain the model with reliable experimental $\overline{ν}$ data, we also include 235 U and 238 U in the evaluation procedure. Then, we additionally produce evaluations for 232 U, 237 U and 239 U $\overline{ν}$ as a byproduct. Elsewhere, we will report our efforts on a stand-alone 233 U $\overline{ν}$ evaluation. This report is organized in the following manner. In Sec. 2, we briefly outline the updates to CGMF that were needed to be able to calculate all of these minor U fission reactions. The experimental data overview is given in Sec. 3. The evaluation methodology and results are presented in Secs. 4 and 5, respectively. Finally, we conclude and outline work for FY26 in Sec. 6.

07 ISOTOPE AND RADIATION SOURCES↗

A highly-enriched 244 Pu reference material for nuclear safeguards and nuclear forensics measurements

A highly-enriched 244 Pu isotope dilution reference material has been prepared and characterized for metrologically traceable measurements of very small quantities of plutonium. The amount of plutonium in samples associated with nuclear safeguards and nuclear forensic measurements can be significantly less than 1 ng. Accordingly, the ability to quantify the amount and isotopic composition of plutonium from a single mass-spectrometric analysis is particularly desirable. The highly-enriched 244 Pu reference material, described here, will minimize the magnitude of spike corrections necessary to obtain accurate information on plutonium isotopic composition from isotope dilution measurements.

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Examination of Ac-225 production from Ra-226 using fast reactor JOYO

In this study, the authors investigated the method of producing the radionuclide Ac{sup 225} used for targeted alpha therapy (TAT). Currently, Ac{sup 225} is mainly generated from ORNL's Th{sup 229} generator, and the annual production amount is limited to about 63 GBq, and methods for generating it using accelerators are under development in each country. The method using an accelerator has the advantage of being able to generate Ac{sup 225} from a small amount of target nuclides with high efficiency but has the disadvantage of not being able to irradiate a large amount of target nuclides at once due to the small irradiation area. Therefore, the authors investigated a method to generate Ac{sup 225} by neutron irradiation of Ra{sup 226} as a target nuclide using the experimental fast reactor JOYO, which has abundant neutrons and a large loading region. Irradiation of Ra{sup 226} with fast neutrons causes a (n, 2n) reaction to generate Ra{sup 225}, and then decay to produce Ac{sup 225}. In addition, although harmful Ac{sup 227} is also produced at the same time by the (n,γ) reaction, first of all the actinium isotope is chemically separated and eliminated. Since the remaining Ra{sup 225} collapses and Ac{sup 225} is produced, pure Ac{sup 225} can be extracted by performing chemical separation again. As a result of the analysis, 1 g of Ra{sup 226} is irradiated with JOYO for 60 days, and milking is performed 4 times every 17.5 days. By doing these three times a year, it was found that about 50 GBq of Ac{sup 225} was generated. (authors)

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NanoSIP: NanoSIMS Applications for Microbial Biology

High-resolution imaging with secondary ion mass spectrometry (nanoSIMS) has become a standard method in systems biology and environmental biogeochemistry and is broadly used to decipher ecophysiological traits of environmental microorganisms, metabolic processes in plant and animal tissues, and cross-kingdom symbioses. When combined with stable isotope-labeling—an approach we refer to as nanoSIP—nanoSIMS imaging offers a distinctive means to quantify net assimilation rates and stoichiometry of individual cell-sized particles in both low- and high-complexity environments. While the majority of nanoSIP studies in environmental and microbial biology have focused on nitrogen and carbon metabolism (using 15 N and 13 C tracers), multiple advances have pushed the capabilities of this approach in the past decade. The development of a high-brightness oxygen ion source has enabled high-resolution metal analyses that are easier to perform, allowing quantification of metal distribution in cells and environmental particles. New preparation methods, tools for automated data extraction from large data sets, and analytical approaches that push the limits of sensitivity and spatial resolution have allowed for more robust characterization of populations ranging from marine archaea to fungi and viruses. Further, NanoSIMS studies continue to be enhanced by correlation with orthogonal imaging and ‘omics approaches; when linked to molecular visualization methods, such as in situ hybridization and antibody labeling, these techniques enable in situ function to be linked to microbial identity and gene expression. Here we present an updated description of the primary materials, methods, and calculations used for nanoSIP, with an emphasis on recent advances in nanoSIMS applications, key methodological steps, and potential pitfalls.

07 ISOTOPE AND RADIATION SOURCES↗

Harvesting 88 Zr from heavy-ion beam irradiated tungsten at the National Superconducting Cyclotron Laboratory

Tungsten is a commonly used material at many heavy-ion beam facilities, and it often becomes activated due to interactions with a beam. Many of the activation products are useful in basic and applied sciences if they can be recovered efficiently. In order to develop the radiochemistry for harvesting group (IV) elements from irradiated tungsten, a heavy-ion beam containing 88 Zr was embedded into a stack of tungsten foils at the National Superconducting Cyclotron Laboratory and a separation methodology was devised to recover the 88 Zr. The foils were dissolved in 30% hydrogen peroxide, and the 88 Zr was chemically purified from the tungsten matrix and from other co-implanted radionuclides (such as 85 Sr and 88 Y) using strong cation-exchange (AG MP-50) chromatographic resin in sulfuric acid media. The procedure provided 88 Zr in approximately 60 mL 0.5 M sulfuric acid with no detectable radio-impurities. The overall recovery yield for 88 Zr was (92.3 ± 1.2)%. In conclusion, this proof-of-concept experiment has facilitated the development of methodologies to harvest from tungsten and tungsten-alloy parts that are regularly irradiated at heavy-ion beam facilities.

07 ISOTOPE AND RADIATION SOURCES↗

Risk Informed, Performance-Based, Technology-Inclusive Regulatory Infrastructure: Technology-Inclusive Determination of Mechanistic Source Terms for Offsite Dose-Related Assessments for Advanced Nuclear Reactor Facilities

This report summarizes a risk informed, performance-based and technology-inclusive approach to determine source terms for dose related assessments at advanced nuclear facilities. This approach uses a graded process which allows both the non-mechanistic source terms calculation methods, which adopt conservative approaches and assumptions based on known physical and chemical principles, and more importantly the mechanistic source term calculation methods, which consider design-specific scenarios and use best estimate models with uncertainty quantification for a range of licensing basis events (LBEs), to be used for the design and licensing of advanced nuclear technologies. The source terms developed with this graded approach, and radionuclide inventories elsewhere in the facility that are determined during source term analysis, can be used to address licensing issues to support the application processes of 10 CFR Part 50 for a construction permit and operating license or 10 CFR Part 52 for a Combined Operating License (COL), Standard Design Certification, Early Site Permit, Standard Design Approval or Manufacturing License. They can also be used for other purposes including equipment environmental qualification, control room habitability analyses, and assessments of severe accident risks in environmental impact statements. There are many advanced reactor concepts being developed including high temperature gas-cooled reactor (HGTR), sodium-cooled fast reactor (SFR), lead-cooled fast reactor (LFR), molten salt reactor (MSR), micro-reactor, etc. The graded approach presented in this report for source terms determination is, to the extent possible, generic to any of these reactor designs and to future reactor designs. This report provides information on the review of the regulatory foundation for use of conservative bounding source terms as well as event-specific mechanistic source terms for advanced nuclear reactor designs.

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