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At least 145 records · Page 8

Pu-238 Production Progress at INL From December 2022 to December 2023

Idaho National Laboratory (INL) has an ongoing effort to produce Pu-238 for NASA deep space missions. Recent work at INL has consisted of irradiation of Pu 238 production targets in the Advanced Test Reactor (ATR), generating more than an estimated 400 grams of Pu-238 heat source material between March and October 2023. Additionally, INL began qualifying Pu-238 production targets with a higher loading of Np-237 to further increase the production of Pu-238 production in later years. INL has also updated the analysis as a result of operational changes at ATR. One instance was updating the analysis to enable a single Pu-238 production target to be run in ATR’s South Flux Trap (SFT), rather than the previous seven production targets, to make use of a spare target from a discontinued design. Higher lobe powers in ATR were also analyzed due to potential changes in planned lobe powers.

07 ISOTOPE AND RADIATION SOURCES↗

Harvesting Isotopically Pure Ac-225 from Ra-225 Produced in Thorium Target Spallation Reaction

A method for isolating Ra-225 from linear accelerator irradiated Th metal chemical processing waste streams has been established. Separating Ra-225 from the complex matrix following proton irradiation of Th metal provides a source of isotopically pure Ac-225 free of the Ac-227 impurity that is present in accelerator-produced Ac-225. Ra isotopes are first separated from the irradiated Th target via cation exchange methods. Importantly, the Ra-containing fraction is cleaned from residual citrate via dilute nitric acid washes (0.5 M) on AG50W-X8 resin. The mixed Ra isotopes are then further purified from Ba-140 impurity using a Sr resin column. Ra elutes through the resin with successive washes of 2.5 M HNO 3 while Ba-140 is retained. Ac-225 is then harvested by loading the Ra content onto an AG50W-X8 cation exchange column where the Ra-225 parent is eluted with 2.5 M HNO 3 before the Ac-225 daughter is eluted with 8 M HNO 3 .

07 ISOTOPE AND RADIATION SOURCES↗

Measuring Neptunium Concentration using Optical Spectrometry for the Pu-238 Supply Program

Targets containing 237 Np are irradiated at the High Flux Isotope Reactor at Oak Ridge National Laboratory to produce 238 Pu, as plutonium dioxide (PuO 2 ), a heat source material for use in future NASA space missions. Kilogram quantities of Np are processed yearly and developing methods to efficiently characterize and monitor the Np processing streams with optical spectroscopy and real-time monitoring software is a critical aspect of this effort. Here, we evaluate how ultraviolet/visible/near-infrared (UV-Vis-NIR) absorbance and Raman spectroscopic techniques are applicable to characterizing concentrated Np solutions and provide proof-of-principle and proof-of-concept results for each technique. Both techniques were tested in lab-scale studies and should improve the timeliness of production efforts. However, spectrophotometry is the more mature option and has been successfully demonstrated in a hot cell environment. An overview of the initial findings, a brief demonstration, and areas for future work will be highlighted in this report.

07 ISOTOPE AND RADIATION SOURCES↗

Northstar Mo100 Target Beam Spot Size Sensitivity Study

Northstar Mo100 target for production of the medical isotope Mo99 is particularly sensitive to beam over focusing because of the intended high power density. At 38 MeV and 6.32 mA (240 kW beam power, nominally 160 kW th in the target), small deviation from the nominal 12 mm FWHM beam can significantly increase the target disk temperatures and more importantly the load bearing target window temperature. A rhodotron will be the source of the electron beam to be used in the isotope production. This machine operates in a pulsed beam mode, currently expected to be at 50 Hz, which results in a 100 C temperature oscillation above and below the steady state temperature that is the focus of this study. This must be considered in the determination of minimum beam spot size that can be accepted by the target without risk of failure. In addition to the nominal beam spot size of 12 mm, the analysis of 10, 11 and 14.5 mm beam spot sizes are analyzed. The primary conclusion is that an over focused beam to just 11 mm FWHM is the minimum beam spot allowable, based on window temperature and the Ultimate Tensile Stress (UTS) of the window material Inconel 718 as a function of temperature. In contrast an under focused beam of 14.5 mm FWHM has much reduced target and window temperatures, but there is a resulting 6% drop in isotope production, all other factor staying the same. These results are presented herein.

07 ISOTOPE AND RADIATION SOURCES↗

Integration of High-Z Converter into Full-scale Production Target for Accelerator-based Production of 99 Mo

NorthStar Medical Technologies is planning to produce the 99Mo isotope via the photonuclear route. The Rhodotron accelerator designed by IBA will be used as an electron-beam source. The Rhodotron is an efficient recirculating accelerator, providing low energy dispersion and a low-emittance electron beam. The nominal beam power is assumed to be 120 kW at 40 MeV. In photonuclear production of 99 Mo, a high-power electron beam impinges on a helium-cooled Mo disk target. Electrons are converted into photons through the Bremsstrahlung process. Consequently, high-energy photons interact with the target nuclei, producing 99 Mo through the 100 Mo(γ, n) 99 Mo reaction. Traditionally, photonuclear production is realized using high-Z material as the electron-to-photon converter. NorthStar plans not to use a high-Z converter in the initial production target design, but it may be interested in the increased production capabilities a high-Z converter can provide. The purpose of this report is to evaluate the advantages and disadvantages of incorporating a high-Z converter into the target design.

07 ISOTOPE AND RADIATION SOURCES↗

Pu-238 Production Progress at Idaho National Laboratory From December 2023 to November 2024

Idaho National Laboratory (INL) has continued in the effort to produce Pu-238 to support NASA deep space missions. In support of the production goal of contributing 700 g to the 1.5 kg per year constant rate production of Pu-238 heat source material in the United States by 2026. All available inner core positions of the Advanced Test Reactor (ATR) have been qualified for production for a 20% Np target, with efforts nearing completion for a 30% Np target further increasing production amounts. This includes the North East Flux Trap (NEFT), South Flux Trap (SFT), Inner A, H positions. With the completion of qualifying the inner core of ATR, work has started on the qualifying the outer core. The portion of the outer core that will produce Pu-238 includes the Large and Medium I positions. With the continued qualification work, INL is on track to contribute to the production goal by 2026.

07 - ISOTOPES AND RADIATION SOURCES↗

Abatement Case Study

Radioxenon emissions from industrial sources such as fission based medical isotope production (MIP) facilities and nuclear reactors are generally known to be well below levels of public health and safety concern. However, the global background of radioxenon produced by MIP interferes with nuclear explosion monitoring by the International Monitoring System (IMS) developed for the Comprehensive Nuclear-Test-Ban Treaty (CTBT) (CTBTO, 2024). It was calculated that xenon emissions levels of 5×10 9 Bq/day 133 Xe were low enough to have minimal impact on International Monitoring System (IMS) stations (Bowyer et al, 2013). There are several technologies currently used to abate radioactive xenon emissions to meet regulatory release levels, and some alternative methods have been investigated to reduce xenon release levels well below required regulatory levels (Doll et al, 2014, Gueibe, et al, 2014). While MIP producers are sympathetic to the issue of radioxenon interference with IMS monitoring, the cost to implement and maintain additional abatement systems has resulted in limited implementation. Therefore, more cost-effective options for xenon abatement are needed to help reduce the impact of these emissions on nuclear explosion monitoring.

07 ISOTOPE AND RADIATION SOURCES↗

Measurement of Plutonium Ratios for CRM 137A Recertification

This report documents the analytical methodologies used by the Chemical and Isotopics Mass Spectrometry (CIMS) Group at the US Department of Energy’s Oak Ridge National Laboratory (ORNL) for plutonium isotopic ratio characterizations on purified ~1 mg units prepared by Lawrence Livermore National Laboratory (LLNL) from a mother solution created from an existing 250 mg unit of certified reference material (CRM) 137. The analytical processes described are designed to maintain traceability of the final certified attributes and to eliminate sources of systematic bias for the measurements described. The measurands for certification are the plutonium isotope ratios: 238 Pu/ 239 Pu, 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu. The preparation and analytical process included the following activities: Preparation of reference materials to be used as calibrants to establish traceability to the SI unit of mass for the isotopic analyses and quality controls. For the plutonium isotopic analyses, CRM 128 (a CRM comprising equal atoms of 239 Pu and 242 Pu) was used as the primary calibrant; Each CRM 137A unit was reconstituted using dilute high-purity HNO3. From each, seven replicates were distributed for the isotopic characterizations by thermal ionization mass spectrometry (TIMS) using the total evaporation (TE) method for isotope ratio measurements and MC-ICP-MS using a dynamic peak hooping method for secondary isotope ratio measurements; Due to time delay in the analyses from the last purification of the original CRM 137 mother solution by LLNL, an aliquot of the three provided plutonium units was purified using Eichrom TEVA separation methods to remove americium in-growth and uranium impurities; Minimally corrected data were reported from each analysis using reporting templates provided by the New Brunswick Laboratory Program Office (NBL PO) for the specific methods used for isotopic measurements. In addition, a copy of the instrument exports, Excel templates for isotopic data corrections, and the uncertainty budgets completed with the GUM Workbench software package were submitted to NBL PO.

07 ISOTOPE AND RADIATION SOURCES↗

Improvements to the 115g/115m Cd Nuclear Data

Repeated measurements of the isotope 115m Cd by Los Alamos National Laboratory (LANL), Pacific Northwest National Laboratory (PNNL), and Atomic Weapons Establishment (AWE) have revealed a consistent discrepancy between beta and gamma counting. This suggests that a significant disparity exists between the true value of the isotope’s gamma-ray branching ratios and the values reported by the National Nuclear Data Center (NNDC). Enriched 114 Cd was irradiated using thermal neutrons to produce a high-purity 115m/g Cd source for counting and analysis using traditional singles gamma-ray spectroscopy, liquid scintillation counting, gas-proportional counting, and analysis using the new Gamma-Alpha-Beta-Gamma (GABγ) and Gamma-Alpha-Beta Radio-Isotope EvaLuator (GABRIEL) coincidence detection systems. Using the D-T fusion generated neutrons, reduces the wait time required to let the short-lived 115Cd ground state decay away by leveraging the 1:1 production ratio of the ground and metastable state of 115 Cd from the 115 In (n,p) reaction relative to the 10:1 production ratio of the ground and metastable isotopes of 115 Cd by thermal neutron capture on 114 Cd. However, the much higher flux in from the Washington State University TRIGA reactor is a more rapid method of production of 115m/gCd but requires access to enriched 114 Cd. High purity 115m/g Cd samples were analyzed on regular intervals over a period of 140-days. The activity of 115m Cd measured by beta and gamma show a clear discrepancy using the current best known gamma-ray decay branching ratios. Based on these observations and measurements, a set of new branching ratio recommendations have been produced using conventional counting techniques and the advanced GAB? and GABRIEL instruments.

07 ISOTOPE AND RADIATION SOURCES↗

Cross Section Measurements of Photonuclear Reaction Pathways Towards Promising Medical Radioisotopes

Project Objectives: The goal of this project was to generate data relevant to radioisotope production while developing innovative technologies that foster and enhance novel production of radioisotopes, and, also, while providing opportunities for cultivating and training future generations of scientists. This work has provided the foundation for methodologies for determination of photonuclear cross sections over multiple energies in a single irradiation. Simultaneously, the feasibility of electron LINAC production of several in-demand radioisotopes such as 47 Sc, 67 Cu, 77 As, and 186 Re has been demonstrated. To accomplish these objectives a collaboration was formed between two complimentary facilities, the Low Energy Accelerator Facility (LEAF) at Argonne National Laboratory and the High Intensity Gamma-ray Source (HIGS) at Triangular Universities Nuclear Laboratory (TUNL). The involvement of the research group from North Carolina Central University gave students at this Historically Black University experience in forefront nuclear-physics research relevant to addressing a high-priority interdisciplinary issue. Project Description: HIGS provides a nearly monoenergetic gamma-ray beam by intra-cavity Compton backscattering of free-electron photons from electrons circulating in a storage ring. This beam can be collimated to produce a very precise energy beam. If the beam is un-collimated a calculated and precise energy spread of the beam occurs radially. The γ-flux can be evenly distributed over the radial distribution of energy and used to perform activation experiments on concentric ring targets. Thus providing multiple energy ranges in a single irradiation. Each concentric ring target can be counted separately in order to determine activation at the given energy and successively be correlated to the activation cross section. Targets were activated to determine production feasibility using electron beams at LEAF. Potential Impact: The Nuclear Science Advisory Committee recently named production of radioisotopes with electron LINACs as one of the most compelling and largest-impact opportunities for the production of high specific activity radioisotopes. Improving the photonuclear cross sectional data base with experimentally verified results will greatly enhance a researcher’s ability to rationalize electron LINAC production routes towards desired radioisotopes. This work will provide the foundation for methodologies for determination of photonuclear cross sections over multiple energies and multiple targets in a single irradiation. The techniques developed in this project will enable future studies to continue verifying theoretically predicted photonuclear cross section with experimental results. These data will also enable adaptation of models and support more precise theoretical calculation of photonuclear cross sections. This research will involve undergraduates, graduate students, and post-docs to give them a valuable research experience leading towards the next generation of scientists in the field of medical isotopes.

07 ISOTOPE AND RADIATION SOURCES↗

Exploring rapid chemical separations of Sc-47 produced from photonuclear reactions on natural vanadium targets

Scandium-47 ( 47 Sc) production via bremsstrahlung irradiation of natural vanadium targets offers significant advantages for producing high purity 47 Sc; this work evaluates several rapid dissolution and chemical separation techniques for recovering high purity 47 Sc from irradiated vanadium. Here, techniques developed are combined into a simple, gram-scale, semi-automated target processing system that enables 47 Sc recovery from irradiated vanadium targets with chemical yields as high as 93 ± 3% and 47 Sc/V separation factors of 6 ± 3 ·10 11 within 90 min total processing times. Future research into H 2 O 2 resistant separation techniques and their applicability for direct process coupling to chelation are recommended.

07 ISOTOPE AND RADIATION SOURCES↗

Oxygen stable isotopes in the nuclear fuel cycle: Assessment of the potential for determining the fabrication and provenance history of anhydrous and hydrous uranium oxides

Determining the origin and history of interdicted nuclear materials is a central challenge in nuclear forensics. The oxygen stable isotope composition of uranium oxide compounds has emerged as a promising forensic signature, attracting increasing attention since the early 2000s. This review examines analytical techniques for measuring oxygen isotope compositions in uranium oxides and evaluates how the nuclear fuel production cycle introduces or modifies these isotopic signatures. The potential for forensic geolocation is explored through workflows that calibrate the relationship between environmental water oxygen isotopes and those found in uranium oxides. Key strengths and limitations of this approach are assessed, including gaps in knowledge related to isotope fractionation during specific stages of the fuel cycle, and processing facility water inputs. The importance of proper sample handling and storage under inert atmospheres, as well as a deeper understanding of both intra-sample oxygen isotope heterogeneity, and hydrous uranium oxide phase formation, is highlighted for improving the reliability of forensic interpretations. In conclusion, the development of uranium oxide standards with well-characterized δ 18 O values and international collaboration toward consensus on their use are identified as essential steps for advancing the field.

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Large-scale production of 88 Y and 88 Zr/ 88 Y generators: A proof of concept study for a 70 MeV H – cyclotron

Here, the large-scale production of 88 Y with proton-induced reactions has been investigated from the perspective of new generation 70 MeV H – cyclotrons. Tandem target configurations are presented for both the direct production of 88 Y as well as for producing 88 Zr/ 88 Y generators. Based on the relevant excitation functions, physical yields have been derived for 88 Y production with Y 2 O 3 /SrCO 3 tandem targets and 88 Zr production with Zr/Y 2 O 3 tandem targets. Yields are presented for optimized targets (i.e. optimum yield) as well as for balanced thermal loads on the individual targets. Liquid 88 Zr/ 88 Y generators have been produced using both natural Zr and Nb target materials, the former for dedicated productions and the latter as a byproduct by processing spent irradiated Nb capsules which normally would constitute radioactive waste. These stock solutions, which contain both the target material and 88 Zr precursor, are retained virtually unchanged after processing except for the removal of 88 Y on AG MP-50 macroporous cation-exchange resin. Methods are presented for the preparation of Nb stock solutions in hydrofluoric acid and Zr stock solutions in sulfuric acid. It is shown that multi-Ci productions of 88 Y are feasible at a 70 MeV cyclotron facility, suitable for the needs of fracking applications. In addition, 88 Zr/ 88 Y generators can provide 88 Y with very high specific activity, suitable for labelling of biomolecules.

07 ISOTOPE AND RADIATION SOURCES↗

Measurement of 227 Ac impurity in 225 Ac using decay energy spectroscopy

225 Ac is a valuable medical radionuclide for targeted $\alpha$ therapy, but 227 Ac is an undesirable byproduct of an accelerator-based synthesis method under investigation. Sufficient detector sensitivity is critical for quantifying the trace impurity of 227 Ac, with the 227 Ac/ 225 Ac activity ratio predicted to be approximately 0.15% by end-of-bombardment (EOB). Superconducting transition edge sensor (TES) microcalorimeters offer high resolution energy spectroscopy using the normal-to-superconducting phase transition to measure small changes in temperature. By embedding 225 Ac production samples in a gold foil thermally coupled to a TES microcalorimeter we can measure the decay energies of the radionuclides embedded with high resolution and 100% detection efficiency. This technique, known as decay energy spectroscopy (DES), collapses several peaks from $\alpha$ decays into single Q-value peaks. In practice there are more complex factors in the interpretation of data using DES, which we will discuss in this paper. Using this technique we measured the EOB 227 Ac impurity to be (0.142 ± 0.005)% for a single production sample. This demonstration has shown that DES is a useful tool for quantitative measurements of complicated spectra.

07 ISOTOPE AND RADIATION SOURCES↗

Evaluation of hydroxamate-based resins towards a more clinically viable 44 Ti/ 44 Sc radionuclide generator

For this research, several hydroxamate-based resins were synthesized and tested for use in 44 Ti/ 44 Sc generator systems in small scale experiments (740 kBq 44 Ti). The most promising resin was tested further in larger scale generator studies (37 MBq). This resin displayed impressive retention of 44 Ti over several elutions, and high quantities of 44 Sc were obtained in small volumes of dilute HCl eluents. Initial radiolabeling experiments were conducted and demonstrated the possibility of direct radiolabeling of the generator produced 44 Sc with DOTA.

07 ISOTOPE AND RADIATION SOURCES↗

Development of ultralow-background cryogenic calorimeters for the measurement of surface α contamination

Next-generation experiments searching for rare events must satisfy increasingly stringent requirements on the bulk and surface radioactive contamination of their active and structural materials. The measurement of surface contamination is particularly challenging, as no existing technology is capable of separately measuring parts of the 232 Th and 238 U decay chains that are commonly found to be out of secular equilibrium. We will present the results obtained with a detector prototype consisting of 8 silicon wafers of 150mm diameter instrumented as bolometers and operated in a low-background dilution refrigerator at the Gran Sasso Underground Laboratory of INFN, Italy. Furthermore, the prototype was characterized by a baseline energy resolution of few keV and a background <100nBq/cm 2 in the full range of α energies, obtained with simple procedures for cleaning of all employed materials and no specific measures to prevent recontamination. Such performance, together with the modularity of the detector design, demonstrate the possibility to realize an alpha detector capable of separately measuring all alpha emitters of the 232 Th and 238 U chains, possibly reaching a sensitivity of few nBq/cm 2 .

07 ISOTOPE AND RADIATION SOURCES↗

Photonuclear production of 47 Ca for 47 Ca/ 47 Sc generator from natural CaCO 3 targets

Here this work investigated the indirect production of 47 Sc from natural Ca targets via 48 Ca(γ,n) 47 Ca → 47 Sc +β - +$\bar{\nu}_e$ with incident electron energies of 30, 35, and 40 MeV. The 47 Ca production yields were simulated using the PHITS Monte Carlo simulation code and compared to experimental data. The simulated production rates for all three irradiations are in good agreement with experimental data within uncertainties. As a demonstration of the 47 Ca/ 47 Sc generator system, one of the irradiated CaCO 3 targets was dissolved in nitric acid, and 47 Sc was isolated from the target material using commercially available Eichrom DGA resin. The 47 Sc was allowed to grow in, and the purification process was repeated with promising 47 Sc and Ca recovery yields.

07 ISOTOPE AND RADIATION SOURCES↗

Measurement of the 70 Ge( d , n ) 71 As cross section from 2.1 MeV to 10 MeV

This work reports experimental 70 Ge(d,n) 71 As cross sections producing Arsenic-71 (t 1/2 = 65.3 h, 28% β + ), a potentially useful diagnostic radionuclide. Target stacks containing two nat Ge foils, a nat Ni monitor foil, and an Al degrader were irradiated with 5.5–10 MeV deuterons using an FN Tandem Van de Graaff accelerator. 71 As and 61 Cu, 56 Co, and 58 Co (from nat Ni(d,x)) were quantified in the foils by high purity germanium gamma spectrometry. Furthermore, the measured cross sections are larger than previously reported and suitable for producing preclinical quantities of diagnostic radiopharmaceuticals.

07 ISOTOPE AND RADIATION SOURCES↗