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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Enhancing Radionuclide Production Capabilities at the Duke University Medical Center Cyclotron with a Focus on Astatine-211

Radionuclides play an important role in a diverse array of fields including physics, chemistry, agriculture, materials science, national security, medical research and patient care. Establishing a reliable domestic supply of key radionuclides is critical to our national competitiveness in these areas. Regarding medical applications, targeted alpha-particle therapy (TAT) has become of great interest to basic researchers and clinicians alike and is emerging as a valuable and cost-effective approach for cancer treatment. Unfortunately, progress in TAT, particularly with regard to its clinical translation, has been severely hampered by the limited availability of the most promising radionuclides at a reasonable cost, and with appropriate chemical and radiochemical purity. In this project, we have attempted to address this problem by focusing on production of the 7.2-h half-life α-particle emitter, 211 At, which has long been considered to be one of the most promising radionuclides for TAT. We note that he critical importance of improving the supply of 211 At in the United States was noted in the Funding Opportunity Announcement related to this project. At Duke University, we have a CS-30 cyclotron that is one of the few accelerators in the United States that has an alpha-particle beam that has enough energy to make useful quantities of 211 At. With this cyclotron, we have been able to produce more 211 At than anywhere else in the world because of our unique internal cyclotron target system. However, the CS-30 cyclotron is nearly 40 years old and was no longer reliable. In addition, its operation required considerable skill, largely because it had analog control systems, and vital parts including old-fashioned power supplies, were becoming unavailable. For these reasons, the current project was undertaken to evaluate all the subsystems of the CS-30 cyclotron and replace, repair, and update them. With help from our consultant, Ionetix, this has now been accomplished. We believe that because of this work, the CS-30 can reliably supply 211 At for basic research and clinical trials both at Duke and beyond.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2020

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.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

Sustainable production of radionuclidically pure antimony-119

Background Radiopharmaceutical therapy (RPT) uses radionuclides that decay via one of three therapeutically relevant decay modes (alpha, beta, and internal conversion (IC) / Auger electron (AE) emission) to deliver short range, highly damaging radiation inside of diseased cells, maintaining localized dose distribution and sparing healthy cells. Antimony-119 ( 119 Sb, t 1/2 = 38.19 h, EC = 100%) is one such IC/AE emitting radionuclide, previously limited to in silico computational investigation due to barriers in production, chemical separation, and chelation. A theranostic (therapeutic/diagnostic) pair can be formed with 119 Sb’s radioisotopic imaging analogue 117 Sb (t 1/2 = 2.80 h, E γ = 158.6 keV, I γ = 85.9%, β + = 262.4 keV, I β+ = 1.81%). Results Within, we report techniques for sustainable and cost-effective production of pre-clinical quality and quantity, radionuclidically pure 119 Sb and 117 Sb, novel low energy photon measurement techniques for 119 Sb activity determination, and physical yields for various tin target isotopic enrichments and thicknesses using (p, n) and (d, n) nuclear reactions. Additionally, we present a two-column separation providing a radioantimony yield of 73.1% ± 6.9% (N = 3) and tin separation factor of (6.8 ± 5.5) x 10 5 (N = 3). Apparent molar activity measurements for deuteron produced 117 Sb using the chelator TREN-CAM were measured at 42.4 ± 25 MBq 117 Sb/µmol (1.14 ± 0.68 mCi/µmol), and we recovered enriched 119 Sn target material at a recycling efficiency of 80.2% ± 5.5% (N = 6) with losses of 11.6 mg ± 0.8 mg (N = 6) per production. Conclusion We report significant steps in overcoming barriers in 119 Sb production, chemical isolation and purification, enriched target material recycling, and chelation, helping promote accessibility and application of this promising therapeutic radionuclide. We describe a method for 119 Sb activity measurement using its low energy gamma (23.87 keV), negating the need for attenuation correction. Finally, we report the largest yet-measured 119 Sb production yields using proton and deuteron irradiation of natural and enriched targets and radioisotopic purity > 99.8% at end of purification.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Nuclear excitation functions for medical isotope production: Targeted radionuclide therapy via nat IR$(d, x)$ 193m Pt

193m Pt is an Auger emitting radionuclide which may have therapeutic potential, particularly when labeled to the chemotherapeutic drug cisplatin. One challenge to broader explorations of its clinical potential is the need for production routes with high specific activity. As part of a larger campaign to address gaps in reaction data for emerging medical radionuclides, this work seeks to characterize the nat Ir(d,x) reactions as a potential production pathway for 193m Pt. A stacked target irradiation, consisting of natural iridium, iron, nickel, and copper foils, was performed using a 33 MeV deuteron beam at the Lawrence Berkeley National Laboratory 88-Inch Cyclotron. This measurement, along with previous experimental data, suggests an energy window between 11 to 18 MeV to maximize the production and radiopurity of 193m Pt. This experiment has yielded cross sections for 43 channels of deuteron-induced reactions from threshold to 30 MeV, including the first experimental results of nat Ir(d,x) 188m1+g,190m1+g Ir (cumulative), nat Ni(d,x) 56,57,58 m,58g Co (independent), nat Cu(d,x) 61 Co (cumulative) and nat Fe(d,x) 53 Fe, 48 V (cumulative). The results were compared with literature data, the TENDL-2023 database, and default theoretical calculations from the TALYS-2.04, CoH-3.6.0, EMPIRE 3.2.3, and ALICE-2020 reaction modeling codes. Here, this work presents another example of the lack of predictive capabilities for this set of modern nuclear-reaction modeling codes, and highlights the unsatisfactory modeling of experimental cross sections. Experimental data are important to improve the codes in general, and new experimental results can be used to improve the models. Finally, this measurement has revealed the need for an updated evaluation of the nat Cu(d,x) 63 Zn deuteron monitor reaction.

193mPt↗
DOE OSTI2024

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 (Final Technical Report)

The overall objectives of this project were (1) to develop methods for the production and separation of a diagnostic and therapeutic or “theranostic” pair of radioisotopes, terbium-155 ( 155 Tb) and terbium-161 ( 161 Tb) and (2) to train graduate students and postdoctoral fellows in technologies and methods used in radionuclide production. Radionuclides can be incorporated into drugs called radiopharmaceuticals that target a specific disease (e.g., cancer). The need for theranostic radionuclides is escalating with the clinical translation of radiopharmaceuticals due to their implementation in personalized medicine, which has demonstrated enhanced patient treatments. High purity and high specific activity radionuclides are critical for theranostic agent development, for example to maintain diagnostic image quality, to minimize radiation dose to the patient, and to increase uptake in the targeted tissue (e.g., tumor), especially in the case of receptor- and antigen-targeted agents. The 155 Tb (diagnostic) and 161 Tb (therapeutic) radioisotopes that were generated through this project are a theranostic pair with demonstrated potential for the development and translation into individualized, targeted, and dosimetry-driven radiotherapies. However, the development of such radiotherapies has been hindered by the lack of a routine and reliable supply of these isotopes in the United States. Methods for the production, separation, and supply of 155 Tb and 161 Tb were investigated and developed in this project. Further, the strong emphasis throughout the project on the training of graduate students and postdoctoral fellows has helped to ensure and enhance the nuclear science workforce through the training of the next generation of highly qualified scientists in nuclear and radiochemistry. This grant also continued a collaboration between scientists at the University of Washington (UW), the University of Missouri (MU) and Brookhaven National Laboratory (BNL). All three institutions were involved in the project, but to different degrees on the various tasks through which the overall objectives were met.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2025

Computational Modeling to Advance Novel Medical Isotopes for Radiotheranostics: A DOE-NIH Joint Workshop Executive Summary

The DOE-NIH Joint Workshop on Computational Modeling to Advance Novel Medical Isotopes for Radiotheranostics, held on September 27, 2024, brought together experts from government, academia, and industry to address critical challenges in radionuclide production and clinical translation. Here, the workshop emphasized interdisciplinary collaboration, particularly between the Department of Energy (DOE) and the National Institutes of Health (NIH), to strengthen the domestic isotope supply, streamline regulatory pathways, and further integrate computational tools into radiopharmaceutical therapy (RPT). Key discussions explored the role of AI-driven modeling, machine learning, and digital twin technologies in optimizing dosimetry, dynamically personalizing treatments, and reducing time to clinical adoption. Advances in predictive computational modeling were highlighted as essential for improving radionuclide yield, purity, and synthesis efficiency. Regulatory considerations and equitable access were central themes, with participants advocating for harmonized global standards, adaptive trial designs, and expanded infrastructure for clinical implementation. DOE computational and production infrastructure was emphasized. Future priorities identified include increased investment in radionuclide production infrastructure, expanded workforce development in radiopharmaceutical sciences and computational modeling, and the creation of robust public-private partnerships. The workshop concluded that continued strategic collaboration and sustained resources will be vital for advancing next-generation radiotheranostics, ensuring safe and effective therapies accessible to all patients.

digital twins↗
DOE OSTI2023

Support for Students, Postdoctoral Fellows and Trainees to Attend Radiochemistry-Related Symposia at Pacifichem 2020

This project was undertaken to help meet the need for training personnel who will be involved in professional careers requiring knowledge of radiochemistry, such as those working in radionuclide production, and in biological, industrial, medical and environmental fields that use radionuclides in their work. The goal of the project was to provide financial assistance to students and trainees from US academic and government institutions to attend selected radiochemistry related symposia at the Pacifichem 2020 meeting, which was to be held in Honolulu, Hawaii in December 2020. The funding, meant to provide a portion of an awardee’s travel cost, was specifically directed at awardees attendance to the following symposia: #190, Advancements in Isotope production-Providing Important Materials for Research and Applications; #180, Advancements in the Chemistry of Targeted Alpha Therapy, and #178, The Chemistry of 18 F, 11 C and Radiometal-based Probes for Molecular Imaging & Precision Medicine. It was/is believed that attendance of students/postdocs at the meeting would point out the critical role radiochemistry and radionuclides can have in the development of future diagnostic and therapeutic agents which would stimulate student interest in radiochemistry, and thus, provide support for making, or an impetus to make, this technical area a career choice.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Measurement of 139 La(p,x) cross sections from 35–60 MeV by stacked-target activation

A stacked-target of natural lanthanum foils (99.9119% 139 La) was irradiated using a 60 MeV proton beam at the LBNL 88-Inch Cyclotron. 139 La(p,x) cross sections are reported between 35–60 MeV for nine product radionuclides. The primary motivation for this measurement was the need to quantify the production of 134 Ce. As a positron-emitting analogue of the promising medical radionuclide 225 Ac, 134 Ce is desirable for in vivo applications of bio-distribution assays for this emerging radio-pharmaceutical. Finally, the results of this measurement were compared to the nuclear model codes TALYS, EMPIRE and ALICE (using default parameters), which showed significant deviation from the measured values.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

DICER: A new instrument at LANSCE to constrain neutron capture rates on radionuclides

With very few exceptions, direct measurements of neutron capture rates on radionuclides have not been possible. A number of indirect methods have been pursued such as the surrogate method, the γ-ray strength function method, the Oslo method and the β-Oslo method. Substantial effort has been devoted to quantify the usually large systematic errors that accompany the results from these techniques. A new instrument has been developed at the Los Alamos Neutron Science Center (LANSCE) to provide more accurate data on several radionuclides relevant to nuclear criticality safety, radiochemical diagnostics, astrophysics, nuclear forensics and nuclear security, by measuring the transmission of neutrons through radioactive samples and studying resonance properties. The Device for Indirect Capture on Radionuclides (DICER) and associated radionuclide production at the Isotope Production Facility (IPF), both at LANSCE, as well radioactive sample fabrication, have been under development the last few years. A description of the new apparatus, data on a few mid-weight stable isotopes and efforts on radionuclide measurements will be presented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

DICER: A new instrument at LANSCE to constrain neutron capture rates on radionuclides

. With very few exceptions, direct measurements of neutron capture rates on radionuclides have not been possible. A number of indirect methods have been pursued such as the surrogate method, the γ-ray strength function method, the Oslo method and the β-Oslo method. Substantial effort has been devoted to quantify the usually large systematic errors that accompany the results from these techniques. A new instrument has been developed at the Los Alamos Neutron Science Center (LANSCE) to provide more accu rate data on several radionuclides relevant to nuclear criticality safety, radiochemical diagnostics, astrophysics, nuclear forensics and nuclear security, by measuring the transmission of neutrons through radioactive samples and studying resonance properties. The Device for Indirect Capture on Radionuclides (DICER) and as sociated radionuclide production at the Isotope Production Facility (IPF), both at LANSCE, as well radioactive sample fabrication, have been under development the last few years. A description of the new apparatus, data on a few mid-weight stable isotopes and efforts on radionuclide measurements will be presented.

Nuclear Criticality Safety Program (NCSP)↗
DOE OSTI2024

FLUKA simulation validation to measure the beam energy of a cyclotron

FLUKA is a fully integrated particle physics MonteCarlo simulation package which has many applications in high energy experimental physics and engineering. When using a cyclotron for medical radionuclide production, it is important to know that the beam energy is suitable to cause the intended nuclear reaction and minimize unwanted impurities. Here, this work focuses on the comparison of FLUKA as a tool to measure the beam energy of a cyclotron with experimental results using the method of stacked copper foils interspaced by an aluminum degrader. We compared two methods to determine the activity ratio: determining the activity in each foil using the experimentally measured cross-sections from the National Nuclear Data Center (NNDC) cross-section data and calculating the activity in the two Cu foils using the FLUKA program. These results were compared to those reported by Gagnon et al., 2011. The FLUKA results gave energy measurements that were different than the true energy by a percentage in the range of 2.4% to 13%, suggesting that FLUKA is not recommended for pre-calculating the cyclotron beam energy using these low Z materials without experimental confirmation. It also confirms that the experimental cross-section data from the NNDC database is superior for this application giving energy values that ranged from 0.1% to 1.6% from the true energy.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

From Fluid Flow to Coupled Processes in Fractured Rock: Recent Advances and New Frontiers

Abstract Quantitative predictions of natural and induced phenomena in fractured rock is one of the great challenges in the Earth and Energy Sciences with far‐reaching economic and environmental impacts. Fractures occupy a very small volume of a subsurface formation but often dominate fluid flow, solute transport and mechanical deformation behavior. They play a central role in CO 2 sequestration, nuclear waste disposal, hydrogen storage, geothermal energy production, nuclear nonproliferation, and hydrocarbon extraction. These applications require predictions of fracture‐dependent quantities of interest such as CO 2 leakage rate, hydrocarbon production, radionuclide plume migration, and seismicity; to be useful, these predictions must account for uncertainty inherent in subsurface systems. Here, we review recent advances in fractured rock research covering field‐ and laboratory‐scale experimentation, numerical simulations, and uncertainty quantification. We discuss how these have greatly improved the fundamental understanding of fractures and one's ability to predict flow and transport in fractured systems. Dedicated field sites provide quantitative measurements of fracture flow that can be used to identify dominant coupled processes and to validate models. Laboratory‐scale experiments fill critical knowledge gaps by providing direct observations and measurements of fracture geometry and flow under controlled conditions that cannot be obtained in the field. Physics‐based simulation of flow and transport provide a bridge in understanding between controlled simple laboratory experiments and the massively complex field‐scale fracture systems. Finally, we review the use of machine learning‐based emulators to rapidly investigate different fracture property scenarios and accelerate physics‐based models by orders of magnitude to enable uncertainty quantification and near real‐time analysis.

58 GEOSCIENCES↗
DOE OSTI2023

Late Holocene Cliff Retreat in Del Mar, CA, Revealed From Shore Platform 10 Be Concentrations and Numerical Modeling

Rocky coast cliff retreat presents a hazard to coastal communities and infrastructure that is potentially amplified under rising sea level conditions, among other factors. Unfortunately, constraints on retreat rates are typically limited to those derived from imagery and maps spanning the last ~100 years. Here, we use a newly developed coupled model of shore platform profile evolution and cosmogenic radionuclide production that considers the influence of relative sea level (RSL) rise, weathering, material resistance, and wave height decay to model cliff retreat over millennial timescales and its potential drivers in Del Mar, California. We demonstrate the ability to use topographic and bathymetric measurements from a narrow shore platform along with a limited data set of nine cosmogenic 10Be concentrations extending ~125 m from the cliff base to obtain modeled cliff retreat rates that steadily range from 5.0 to 12.5 cm yr -1 over the last two millennia until 100 years before present. These rates are consistent with modern retreat rates of about 2–19 cm yr -1 here. RSL rise in Southern California remained relatively constant during the late Holocene, potentially explaining the relatively stable modeled cliff retreat rate over this time. We also explore the relative influence of weathering, material resistance, and wave erosion efficacy and find that both weathering and wave-driven erosion are necessary to replicate the measured data at this location, with the latter exerting a stronger control on model acceptance, suggesting that waves may provide a possible mechanism by which RSL rise may influence coastal cliff erosion in southern California.

58 GEOSCIENCES↗
DOE OSTI2022

New capability for indirect neutron capture measurements: The DICER instrument at LANSCE

The Device for Indirect Capture on Radionuclides (DICER) implements a new indirect technique for (n,γ) studies in which the neutron capture rate is determined from analysis of resonance neutron transmission data. The DICER instrument and associated radionuclide production at the Isotope Production Facility (IPF), both at the Los Alamos Neutron Science Center (LANSCE), as well radioactive sample fabrication, have been under development in the last few years. First measurements on a radioactive sample ( 88 Zr, t ½ =83.4 days), which was recently reported to have an extremely large thermal neutron capture cross section and resonance integral, are planned for the winter of 2021. A performance overview, brief details on the 88Zr fabrication and proof of good operation results will be presented.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Assessment of Molybdate Based Corrosion Inhibitor for use at the Savannah River Tank Farm Cooling Water System

The Savannah River Site (SRS) has relied on 51 underground storage tanks, many dating back to the 1950s, to store radioactive liquid waste generated from nuclear processing and radionuclide production. These tanks use carbon steel cooling coils, cooled by soft, acidic water, to dissipate the decayed heat produced by radioactive waste. For decades, following historical industry practices, chromate has been added to the cooling water (~450 ppm at pH 9-11) to effectively inhibit corrosion, ensuring cooling coil longevity. Inspections of failed coils reveal that chromate-treated surfaces are generally well-preserved.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

M4SF-20LL010302042: Process Model for Radionuclide Incorporation into Corrosion Products

This progress report (Level 4 Milestone Number M4SF-20LL010302042) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline Activity Number SF-20LL010302041. The research is focused on actinide and radionuclide sequestration in steel corrosion products. Fuel matrix degradation models suggest that the near field is likely to be reducing at the time of canister breaching, steel corrosion, and radionuclide release, but more oxidizing conditions may prevail in the far field. The incorporation of radionuclides into corrosion phases may limit the rate of radionuclide release by sequestering a portion of the radionuclide source term. For these reasons there is a need to evaluate the incorporation of Pu and other radionuclides into various Fe-oxide phases, and to understand the behavior of coprecipitated phases during mineral recrystallization processes and during re-oxidation events. Radionuclide coprecipitation with Fe minerals may impact long-term repository performance and is an ongoing research focus at Lawrence Livermore National Laboratory.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Production, Purification, and Applications of a Potential Theranostic Pair: Cobalt-55 and Cobalt-58m

The emerging success of [68Ga/177Lu]Ga/Lu-DOTATATE as a theranostic pair has spurred interest in other isotopes as potential theranostic combinations. Here, we review cobalt-55 and cobalt-58m as a potential theranostic pair. Radionuclidically pure cobalt-55 and cobalt-58m have been produced on small cyclotrons with high molar activity. In vitro, DOTATOC labeled with cobalt has shown greater affinity for SSTR2 than DOTATOC labeled with gallium and yttrium. Similarly, [58mCo]Co-DOTATATE has shown improved cell-killing capabilities as compared to DOTATATE labeled with either indium-111 or lutetium-177. Finally, PET imaging with an isotope such as cobalt-55 allows for image acquisition at much later timepoints than gallium, allowing for an increased degree of biological clearance of non-bound radiotracer. We discuss the accelerator targetry and radiochemistry used to produce cobalt-55,58m, emphasizing the implications of these techniques to downstream radiotracers being developed for imaging and therapy.

60 APPLIED LIFE SCIENCES↗