Electron Accelerators for Radioisotope Production
General overview talk of mechanisms and energies associated with electron-beam radioisotope photonuclear production. A survey with all content freely available in public domain.
Satogata, Todd↗
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Photonuclear Production of 67 Cu From Gallium
Copper-67 is a radioisotope of interest for medical imaging and therapy as well as for under- standing stellar and interstellar evolution pertaining to the formation of proton-rich nuclei. Since 67 Cu decays 100% to 67 Zinc, understanding this reaction can shed light on the abundance of this and other p-nuclei elements in the universe. Here, the photonuclear production of 67 Cu from 71 Ga and natural gallium is examined as an alternative to its photoproduction from zinc. Two research and development production runs were performed at Thomas Jefferson National Accelerator Facility using an electron linac. During the first run, an 805-W, 30.9-MeV beam was used to irradiate a 1-mm tungsten radiator to create a bremsstrahlung flux. The resulting gamma photons irradiated 50.9 g of natural gallium encased in a graphite crucible for 24.2 h; 7.02 Bq/W∙s∙kg of 67 Cu activity was produced. During the second run, a 4380-W, 31.5-MeV beam was used for 12.0 h on the same target containing 60 g of natural gallium; 6.41 Bq/W∙s∙kg of 67 Cu activity was produced. Because of the difficulties in spectroscopically differentiating 67 Cu from 67 Ga, prior to each run, an isotopically pure 71 Ga disk was irradiated using a 100-W beam for 1 h, at the same respective energies. Finally, these baseline irradiations allowed for separation of 67 Cu from 67 Ga in the spectroscopic measurements of the natural gallium targets.
07 ISOTOPE AND RADIATION SOURCES↗
Photon Activation Analysis in Gallium, Nickel, and Vanadium
Here this research explored the development of the photonuclear production method of 67 Cu from 71 Ga as well as 47 Sc from 51 V. Both products serve as high-demand research medical radioisotopes. Furthermore, an understanding of these reactions is significant to fundamental nuclear physics and astrophysics. Bremsstrahlung flux was induced by an electron linac and a 1-mm tungsten radiator. Irradiation of gallium oxide powder, 98.78% pure 71 Ga, and a natural vanadium foil at 30.9 MeV and 100 W for 1 h produced 64.4 ± 0.4 Bq/W·s·kg of 67 Cu and 164 ± 3.1 Bq/W·s·kg of 47 Sc. A secondary irradiation with 99.6% pure 71 Ga and natural vanadium at 31.5 MeV and 100 W for 1.1 h produced 79.8 ± 0.9 Bq/W·s·kg of 67 Cu and 136 ± 7.2 Bq/W·s·kg of 47 Sc. The photoinduced activation is promising; however, further research into optimal geometry and power is required to maximize specific activity. Natural nickel was also irradiated to serve as a benchmark comparison. Effective cross sections for each reaction were inferred.
47Sc↗
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↗
Photonuclear cross sections for the 197 Au (𝛾, 𝑝𝑛) 195𝑚 Pt reaction near threshold
Platinum radioisotopes are of growing interest for targeted cancer therapy and diagnostic imaging because their decay delivers highly localized radiation doses in tissue, herewith enabling precise DNA damage through Auger-electron emission. Developing production technologies that provide platinum isotopes with high specific activity is essential in radioisotope therapy. Photonuclear reactions on stable nuclei offer a viable accelerator-based route for isotope production when supported by reliable cross-section data. We report photonuclear cross-section measurements for the 197 Au(γ, pn) 195m Pt reaction at incident γ-ray energies of 27, 29, and 31 MeV using the activation method. The measurements were performed by irradiating a stack of concentric-ring gold targets with a quasi-monoenergetic γ-ray beam provided by the High Intensity Gamma-ray Source (HI γS). The induced 195m Pt activity was quantified using off-line γ-ray spectroscopy. These data provide the first experimental constraints on the 197 Au(γ, pn) 195m Pt cross section in the near-threshold region. Furthermore, the comparison of the measured excitation function to PHITS and TALYS calculations indicates that the reaction becomes measurable only near 30 MeV and that substantially higher bremsstrahlung end-point energies are required for practically meaningful production.
190 ≤ A ≤ 219↗
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↗
Production of Radioisotopes of Scandium for Imaging and Therapy (Final Report)
This collaborative proposal aims developed techniques for the production of important medical isotopes of scandium; 43Sc, 44Sc, and 47Sc. By leveraging complementary infrastructure available at the three collaborating instructions, we have achieved a robust supply source for these isotopes.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Modeling and Analysis Support for Acceleratro-based Production of Mo-99
NorthStar Medical Radioisotopes, LLC, is in the process of commissioning a medical isotope production facility, which will use high-power electron accelerators to produce molybdenum-99 (Mo-99), the parent of technetium-99m (Tc-99m), through photonuclear reactions in molybdenum-100 (Mo-100). In this approach, a target comprising multiple thin disks of enriched molybdenum metal is bombarded with a 40-MeV electron beam. Electrons that impinge on the molybdenum target produce bremsstrahlung x-rays that cause the nuclear reaction. Because enriched Mo-100 is expensive, there is a desire to use as much beam power as possible to achieve maximum production yield and minimize the size of the target. This requirement leads to very high beam power density (heat deposition in the target), which creates challenging requirements for target cooling. In the latest concept developed by NorthStar, a stack of target (sintered molybdenum) disks is irradiated from two sides by a 40-MeV electron beam, with a total power of 250 kW (125 kW from each side). The target disks are cooled by pressurized helium gas flowing through channels between the disks. Inconel windows in the target housing form a pressure boundary between the helium within the housing and the evacuated beam tube.
07 ISOTOPE AND RADIATION SOURCES↗
Niowave Neutron Source Converter: Lead-Bismuth-Eutectic (LBE) Windowless Target Design and Evaluation
Los Alamos National Laboratory (LANL) is working with Niowave on the design and evaluation of their lead-bismuth-eutectic (LBE) windowless target (i.e., neutron source converter). Niowave plans to use 200 kW electron beam at 40 MeV beam energy to produce neutrons by photonuclear reaction with LBE. Then, the neutrons undergo fission at the surrounding uranium target assembly (UTA) to produce Molybdenum 99 (Mo-99) as a fission product, which eventually decays to Technetium-99 (Tc-99m). Tc-99m is one of important radioisotopes that is used for medical diagnostics. LANL conducted 3D multiphysics analysis for the Niowave neutron converter design and provided design assessment in thermohydraulic aspects. LANL conducted radiation transport calculations using Monte-Carlo N-Particle (MCNP) code with unstructured meshing scheme. The 3D volumetric heating profiles in the LBE and Stainless-Steel (SS) housing were imported into multiphase computational fluid dynamics (CFD) to obtain 3D temperature profiles of LBE and SS through conjugate heat transfer (CHT) analysis. The key findings are: LBE film thickness at the center of the beam is approximately 1.6 cm with a maximum LBE velocity of approximately 1.8 m/s, which is below a 2 m/s limit to avoid erosion issues on supporting structures; Heat deposition in the LBE peaks at ~1 cm depth from the LBE free-surface because of the forward interactions of electron, photon, and neutron with LBE; LBE maximum temperature is ~360 °C, which is below LBE evaporation initiative temperature, ~450 °C; LBE-SS interface temperature is ~350 °C, which is below the safety thermal limit to prevent severe corrosion on SS. The results indicate that Niowave’s neutron converter design satisfies both hydraulic and thermal criteria for safe operation. By virtue of such computational analysis, Niowave can move toward establishing an experimental setup to experimentally test their LBE neutron converter. The following sections describe the detailed work done by LANL.
43 PARTICLE ACCELERATORS↗
Testing of Helium-Cooled Metal Molybdenum Disk Target
NorthStar Medical Radioisotopes LLC is planning to produce an important medical radioisotope, molybdenum-99 (Mo-99), through photonuclear reaction on molybdenum-100 (Mo-100). In this approach, molybdenum metal will be bombarded with a 40-MeV electron beam. Because enriched Mo-100 is expensive, it is desired to use as much beam power as possible to achieve maximum production yield and minimize target mass. This objective leads to very high beam power density (heat deposition in the target), which sets challenging requirements for cooling. Together with scientists at Los Alamos National Laboratory, a team at Argonne National Laboratory has developed and demonstrated a cooling approach using pressurized helium, which allows for efficient heat removal. One of the main challenges in this approach is the management of the heat load on the target window. The target window separates the high-pressure helium inside the target from the vacuum in the beamline, so it is constantly under stress from differential pressure. Also, the window is cooled only by the helium gas flowing on one side, making the window cooling even more challenging. High heat deposition in the target disks also imposes a strict requirement on performance of the helium cooling system and thickness of the target disks. The target disks are produced from metal powder via a press-and-sinter process. The resulting disks do not possess tensile strength as high as solid molybdenum and might not survive the vibration from the high-velocity helium coolant and high thermal stress from beam heating. An Argonne team of scientists performed a series of tests at Argonne’s Low Energy Accelerator Facility (LEAF) [3-7]. This report describes two series of tests for scale down production target designs that utilize full-scale 29 millimeters diameter, 0.75 mm thick press-and-sintered disks. We performed two thermal tests with different beam parameters and configurations of the disk laminations. We compared the results of the window temperature measurements and cooling system parameters obtained in the experiments with those predicted by analytical calculations and Computation Flow Dynamic (CFD) simulations. Results of the experiments and calculations are presented below.
36 MATERIALS SCIENCE↗
Testing of Helium Cooled Metal Molybdenum Disk Target System
NorthStar Medical Radioisotopes LLC is planning to produce the important medical radioisotope molybdenum-99 (Mo-99) through a photonuclear reaction on molybdenum-100 (Mo-100). In this approach, multiple thin disks of enriched molybdenum metal will be bombarded with a 40-MeV electron beam. Because enriched Mo-100 is expensive, we intend to use as much beam power as possible to achieve maximum production yield and minimize the size of the target. This requirement leads to very high beam power density (heat deposition in the target), which sets challenging requirements for cooling. Together with scientists at Los Alamos National Laboratory, a team at Argonne National Laboratory has developed and demonstrated a cooling approach using pressurized helium, which allows for efficient heat removal. One of the challenges in this approach is the management of the heat load on the target window. The target window separates the high-pressure helium atmosphere inside the target from the vacuum in the beamline, so it is constantly under stress from differential pressure. Also, the window is cooled only by the helium gas flow from one side, making the window design challenging. High heat deposition in the target disks also imposes a strict requirement on performance of the helium cooling system and thickness of the target disks. The target disks are produced from metal powder via a press-and-sinter process. The resulting disks do not possess as high a tensile strength as solid molybdenum and might not survive the vibration from the high-velocity helium coolant and the high thermal stress from beam heating.
42 ENGINEERING↗
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↗
IAEA Photonuclear Data Library 2019
Here, photo-induced reaction cross section data are of importance for a variety of current or emerging applications, such as radiation shielding design and radiation transport analyses, calculations of absorbed dose in the human body during radiotherapy, physics and technology of fission reactors (influence of photo-reactions on neutron balance) and fusion reactors (plasma diagnostics and shielding), activation analyses, safeguards and inspection technologies, nuclear waste transmutation, medical isotope production and astrophysical applications. To address these data needs the IAEA Photonuclear Data library was produced in 1999, containing evaluated photo-induced cross sections and neutron spectra for 164 nuclides which were deemed relevant for the applications. Since the release of the IAEA Photonuclear Data Library however, new experimental data as well as new methods to assess the reliability of experimental cross sections have become available. Theoretical models and input parameters used to evaluate photo-induced reactions have improved significantly over the years. In addition, new measurements of partial photoneutron cross sections using mono-energetic photon beams and advanced neutron detection systems have been performed allowing for the validation of the evaluations and assessments of the experimental data. Furthermore, technological advances have led to the construction of new and more powerful gamma-beam facilities, therefore new data needs are emerging. We report our coordinated efforts to address these data needs and present the results of the new up-to-date evaluations included in the new updated IAEA Photonuclear Data Library consisting of 219 nuclides. The new library includes 188 new evaluations produced by the CRP evaluators, and one evaluation taken from the JENDL/PD-2016 library, while 20 evaluations were retained from the previous 1999 IAEA Photonuclear Data Library. In most of the cases, the photon energy goes up to 200 MeV. A total of 55 nuclides are new in this library reflecting the progress in measurements but also the developing data needs. In this paper we discuss the new assessment method and make recommendations to the user community in cases where the experimental data are discrepant and the assessments disagree. In addition, in the absence of experimental data, we present model predictions for photo-induced reaction cross section on nuclides of potential interest to medical radioisotope production.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Simulations Supporting the Development of Northstar's Indirect Beam Parameters Monitoring System
NorthStar Medical Radioisotopes, LLC is planning to produce the important medical radioisotope molybdenum-99 (Mo-99), the parent of technetium-99m (Tc-99m), through photonuclear reactions in molybdenum-100 (Mo-100). In this approach, a target comprising multiple thin disks of enriched molybdenum metal is bombarded with a 40-MeV electron beam. Electrons impinged on the molybdenum target produce bremsstrahlung X-rays that cause the nuclear reaction. Because enriched Mo-100 is expensive, there is a desire to utilize as much beam power as possible to achieve maximum production yield and minimize the size of the target. This requirement leads to very high beam power density (and heat deposition in the target), which creates challenging requirements for the cooling of the target. The critical part of the target is the target window. It separates the high-pressure helium cooled target from the vacuum beamline and the subject of structural and thermal stress. The temperature of the target window is proportional to the energy density deposited by the beam, so it is critical to maintain the desired beam profile on the target window. The feasibility of indirectly monitoring the maximum energy density of the beam on the beam window through beam losses at the main collimator (Collimator) before the production target was verified. A model of the NorthStar beam transport line was constructed for this purpose using MAD-X and Tao/Bmad codes. Beam optics were computed for the standard operational scenario, followed by an investigation involving approximately 400 cases with parameter variations in the last tuning quadrupoles. This was done to assess the correlation between losses in the collimator and the peak energy density on the target. We developed a model to explore the potential application of Optical transition radiation (OTR) for controlling beam parameters in the NorthStar beam delivery system. This model was based on a generic formula derived from the fundamental solution of the inhomogeneous wave equation of the vector potential, and allowed us to consider various surfaces, even those with irregular or random features, using numerical integration. We applied the model to OTR generated by relativistic electrons impacting an Inconel® 718 beam window. We examined cases with different levels of the window’s surface roughness, ranging from 0.5 to 3.0 microns of root square mean (RMS) deviation. The results of the OTR simulations provided distributions of OTR photons that can be used to study the limitations of optical systems for controlling beam parameters.
43 PARTICLE ACCELERATORS↗