Engineering topics
Publications and source records attributed to Gromov, Roman.
Traditional methods of dissolving uranium in nitric acid involve the generation of nitrogen oxide gases (NO x ), which not only are hazardous but also contribute to increased pressure within the dissolver. When uranium metal foils are dissolved in nitric acid, a series of redox reactions occurs, leading to the formation of NO x , such as nitrogen dioxide (NO 2 ) and nitric oxide (NO).
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.
Argonne National Laboratory (Argonne) is assisting NorthStar Medical Technologies in the development of a domestic supply of 99 Mo. Specifically, the present study focuses on the production of 99 Mo-feed solution used by the RadioGenix™ 99m Tc generator. During the target-irradiation phase of production, impurities can potentially be introduced into the feed, and can lead to disturbance of ligand- 99m Tc complexation chemistry and contamination of the final radiopharmaceutical that directly interacts with the patient. To address this issue, Argonne performed irradiations and chemical processing to identify whether the potential contamination of He flow with hydrocarbon oil during irradiation affects the radiochemical purity of the final K 2 MoO 4 (K 2 TcO 4 ) in 5M KOH solution. To mimic the conditions of real irradiation at NorthStar, Argonne used its electron linear accelerator and Van de Graaff facilities, heated the target and oil source to >800°C, and controlled oxygen in the presence of He during irradiation. Following irradiation, scanning electron microscopy (SEM) and carbon analysis (CA) were used to detect carbon contamination on the solid targets. The radiochemical purity of the dissolved targets was studied via thin-layer paper chromatography (TLC). As a result of these experiments, small regions of the surface of some irradiated disks were found to be high in carbon, but the total carbon content was still negligible in comparison to the reference sample, which had experienced no irradiation or contact with oil. The summarized results from the SEM, CA, and TLC tests lead to the conclusion that even an excess of oil and heating during irradiation do not affect the radiochemical purity of the final product.
Production of 99 Mo by the 100 Mo (γ, n) 99 Mo reaction through the bremsstrahlung process using an electron accelerator is one of the feasible options currently pursued by several countries. In this work, we report experimental results on identification of side-reaction products after the irradiation of natural and enriched 100 Mo targets. Side-reaction products identified include various Mo, Nb and Zr isotopes. Comparison of experimentally determined reaction production rates with those determined based on theoretical cross-sections will be presented. Moreover, activation products formed due to presence of impurities introduced during the manufacturing of the Mo targets will also be discussed.
For six days, a 12-mm-diameter metal molybdenum target containing 15 enriched Mo-100 disks was irradiated at Argonne’s electron linac. This report describes the irradiation conditions and the means used to process the targets for shipment to NorthStar Medical Isotopes, LLC, for feed to their RadioGenixTM technetium generator.
NorthStar Medical Isotope, LLC, is planning to produce 99 Mo through a γ,n reaction on 100 Mo. This pathway for 99 Mo production relies on the use of high-power electron accelerators, which are not currently commercially available. IBA Industrial announced in its Summer 2017 newsletter (http://iba-industrial.com/emailing/2017-beamline/index.html) that they have begun working on pulsed Rhodotron features (New Horizon project). This accelerator is capable of producing a high power and high energy electron beam suitable for production via a photonuclear route. Argonne National Laboratory (Argonne), in collaboration with Los Alamos National Laboratory (LANL), provided assistance to NorthStar in technology development. Over the course of several years, we have conducted several demonstrations of the technology that proved the feasibility of photo-nuclear approach. The target, designed by LANL, is composed of a series of 99 Mo disks held in a target holder with cooling gaps between the thin disks. Cooling of the target is provided by flowing helium gas under high pressure through the target holderHandling the high-power beam requires a carefully designed beam transport system because of likely vacuum failure if the beam strikes an uncooled part of the system. This publication summarizes recommendations on the beam transport line equipment, costs, and on the optional components.
NorthStar Medical technologies is planning to produce Mo-99 through the photo-nuclear reaction Mo-100 (γ,n) Mo-99 utilizing multiple high-power electron accelerators. In this approach, the production target consists of multiple thin disks of metal Mo-100 cooled by helium gas at high (300–400 psi) pressure [4]. The cost of enriched Mo-100 is on the order of $500 - 1,000 per gram, which makes a smaller target desirable and requires achieving the highest possible electron flux on the target. The heat deposition in the entrance window limits the maximum flux because the window separates the vacuum in the accelerator beam line from the high-pressure helium in the target and is only cooled on one side by the helium flow. Because the window is continuously under stress from the helium pressure and the heat from the electron beam, it is desirable to estimate a lifetime for the window and develop a replacement schedule for the target holder. Such an estimate requires the ability to predict changes in the window material properties under electron irradiation. Candidate materials for the Mo-99 production target window are Inconel 718, 250 maraging steel, and beryllium. These materials encompass a wide range of thermal conductivity, thermal expansion coefficients, Young’s modulus, tensile strength and tensile ductility. The Mo-99 target window is subjected to internal pressure from the helium coolant and thermal stresses. The operating conditions and relative advantages of each material have been described previously [1]. The current work investigates the effects of electron irradiation on the tensile properties of these materials. Axial tensile tests were conducted with electron-irradiated samples and results were compared to baseline results generated for as-fabricated materials.
Argonne National Laboratory, in cooperation with NorthStar Medical Technologies and Los Alamos National Laboratory, is developing a technology for the production of Mo-99 via photonuclear reaction on a Mo-100 target. The new facility will utilize electron accelerators with high beam power.
As a first step to produce Mo-99 in phase 2 of the Argonne Molybdenum Research Experiment (AMORE), we are performing a series of tests in which Mo-99 and natural Mo are added to a target vessel and the target solution is processed to recover Mo. This report describes a Mo-99 spike test with pH 1 sulfuric acid that was performed with an electron beam on a depleted uranium (DU) target.
After numerous delays, the test of the 29 mm diameter target was conducted on 8/18/2017. The complete target design report, dated 8/15/2016, is reproduced below for completeness. This describes in detail the 10 disk target with varying thickness disks. The report presents and discusses the test results. In brief summary, there appears to have been multiple instrumentation errors. Measured temperatures, pressures and IR camera window temperature measurement are all suspect. All tests were done at 35 MeV, with 171 μA current, or 6 kW of beam power.
Molybdenum-99, the mother of Tc-99m, can be produced from fission of U-235 in nuclear reactors and purified from fission products by the Cintichem process, later modified for low-enriched uranium (LEU) targets. The key step in this process is the precipitation of Mo with α-benzoin oxime (ABO). The stability of this complex to radiation has been examined. Molybdenum-ABO was irradiated with 3 MeV electrons produced by a Van de Graaff generator and 35 MeV electrons produced by a 50 MeV/25 kW electron linear accelerator. Dose equivalents of 1.7–31.2 kCi of Mo-99 were administered to freshly prepared Mo-ABO. Irradiated samples of Mo-ABO were processed according to the LEU Modified-Cintichem process. The Van de Graaff data indicated good radiation stability of the Mo-ABO complex up to ~15 kCi dose equivalents of Mo-99 and nearly complete destruction at doses >24 kCi Mo-99. The linear accelerator data indicate that even at 6.2 kCi of Mo-99 equivalence of dose, the sample lost ~20% of Mo-99. The 20% loss of Mo-99 at this low dose may be attributed to thermal decomposition of the product from the heat deposited in the sample during irradiation.
Argonne National Laboratory is assisting SHINE Medical Technologies in their efforts to develop the technology to become a domestic Mo-99 producer using low-enriched uranium (LEU). Mini-SHINE experiments are being performed with the high-current electron linear accelerator (linac) at Argonne. The target solution is a 90-150 g-U/L LEU uranyl sulfate at pH 1. In Phase 1, the convertor was tantalum with a maximum beam power on the convertor of 10 kW, and the target solution was limited to 5 L. This configuration generated a peak fission power density of 0.05 W/mL. Nine experiments were performed between February and October 2015. Results are reported and discussed for each experiment regarding the off-gas analysis system, the sampling and Mo-recovery operation, and the Mo-product concentration and purification system. In Phase 2, the convertor will be depleted uranium; beam power will increase to 20 kW; and the solution volume will be 18 L. This configuration will generate a fission power density of up to 1 W/mL.
NorthStar Medical Technologies is pursuing production of an important medical isotope, Mo-99, through a photo-nuclear reaction of a Mo-100 target using a high-power electron accelerator. The current target utilizes an Inconel 718 window. The purpose of this study was to evaluate other candidate materials for the target window, which separates the high-pressure helium gas inside the target from the vacuum inside the accelerator beamline and is subjected to significant stress. Our initial analysis assessed the properties (density, thermal conductivity, maximum stress, minimum window thickness, maximum temperature, and figure of merit) for a range of materials, from which the three most promising were chosen: Inconel 718, 250 maraging steel, and standard-grade beryllium. These materials were subjected to further analysis to determine the effects of thermal and mechanical strain versus beam power at varying thicknesses. Both beryllium and the maraging steel were calculated to withstand more than twice as high beam power than Inconel 718.
Four irradiations of ultra-high-purity natural Mo targets and one irradiation using 97.4% Mo-100-enriched material were performed. The purpose of these irradiations was to determine whether the presence of Sn stabilizer in the H 2 O 2 used for the dissolution of sintered Mo disks can affect the radiochemical purity of the final K 2 MoO 4 in 5M KOH solution. Results from radiochemical purity tests performed using thin-layer paper chromatography show that even 2– 3× excess of Sn-stabilized H 2 O 2 typically used for dissolution of sintered Mo disks did not affect the radiochemical purity of the final product.
A thorough test of the thermal performance of a target for Mo 99 production using solid Mo 100 target to produce the Mo 99 via a gamma-n reaction has previously been conducted at Argonne National Laboratory (ANL). The results are reported in “Zero Degree Line Mo Target Thermal Test Results and Analysis,” LANL report Number LA-UR-15-23134 dated 3/27/15. This target was comprised of 25 disks 1 mm thick and 12 mm in diameter, separated by helium coolant gaps 0.5 mm wide. The test reported in the above referenced report was conducted with natural Mo disks all cut from commercial rod. The production plant will have Mo 100 disks pressed and sintered using a process being developed at Oak Ridge National Laboratory (ORNL). The structural integrity of press-and-sinter disks is of some concern. The test reported herein included 4 disks made by the ORNL process and placed in the high heat, and therefore high thermal stress, region of the target. The electron beam energy was 23 MeV for these tests. Beam spot size was 3.5 mm horizontal and 3 mm vertical, FWHM. The thermal stress test of pressed-and-sintered disks resulted in no mechanical failures. The induced thermal stresses were below yield stress for natural Mo, indicating that up to that stress state no inherent deficiencies in the mechanical properties of the fabricated disks were evident.
Explore the source record for details and available documents.
In order to test and verify the experimental designs at the linear accelerator (LINAC), several micro-scale bubble ("micro-bubble") experiments were conducted with the 3-MeV Van de Graaff (VDG) electron accelerator. The experimental setups included a square quartz tube, sodium bisulfate solution with different concentrations, cooling coils, gas chromatography (GC) system, raster magnets, and two high-resolution cameras that were controlled by a LabVIEW program. Different beam currents were applied in the VDG irradiation. Bubble generation (radiolysis), thermal expansion, thermal convection, and radiation damage were observed in the experiments. Photographs, videos, and gas formation (O 2 + H 2 ) data were collected. The micro-bubble experiments at VDG indicate that the design of the full-scale bubble experiments at the LINAC is reasonable.