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Stepinski, Dominique C.

Publications and source records attributed to Stepinski, Dominique C..

Direct Down-scale Experiments of Concentration Column Designs for SHINE Process

Argonne is assisting SHINE Medical Technologies in their efforts to become a domestic Mo-99 producer. The SHINE accelerator-driven process uses a uranyl-sulfate target solution for the production of fission-product Mo-99. Argonne has developed a molybdenum recovery and purification process for this target solution. The process includes an initial Mo recovery column followed by a concentration column to reduce the product volume from 15-25 L to < 1 L prior to entry into the LEU Modified Cintichem (LMC) process for purification.1 This report discusses direct down-scale experiments of the plant-scale concentration column design, where the effects of loading velocity and temperature were investigated.

42 ENGINEERING↗

Development Of ABEC Column For Separation Of Tc-99 From Northstar Dissolved Target Solution

Batch and column breakthrough experiments were performed to determine isotherms and mass-transfer parameters for adsorption of Tc on aqueous biphasic extraction chromatographic (ABEC) sorbent in two solutions: 200 g/L Mo, 5.1 M K + , 1 M OH - , and 0.1 M NO 3 - (Solution A) and 200 g/L Mo, 9.3 M K + , 5 M OH - , and 0.1 M NO 3 - (Solution B). Good agreement was found between the isotherm values obtained by batch and column breakthrough studies for both Solutions A and B. Potassium-pertechnetate intra-particle diffusivity on ABEC resin was estimated by VERSE simulations, and good agreement was found among a series of column-breakthrough experiments at varying flow velocities, column sizes, and technetium concentrations. However, testing of 10 cc cartridges provided by NorthStar with Solutions A and B did not give satisfactory results, as significant Tc breakthrough was observed and ABEC cartridge performance varied widely among experiments. These different experimental results are believed to be due to inconsistent preparation of the ABEC resin prior to packing and/or inconsistent packing.

36 MATERIALS SCIENCE↗

Compendium of Phase-I Mini-SHINE Experiments

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.

43 PARTICLE ACCELERATORS↗

SHINE and Mini-SHINE Column Designs for Recovery of Mo from 140 g-U/L Uranyl Sulfate

Argonne is assisting SHINE Medical Technologies (SHINE) in their efforts to develop an accelerator-driven process that utilizes a uranyl-sulfate solution for the production of fission Mo-99. In an effort to design a Mo-recovery system for the SHINE project using low-enriched uranium (LEU), we conducted batch, breakthrough, and pulse tests to determine the Mo isotherm, mass-transfer zone (MTZ), and system parameters for a 130 g-U/L uranyl sulfate solution at pH 1 and 80°C, as described previously. The VERSE program was utilized to calculate the MTZ under various loading times and velocities. The results were then used to design Mo separation and recovery columns employing a pure titania sorbent (110-μm particles, S110, and 60 Å pore size). The plant-scale column designs assume Mo will be separated from 271 L of a 141 g-U/L uranyl sulfate solution, pH 1, containing 0.0023 mM Mo. The VERSE-designed recovery systems have been tested and verified in laboratory-scale experiments, and this approach was found to be very successful.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Low-enriched uranium high-density target project. Compendium report

At present, most 99 Mo is produced in research, test, or isotope production reactors by irradiation of highly enriched uranium targets. To achieve the denser form of uranium needed for switching from high to low enriched uranium (LEU), targets in the form of a metal foil (~125-150 µm thick) are being developed. The LEU High Density Target Project successfully demonstrated several iterations of an LEU-fission-based Mo-99 technology that has the potential to provide the world’s supply of Mo-99, should major producers choose to utilize the technology. Over 50 annular high density targets have been successfully tested, and the assembly and disassembly of targets have been improved and optimized. Two target front-end processes (acidic and electrochemical) have been scaled up and demonstrated to allow for the high-density target technology to mate up to the existing producer technology for target processing. In the event that a new target processing line is started, the chemical processing of the targets is greatly simplified. Extensive modeling and safety analysis has been conducted, and the target has been qualified to be inserted into the High Flux Isotope Reactor, which is considered above and beyond the requirements for the typical use of this target due to high fluence and irradiation duration.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Optimization of SHINE Process: Design and Verification of Plant-Scale AG 1 Anion-Exchange Concentration Column and Titania Sorbent Pretreatment

Argonne National Laboratory has developed a Mo-recovery and -purification system for the SHINE medical technologies process, which uses a uranyl sulfate solution for the accelerator-driven production of Mo-99. The objective of this effort is to reduce the processing time for the acidification of the Mo-99 product prior to loading onto a concentration column and concentration of the Mo-99 product solution. Two methods were investigated: (1) the replacement of the titania concentration column by an anion-exchange column to decrease processing time and increase the radioiodine-decontamination efficiency and (2) pretreatment of the titania sorbent to improve its effectiveness for the Mo-recovery and -concentration columns. Promising results are reported for both methods.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Plant-Scale Concentration Column Designs for SHINE Target Solution Utilizing AG 1 Anion Exchange Resin

Argonne is assisting SHINE Medical Technologies (SHINE) in their efforts to develop SHINE, an accelerator-driven process that will utilize a uranyl-sulfate solution for the production of fission product Mo-99. An integral part of the process is the development of a column for the separation and recovery of Mo-99, followed by a concentration column to reduce the product volume from 15-25 L to <1 L. Argonne has collected data from batch studies and breakthrough column experiments to utilize the VERSE (Versatile Reaction Separation) simulation program (Purdue University) to design plant-scale product recovery and concentration processes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Verification Of Column Design for Recovery of Mo from Low-Enriched Uranium Target Using Irradiated Target Tracer Solution

The Conversion Program of the Global Threat Reduction Initiative (GTRI) is developing technology necessary to enable the conversion of civilian facilities using high-enriched uranium (HEU) to low-enriched uranium (LEU) for fuels and targets. The conversion of conventional HEU dispersion targets to LEU for the production of 99Mo requires approximately five times the uranium to maintain the 99Mo yield per target. Under GTRI, Argonne is developing two front end options to the current processes to allow the use of LEU-foil targets. In both processes, the aim is to produce a product after the front end that will be compatible with current purification operations and that will, with the same number of targets irradiated, provide the same or higher yield of 99Mo at the end of processing. The goal of the front-end process is to deliver a product solution that is of the same or higher Mo purity than the current solution and is of equal or better compatibility with current purification processes.

Column Design↗

Documenting Dual-Column Experiment with Mini-SHINE Solution

Argonne National Laboratory (Argonne) is assisting SHINE Medical Technologies (SHINE) in developing a production method and recovery and purification processes for molybdenum 99 (Mo-99) using an accelerator-driven, subcritical target consisting of an aqueous uranyl-sulfate solution. An integral part of the process is the development of a column for the separation and recovery of Mo-99, followed by a concentration column to reduce the product volume from 15–25 L to <1 L prior to entry into the low-enriched uranium (LEU)-Modified Cintichem purification process. Argonne has developed plant-scale column designs for the initial Mo-recovery column and the concentration column.

Stepinski, Dominique C.↗