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Adapting LEU-Modified Cintichem Process for Processing Up to 750 Grams of Uranium Targets

Argonne National Laboratory (Argonne) developed a low-enriched uranium (LEU)-modified Cintichem (LMC) process to enable production and purification of fission-produced molybdenum-99 (Mo-99) from LEU foil targets. This separation scheme starts with nitric acid (HNO 3 ) dissolution of irradiated LEU foil targets that yields an approximate final volume of 2 L. The dissolved uranium solution containing fission products, including Mo-99, is then treated by loading the solution on a titania-based recovery column to separate Mo-99 from bulk uranium. After several washing steps, Mo and other fission products are stripped from the titania column using sodium hydroxide (NaOH). The eluate is then acidified using nitric acid and subsequently processed for final purification using the LMC process. Uranium and most fission products are not adsorbed on the titania column but are eluted (i.e., removed using a solvent) during the wash steps; they can be purified and recycled into new uranium targets.

07 ISOTOPE AND RADIATION SOURCES↗

PNNL's Characterization Summary for MP-2 Experiment

Characterization of as-fabricated fuel was performed at Pacific Northwest National Laboratory (PNNL) in accordance with the characterization plan for the fabrication of U 10Mo plate fuel for the U.S. High Performance Research Reactor conversion program’s Fuel Fabrication Pillar (INL 2021). Similar characterization work is also being performed at Idaho National Laboratory to provide a detailed understanding of the as-fabricated foils that would be irradiated in the Mini-Plate 2 (MP 2) experiment. Under the MP 2 characterization plan, foils are studied that have different fabrication parameters (such as rolling condition, rolling thickness reduction, co-rolling with Zr layers). Similar samples from master foils were sent to both the organizations, so that the testing and analysis can be done independently using similar equipment and standardized measurement and analysis procedures. A final, consolidated report will be prepared based on this work and will summarize all the information obtained from the two laboratories. The MP 2 experiment will provide an opportunity to understand the effects of processing conditions on the final fuel microstructure, to compare results obtained independently, and achieve a two-way validation. In Fiscal Year 2022, PNNL received five MP 2 cast (PD STD2) samples to examine the foils’ chemistry and microstructure. For each cast sample, PNNL received samples from three different locations. PNNL also received and characterized 24 U 10Mo foil samples, by sectioning four pieces/specimens from each foil, in accordance with the MP 2 Characterization Plan (INL 2021). These 24 samples consist of four types of foils from BWX Technologies: 0.047 in. thick hot-rolled and annealed samples with Zr layers; 0.025 in. thick cold-rolled and annealed samples with Zr layers; 0.0105 in. thick cold-rolled and annealed samples with Zr layers. Along with these, PNNL also received four plates with Zr layers that were 0.025 in. and 0.0105 in. thick. This report describes the results of PNNL’s MP 2 foil characterization. Microstructure, Mo homogeneity, carbide fraction and morphology, U 10Mo foil thickness, and Zr thickness were evaluated in both the longitudinal and transverse directions for all the foils of the three different thicknesses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

U-rich U-Mo Solidus, Liquidus, Enthalpy, and Thermal Diffusivity

Several material properties have been studied as a function of composition as part of the USHPRR effort to use U-10Mo for LEU monolithic fuel foils, with special attention to areas where simulation outcomes can be improved. The liquidus and solidus phase boundaries are important for engineering design of processing parameters and for predicting the degree of microsegregation within initial castings. The numerous phase diagram constructions available in the literature differ significantly in their solid/liquid boundary definitions, therefore, an experimental strategy was employed in order to resolve some of the discord. That strategy focuses not on proving any singular point, but instead to provide data with highly characterized uncertainty. The data presented here is the most consistent with the U-rich liquidus and solidus boundaries provided by H. Okamoto (2012), Berche et al. (2011), and Mardon et al. (1959). The recently suggested change in the peritectic reaction temperature (to 1302 K) suggested by Berchè and adopted by Okamoto is also supported, but with lower confidence. The enthalpy of fusion is a basic characteristic of the solidification reaction property for which is required for both research-oriented predictions of behavior and development of applied design strategies for casting engineering. It has been determined that an admixture model for the heat of fusion between U BCC and Mo BCC is a reasonable assumption within the composition region of interest, though limitations of the measurement accuracy impacts the ability to support any trends more detailed than this baseline behavior. A limited number of thermal diffusivity measurements were also performed into the gamma region to provide additional information for solidification modeling and simulations as well as a check on the component properties of thermal conductivity, density, and heat capacity.

36 MATERIALS SCIENCE↗

NCERC-CL TREAT Free Field Characterization Foil Reaction Rate Results

This report summarizes the analysis and preliminary MCNP reaction rate modeling of free field characterization measurements performed in the Transient Reaction Test Facility (TREAT) at Idaho National Laboratory (INL) between 12/18/2023 and 2/22/2024. A series of seven irradiations were performed using the Big-BUSTER (Broad Use Specimen Transient Experiment Rig) core configuration. Foil sets including 19.5% LEU-Zr alloy wire, S, Au, Fe, Ni, Co, Ti, and Zr were deployed in each irradiation. Identical foil sets were supplied to Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL), and INL. All foils were supplied by INL. Additional details on the experiment can be found in [2]. The foil sets were shipped to the National Criticality Experiments Research Center Counting Laboratory (NCERC-CL) branch at LANL (NCERC-CL NISC) and were received on 3/25/2024. Additional details on receipt and counting are reported in [3]. All reactor dosimetry measurements were performed in adherence to the ASTM standards applicable to reactor dosimetry. Measured reaction rates from Au, Co, Fe, Ni, and Ti are reported. Select reaction rate ratios and simulated reaction rates and ratios are discussed. Reaction rates for all measured reaction products were modeled with MCNP 6.3.1 and a TREAT input deck supplied by Edward Lum. Neutron emission estimates calculated using the measured and simulated reaction rates show excellent agreement between the three fast-threshold n-p reactions with the percent differences being < 9% between the three reactions. The capture reactions had poorer, but still reasonable, agreement with < 20% percent differences between the neutron emission estimates of the three capture reactions. The percent difference between the fast-threshold and capture reactions is ∼ 100% for each reaction. This supports the TREAT model is not accurately modeling the neutron spectrum and additional measurements are required to characterize TREAT and match measurements to simulation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Development of a thermal creep model for aluminum alloy 6061 cladding in U-10Mo monolithic fuel plates

Plate-type fuel elements consisting of a high-density, low-enriched uranium (LEU) U–10Mo-based fuel foil encapsulated in an aluminum alloy (AA) cladding are fabricated using the hot isostatic pressing (HIP) technique. During the HIP process, the fuel plate system is heated to 560 °C, then cooled to room temperature. This heat cycle significantly affects the mechanical properties of the aluminum cladding, and experimental investigations have shown that, post-HIP bonding, the mechanical properties of the aluminum cladding transition from those of AA 6061-T6 to something closer to the O temper. More specifically, the ultimate strength of the cladding decreases while its ductility increases, making it challenging to capture the changes in mechanical behavior and material properties. Understanding the residual stresses generated during the HIP process is critical for assessing the fuel plate’s integrity under various temperature, pressure, and irradiation. To simulate the HIP bonding process, the elastic, plastic, and thermal properties of the cladding are assumed to be similar to those of AA 6061-O temper. However, the primary challenge lies in the lack of available data for the creep model of the AA 6061 cladding during this transient process of HIP. The present study focuses on developing a computational model that predicts the creep behavior of the aluminum cladding in the fuel plates during the HIP process, as cladding creep significantly influences the residual stresses generated in U-10Mo fuel plates during HIP fabrication. Furthermore, as HIP bonding occurs at high temperatures that are nearing the melting point of aluminum, the present work considered a temperature-dependent Arrhenius-type creep model. In particular, a hyperbolic sine creep model is employed to estimate the creep properties of the as-fabricated aluminum cladding. In conclusion, the residual stresses predicted in the U-10Mo fuel when using the newly calibrated creep model closely align with the experimental measurements, validating the model’s accuracy.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Micro X-ray computed tomography examination of mini plate fuel with hot isostatic pressed aluminum cladding

In order to minimize proliferation risks and improve security of nuclear material, the United States high performance research and test reactors (USHPRR) program is tasked with converting nuclear reactors that are fueled with highly enriched uranium (HEU) fuels to operate with low-enriched uranium (LEU) nuclear fuels. One favorable LEU fuel configuration is plate fuel with a metallic uranium-molybdenum foil clad within an aluminum alloy (AA 6061). In this fuel, the aluminum cladding is bonded with a hot isostatic pressing (HIP) method to seal the cladding around the fuel meat. However, the HIP process parameters influence the cladding performance, as a defective or incomplete bond can cause a pathway for corrosion. Micro X-ray computed tomography (XCT), a nondestructive technique that provides volumetric imaging, can be applied to inspect fuel plate cladding at the engineering scale. In this work, XCT methodology was developed and successfully utilized to not only observe the bond line of unirradiated mini fuel plates, but to also identify subsurface abnormalities in the plates’ cladding. Importantly, in future work, this technique could be applied to fuel plates, pre- and post-irradiation, to quantify irradiation effects on cladding defects and bond line integrity.

36 MATERIALS SCIENCE↗

Computational Modeling of Multi-Pass Rolling Parameters Effect on Resulting Fuel Foil Shape

A focus of the U.S. Department of Energy is to improve production yield and reduce the cost of Low Enriched Uranium (LEU)-molybdenum alloy (U-10Mo) monolithic fuel plates that will be replacing High Enriched Uranium (HEU) oxide dispersion fuels used currently in the United States High Performance Research Reactors (USHPRR). One area of improvement is lowering the high transverse waviness and longitudinal waviness currently present within rolled foils prior to cladding to produce fuel plates. Traditional rolling manufacturing techniques for other metal foils use winders to pull and straighten the foil as it is rolled back and forth to the final thickness. This approach cannot be used to roll thin U-10Mo foils (0.008-0.025” thick) because only small castings can be rolled due to nuclear criticality safety concerns. As a result, the fuel foils are too short (1 m in length) to use traditional winders. Therefore, it is crucial to identify other rolling parameters (i.e., roller friction, axial tension load, roller diameter, and roll pass reduction percent) that might reduce transverse waviness and longitudinal waviness in the rolled fuel foil and develop a high-yield, low-cost multi-pass rolling manufacturing process. This report documents a systematic finite element modeling study to investigate the effects of numerous rolling parameters to reduce resulting transverse waviness and longitudinal waviness in the fuel foil during multi-pass rolling of U-10Mo foils. The rolling of a U-10Mo plate with initial dimensions of 1”x1”x 0.048” is modeled using Abaqus CAE. This rolling is modeled to undergo eight 20% reduction roll passes to a final fuel foil thickness of 0.01”. The elastic-plastic constitutive model of the U-10Mo alloy was input to the fuel foil rolling model. The rollers were modeled as rigid bodies. A comparison of rolling friction coefficients of 0.3 and 0.7 over a wide range of applied axial tension loads were investigated in order to evaluate the effect of using a lubricant during rolling. The effect of roller diameter on the resulting transverse waviness and longitudinal waviness of the fuel foil over a wide range of axial tension loads were also investigated by modeling rollers 7/8” and 3.75” in diameter. The results of this systematic finite element method study will aid manufacturers in producing low transverse waviness and reduced longitudinal waviness in U-10Mo fuel foils.

U-10Mo, FEA, Rolling, Residual Stress, Fuel Foil↗

Spot pattern welding scanning strategy for sensor embedding and residual stress reduction in laser-foil-printing additive manufacturing

Here, this paper aims to present spot pattern welding (SPW) as a scanning strategy for laser-foil-printing (LFP) additive manufacturing (AM) in place of the previously used continuous pattern welding (CPW) (line-raster scanning). The SPW strategy involves generating a sequence of overlapping spot welds on the metal foil, allowing the laser to form dense and uniform weld beads. This in turn reduces thermal gradients, promotes material consolidation and helps mitigate process-related risks such as thermal cracking, porosity, keyholing and Marangoni effects. 304L stainless steel (SS) feedstock is used to fabricate test specimens using the LFP system. Imaging techniques are used to examine the melt pool dimensions and layer bonding. In addition, the parts are evaluated for residual stresses, mechanical strength and grain size. Compared to CPW, SPW provides a more reliable heating/cooling relationship that is less dependent on part geometry. The overlapping spot welds distribute heat more evenly, minimizing the risk of elevated temperatures during the AM process. In addition, the resulting dense and uniform weld beads contribute to lower residual stresses in the printed part. To the best of the authors’ knowledge, this is the first study to thoroughly investigate SPW as a scanning strategy using the LFP process. In general, SPW presents a promising strategy for securing embedded sensors into LFP parts while minimizing residual stresses.

36 MATERIALS SCIENCE↗

The Case for and Against a Gadolinium Bias in SCALE: Round 2

The “Opening Arguments” for and against a gadolinium bias in SCALE were presented at the American Nuclear Society Annual Meeting in Philadelphia, Pennsylvania, in June, 2018. Some critical experiments included in the Oak Ridge National Laboratory Verified, Archived Library of Inputs and Data (VALID) indicate a significant bias as a function of gadolinium concentration. Other experiments indicate that no significant bias exists. The work presented here develops a larger suite of gadolinium-bearing benchmark models to further examine code, data, and benchmark performance. The new benchmark models have been reviewed for accuracy, but documentation and review for addition to the VALID library have not been completed. The problematic benchmarks included in VALID are HEU-SOL-THERM-014 and -016. These are two evaluations from a series of experiments from the Institute for Physics and Power Engineering (IPPE), Russia, documented in the International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook. The entire set of evaluations also includes HEU-SOL-THERM-015, -017, -018, -019, and -025. Each evaluation contains a different uranium concentration, and different configurations within each evaluation include different gadolinium concentrations. These 7 evaluations contain a total of 52 configurations and form the largest subset of experiments considered, and they allow for a more complete assessment of the performance of these benchmarks than has historically been possible using just the HEU-SOL-THERM-014 and -016 results. Additional solution experiments are considered, including MIX-SOL-THERM-006 and -007 and PU-SOL-THERM-034. MIX-SOL-THERM-007 is in the VALID library, whereas MIX-SOL-THERM-006 and PU-SOL-THERM-034 are not. The results for MIX-SOL THERM-007 have not shown a gadolinium trend. These mixed- and plutonium-fueled solutions include 28 configurations. Some experiments including solid fuel and solid gadolinium are also included. These experiments include highly enriched uranium (HEU) foils moderated with polyethylene in HEU-MET-THERM-010, -016, and -034, and low enriched uranium (LEU) pin arrays with gadolinia absorber rods in LEU-COMP THERM-036 and -043. A total 32 cases with solid fuel are included. The IPPE solution benchmarks show a fairly high degree of variability, but no clear trend as a function of gadolinium concentration can be observed. The mixed- and plutonium-fueled solutions show less variability than the HEU solutions and also no trend relative to gadolinium concentration. The solid-fueled experiments also show no trend as a function of gadolinium content. The entire set of benchmarks shows no clear trend on gadolinium content or the energy of the average neutron lethargy causing fission.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Unraveling the Mechanics: Computational Modeling of Residual Stresses in U10Mo Fuel with Aluminum Cladding

LEU (Low Enriched Uranium) plate-type fuel elements consist of a high-density, low-enrichment U–Mo alloy-based fuel foil encapsulated in an aluminum cladding and is fabricated through the Hot Isostatic Pressing (HIP) technique. Understanding the mechanism of possible failure modes of nuclear fuel is critical to mitigate potential consequences. One of the major contributing factors in various failure modes is stress and it greatly affects the integrity under temperature, pressure, and irradiation. These stresses could originate from various sources, including manufacturing, and operation, and can lead to deformation, cracking, or even complete failure of fuel elements. This study focuses on the development of a computational model that accurately predicts the residual stresses generated in the U10Mo fuel during fabrication. It has been observed that cladding creep has a substantial impact on the residual stresses in the U10Mo fuel post the HIP fabrication process. Furthermore, during the HIP bonding process the fuel plate system is heated to a temperature of 560 oC and as a result, the aluminum cladding transitions from (Al 6061-T6 to -O). This presents a challenge in capturing the change in material properties accurately. Therefore, a temperature dependent creep model such as hyperbolic sine creep model is considered to estimate the creep properties of the Aluminum cladding. The proposed calibrated creep model accurately predicts the residual stresses in the U10Mo fuel foil and agrees well with the experiments.

42 ENGINEERING↗

Purification of U from U-10Mo scrap generated during the fabrication of high performance research reactor fuel

A low enriched U-Mo alloy fuel is under development to replace highly enriched U fuels currently used in United States high performance research reactors. The alloy casting and fuel fabrication processes will generate scrap streams containing low enriched U (LEU) which must be recovered. Solvent extraction processes were designed using the Argonne Model for Universal Solvent Extraction (AMUSE) to purify solutions containing 20 and 50 g/L U. The feed for the solvent extraction processes was prepared from solutions generated from the dissolution of U-10Mo-Zr foils and U-10Mo-Zr-Al mini-plates. The U purification processes were demonstrated using two, 16-stage banks of miniature mixer-settlers. The solvent extraction experiments demonstrated that all design objectives for the U purification processes could be met. The U recovery in the product stream for each flowsheet was ≥99.9%. The flowsheet demonstrations also showed that the purity of the U Product will meet the requirements of the ASTM International C1462-21 specification for LEU metal enriched to less than 20% 235 U. In conclusion, the AMUSE modeling for both flowsheet demonstrations was validated by comparing predicted and measured concentrations of U, Mo, and Zr in the exit streams and stage samples at steady-state conditions in the mixer-settlers.

modified PUREX process↗

Depletion Benchmark of the AFIP-7 Experiment in the Advanced Test Reactor

Reactor physics depletion benchmarks for low-enriched uranium fuel are limited in number. In particular, there is very limited data for LEU benchmarks for U-10Mo (Uranium-10% Molybdenum) plate fuel developed for use in U.S. high-performance research reactors (USHPRR). USHPRR includes the Advanced Test Reactor (ATR), Advanced Test Reactor Critical Facility (ATR-C), High Flux Isotope Reactor (HFIR), University of Missouri Research Reactor (MURR), Massachusetts Institute of Technology Reactor (MITR), and National Bureau of Standards Reactor (NBSR) at the National Institute of Science and Technology. These reactors are fueled with high-enriched uranium dispersed fuel in a silicon/aluminum matrix. In support of conversion to a HALEU fuel, qualification of U-10Mo formed into a monolithic foil is being performed. Fuel qualification involves irradiated fueled specimens in the ATR. The irradiation tests provide an opportunity to benchmark depletion capabilities of reactor physics codes in support of the ATR operation, as well as develop benchmarks that can be used by other institutions to benchmark other reactor physics codes. This report documents the development of a benchmark model of the irradiation of the ATR Full -size plate In center flux trap Position 7 (AFIP-7) experiment.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Interfacial Analysis of Blister Formation in U-10Mo Mini-Plates

A thorough investigation of potential failure mechanisms builds confidence in the performance of monolithic U-10wt%Mo (U-10Mo) fuel plates. The lowenriched uranium (LEU) fuel system is currently undergoing qualification as a high U-density fuel that can be used to convert United States high-performance research reactors from high-enriched uranium (HEU) operation. This will require establishing fuel operational limits such that fission products and a coolable geometry are retained, even during off-normal reactor operation conditions [1]. Such off-normal conditions can subject the fuel plates to temperatures where the internal pressure of precipitated fission gasses result in a permanent deformed, raised area of the cladding, referred to as a blister. These blisters can reduce the local coolability of a fuel plate and can even close coolant channels of a fuel assembly, so blistered plates are considered failed regardless of whether the fuel is truly breached. Historically, a marginto- failure is established through out-of-pile blister threshold testing of irradiated fuel plates. This is accomplished by incrementally heating irradiated fuel plates until blisters are observed. This reveals the temperature threshold that would have resulted in a blister if a plate experienced them at those irradiation conditions [2]. While the blister testing itself reveals the temperatures at which the cladding mechanical integrity was exceeded, a more thorough investigation of the interface evolution in proximity to formed blisters may reveal mechanisms as to the blister formation and retention of fission gases. Previous studies have explored potential underlying mechanisms in historical plates that may have been close to blistering [3]; however, this work is the first exploration of blister tested irradiated plates, fabricated by a commercial vendor—another requirement for qualification of the fuel system [1]. The Mini-plate 1 (MP-1) experiment was the first in a series of irradiation and post-irradiation examination (PIE) campaigns to qualify the U-10Mo monolithic fuel system. It consisted of commercially fabricated 25.4×101.5 mm Al-clad mini-plates with a monolithic U-10Mo foil coated in a Zr diffusion barrier. The primary MP-1 PIE campaign was previously completed. Among the suit of examinations was a blister testing campaign, where plates were incrementally annealed in 25°C increments until blisters were observed or a maximum temperature of 550°C was reached [4]. The previously blistered plates from this campaign were revisited in this work.

25228↗