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At least 271 records · Page 15

Extension of OpenMC for Fixed Source Transmutation Calculations

This report documents work performed under a Strategic Partnership Project between Argonne National Laboratory (ANL) and the United Kingdom Atomic Energy Authority (UKAEA). The overall goal of this project is to extend OpenMC [1], a community-developed Monte Carlo particle transport code, to be able to perform fixed-source transmutation calculations. In fission and fusion reactors, the high flux of energetic neutrons causes materials within the reactor to “transmute,” or undergo a nuclear reaction that results in the addition/removal of neutrons and protons from the nucleus of an atom. If subjected to these reactions for long enough, the overall composition and physical properties of the material itself begin to change as a result of transmutation. Such a feature is vital for predicting the decrease in tritium production rate within a breeder blanket during the lifetime of a fusion reactor. OpenMC is capable of simulating neutron transport in fission/fusion systems, thereby allowing it to estimate the flux that causes transmutation. It is also capable of solving the transmutation equations, which determine how the composition of a material changes over time due to neutron irradiation and radioactive decay. However, solving the transmutation equations was previously only possible when the source of neutrons came from a fission system. In a fusion system, the source of neutrons is typically determined by a separate code and then given as an input to the particle transport simulation. This is known as a fixed source calculation. Through this project, we have extended OpenMC to solve the transmutation equations for a fixed source calculation. Evaluating the change in material compositions due to transmutation and its effect on physical properties is of key importance to a range of engineering analyses for fission and fusion systems. For example, in a fusion reactor, estimating the dose rate at different physical locations resulting from irradiated materials in the reactor allows designers to ensure that workers are not exposed to doses beyond applicable regulations. In order to properly dispose of irradiated materials, designers also need to estimate the radiotoxicity, which again relies on knowledge of the material composition at some future time. The specific tasks for this project that were agreed to between ANL and UKAEA were as follows: 1. Make changes and additions in the openmc.deplete and related modules in OpenMC to support transmutation calculations following a fixed source transport simulation. 2. Make necessary changes to OpenMC to model transmutation due to an arbitrary set of reactions needed for fusion applications. Use this new capability to generate a depletion chain file based on the TENDL nuclear data library. 3. Improve the openmc.deplete module in OpenMC to keep track of gases produced as a by-product of nuclear reactions during transmutation calculations. 4. Validate the new capabilities by carrying out fixed-source transmutation calculations on a suitable benchmark problem using OpenMC and a comparable Monte Carlo neutron transport code.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Discovering tungsten-based composites as plasma facing materials for future high-duty cycle nuclear fusion reactors

Abstract Despite of excellent thermal properties and high sputtering resistance, pure tungsten cannot fully satisfy the requirements for plasma facing materials in future high-duty cycle nuclear fusion reactions due to the coupled extreme environments, including the high thermal loads, plasma exposure, and radiation damage. Here, we demonstrated that tungsten-based composite materials fabricated using spark-plasma sintering (SPS) present promising solutions to these challenges. Through the examination of two model systems, i.e., tungsten-zirconium composite for producing porous tungsten near the surface and dispersoid-strengthened tungsten, we discussed both the strengths and limitations of the SPS-fabricated materials. Our findings point towards the need for future studies aimed at optimizing the SPS process to achieve desired microstructures and effective control of oxygen impurities in the tungsten-based composite materials.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Development of a compact fast-neutron spectrometer for nuclear emergency response applications

We have developed a Compact Fast Neutron Spectrometer (CFNS) for passive assay of special nuclear material (SNM) through the observation of fast neutrons. The CFNS consists of eight organic glass scintillators (OGS) coupled to silicon photomultipliers and a waveform digitizer, which are integrated within a human-portable box. The CFNS determines the neutron energy profile by spectrum unfolding using the Maximum-Likelihood Expectation Maximization method. The detector acquisition system was optimized to have a dynamic range of up to 10 MeV neutron energy. Bulk special nuclear material (SNM) measurements from the National Criticality Experiments Research Center were analyzed for SNM validation/examination. Additionally, the results show that the CFNS can be used to distinguish between fission and (α, n) neutron emitters, regardless of intervening material type (Cu and polyethylene) and thickness, by taking the ratio of neutron counts at different regions in the unfolded energy spectrum. Additionally, by fitting an exponential curve to the unfolded energy spectrum of PuO 2 and Pu neutron emitters, the CFNS showed the ability of distinguishing between pure Pu oxide, pure Pu metal and mixed oxide-metal configurations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Microstructure and fracture toughness characterization of three 9Cr ODS EUROFER steels with different thermo-mechanical treatments

Ferritic martensitic ODS steels are one of the candidate structural materials for future Gen-IV nuclear fission and fusion reactors. Here, the dependence of fracture toughness on microstructure was investigated by comparing three 9Cr ODS EUROFER steels manufactured through different thermo-mechanical processing routes. Quasi-static fracture toughness testing was performed with sub-sized C(T) specimens and microstructural characterization was carried out using scanning electron microscopy, electron backscatter diffraction, and transmission electron microscopy. It was found that at lower test temperatures (-100 – 22 °C), the fracture toughness was primarily controlled by crack initiation at sub-micron particles and by production of secondary cracks during fracture. At higher temperatures (above 100 °C), fracture toughness was predominantly controlled by the matrix ductility and the grain boundary strength with a relatively ductile coarse-grained alloy demonstrating higher fracture toughness compared to high-strength fine-grained alloys. These results and discussion show that variations in thermomechanical treatments can produce significant differences in microstructure and fracture toughness behavior of ferritic martensitic ODS steels.

36 MATERIALS SCIENCE↗

Gamma-ray spectrometry analysis methods for radioisotope dissolution and mixing for nuclear forensics applications

We report the production of surrogate nuclear explosive debris involves the dissolution of irradiated fissile material, elemental isolation, and recombination based on required fission product ratios. Gamma-ray spectrometry is used following each step to assess the radioactive fission product inventory. A high-purity germanium detector is used to measure each sample, and the detector efficiencies are determined prior to sample measurements. Through radiochemical techniques, elements are isolated and recombined into samples with specific fission product ratios. As a result, a matrix-based approach can account for imperfect chemical separations to calculate the proper mixture volumes to obtain intended volatile-to-refractory fission product ratios, or R-values.

07 ISOTOPE AND RADIATION SOURCES↗

Computational Materials Design for Ceramic Nuclear Waste Forms Using Machine Learning, First-Principles Calculations, and Kinetics Rate Theory

Ceramic waste forms are designed to immobilize radionuclides for permanent disposal in geological repositories. One of the principal criteria for the effective incorporation of waste elements is their compatibility with the host material. In terms of performance under environmental conditions, the resistance of the waste forms to degradation over long periods of time is a critical concern when they are exposed to natural environments. Due to their unique crystallographic features and behavior in nature environment as exemplified by their natural analogues, ceramic waste forms are capable of incorporating problematic nuclear waste elements while showing promising chemical durability in aqueous environments. Recent studies of apatite- and hollandite-structured waste forms demonstrated an approach that can predict the compositions of ceramic waste forms and their long-term dissolution rate by a combination of computational techniques including machine learning, first-principles thermodynamics calculations, and modeling using kinetic rate equations based on critical laboratory experiments. By integrating the predictions of elemental incorporation and degradation kinetics in a holistic framework, the approach could be promising for the design of advanced ceramic waste forms with optimized incorporation capacity and environmental degradation performance. Such an approach could provide a path for accelerated ceramic waste form development and performance prediction for problematic nuclear waste elements.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Neutron calorimeter development at fission and fusion pulsed neutron sources

A neutron calorimeter fielded in pulsed neutron irradiation experiments at the National Ignition Facility (NIF) and White Sands Missile Range Fast Burst Reactor (WSMR FBR) is described, and results are provided and discussed. The calorimeter is modular in design to allow fielding of various neutron absorber materials and thicknesses, as well as use at both fission and fusion sources, all of which has been done. Neutron calorimeters designed for fission sources have been fielded at fusion sources as well, but these instances are not documented in available literature—making this work novel. The functional calorimeter consists of a neutron absorber and two sheathed, grounded thermocouples secured within a subassembly made of thermally insulating materials. This subassembly is placed into a sealed vessel for material and facility safety considerations. The device was fielded at NIF in four polar-direct-drive exploding pusher shots and eleven WSMR FBR pulses. Calorimeter data from NIF experiments show a discernable thermal response accredited to neutron heating within the first 10 s, but the data are dominated by noise from ambient X-ray heating after time = 10 s post-pulse. This response is highly consistent between shots and linearly related to incident neutron fluence and neutron absorber thickness. A temperature rise of 1.1E-2 K/(10 13 neutrons/cm 2 ) per millimeter of absorber thickness was determined for both 0.4 mm and 1 mm thick depleted uranium absorbers with linear best fit R 2 of 0.97 and 0.98 for each thickness and y-axis offsets of 8.8E-3 and 1.3E-2, respectively. WSMR FBR experiment data show a temperature rise of 6.2E-2 K/(10 13 neutrons/cm 2 ) with linear best fit R 2 of 0.14 and y-axis offset of 7.6E-3 for a calorimeter with a 1 mm thick enriched boron carbide ( 10 B 4 C) absorber, though it must be noted that device-to-device variability is significant at both facilities. So these data are also affected by noise on a similar timescale as at NIF, though the noise is significantly lesser in magnitude but oscillatory.

42 ENGINEERING↗

Source term analysis of FeCrAl accident tolerant fuel using MELCOR

It has been established that incremental improvements in beyond design basis accident performance can be achieved through accident tolerant fuel (ATF). However, they have the potential to recover margin with respect to conventional fuel and therefore enhance plant economics through uprate or cycle length increase. To realize this potential, it is necessary to quantify the reduction in source term due to use of ATF, and correspondingly how this is affected by increasing the cycle length and/or burnup. This requires development of a risk informed analysis methodology for ATF under high burnup conditions, which is being developed within LWRS. To this end, a MELCOR simulation of FeCrAl ATF in a recovered Large Break LOCA (LBLOCA) scenario has been developed, using a model based on the Zion Pressurized Water Reactor (PWR). The new user defined material capability, along with the inclusion of detailed neutronics- and depletion-derived parameters such as core power distribution, decay heat behavior, and fission product inventories, allows a more detailed simulation of FeCrAl clad material properties and behavior than has previously been possible using MELCOR. These detailed FeCrAl results were compared with a zircaloy clad model to investigate the differences between the two clad types and quantify the benefits of FeCrAl ATF with an 18-month cycle. Next, the fuel cycle with ATF was extended to 24 months, to determine whether any additional safety margin provided by FeCrAl ATF could be leveraged to implement high burnup FeCrAl-clad fuel while retaining the same operating and safety limits as current zircaloy-clad fuel. For the particular scenario analyzed, the delay to fuel failure from using ATF was of the same order as the LOCA recovery time, and hence significant in reducing fission product release, with the 24-month FeCrAl core performing better than the 18-month zircaloy core. It is noted that for other transients, the reduction in release due to using FeCrAl may be less significant. Furthermore, the material model developed here can be used in such further studies in support of determining the overall source term.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Measuring thermal diffusivity and gap conductance in uranium nitride and Zircaloy relevant for microreactor applications

Heat transfer across nuclear fuels and structural interfaces is an important factor for evaluating the performance of nuclear power systems. Specifically, heat generated as nuclear fuel fissions must be transported through the cladding material and through the reactor to reach the steam turbine for power generation. As new microreactor designs emerge, maximizing the efficiency of this heat transfer process becomes crucial to make them commercially viable. This article examines thermal diffusivity and gap conductance in uranium nitride (UN) fuel and Zircaloy-4 (Zry4) cladding using light flash analysis (LFA). Thermal diffusivity measurements were made on monolithic UN pellets and Zry4 exposed to carbon at peak operating temperatures of microreactors and show that carbon ingress has a minimal effect on thermal diffusivity when compared with identical materials not exposed to carbon. Evaluation of gap conductance at the UN-Zry4 interface was done using one-dimensional two-layer thermal transport models as a function of applied pressure. Here the results show that increasing pressure on the UN-Zry4 interface leads to gains in gap conductance per unit area in fuel-cladding assemblies at microreactor operating temperatures. While many other variables are expected to influence UN-Zry4 interfacial gap conductance (e.g. contact surface roughness, porosity, localized heating, environmental gas pressure), the work offers a demonstration of using a conventional LFA apparatus to determine this parameter at elevated temperatures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Elucidating the Transition of 3D Morphological Evolution of Binary Alloys in Molten Salts with Metal Ion Additives

Molten salts serve as effective high-temperature heat transfer fluids and thermal storage media used in a wide range of energy generation and storage facilities, including concentrated solar power plants, molten salt reactors and high-temperature batteries. However, at the salt–metal interfaces, a complex interplay of charge-transfer reactions involving various metal ions, generated either as fission products or through corrosion of structural materials, takes place. Simultaneously, there is a mass transport of ions or atoms within the molten salt and the parent alloys. The precise physical and chemical mechanisms leading to the diverse morphological changes in these materials remain unclear. Here, to address this knowledge gap, this work employed a combination of synchrotron X-ray nanotomography and electron microscopy to study the morphological and chemical evolution of Ni-20Cr in molten KCl-MgCl 2 , while considering the influence of metal ions (Ni 2+ , Ce 3+ , and Eu 3+ ) and variations in salt composition. Our research suggests that the interplay between interfacial diffusivity and reactivity determines the morphological evolution. The summary of the associated mass transport and reaction processes presented in this work is a step forward toward achieving a fundamental comprehension of the interactions between molten salts and alloys. Overall, the findings offer valuable insights for predicting the diverse chemical and structural alterations experienced by alloys in molten salt environments, thus aiding in the development of protective strategies for future applications involving molten salts.

36 - MATERIALS SCIENCE↗

Sodium-Cooled Fast Reactor Reference Plant Model

This report details the progress of Idaho National Laboratory (INL) in creating a reference plant multiphysics model for the Advanced Burner Test Reactor (ABTR). This model was developed under Task 13 of the U.S. Nuclear Regulatory Commission project “Development and Modeling Support for Advanced Non-Light Water Reactors,” and is an extension of the reference plant model developed in Task 4b, which was improved upon in the following ways. (1) The discrete ordinates method was used in lieu of the super-homogenization (SPH)-corrected diffusion approximation in order to better capture the anisotropic scattering contribution and the neutron leakage change due to thermal expansion. (2) The novel neutronic spatial discretization approach, termed the ring-heterogeneous (RH) approximation, was conceptualized and introduced to capture the differential expansion of the materials in the core. This new technique proved capable of preserving fission rates and maintaining the eigenvalue within 2.5% and 266 pcm with 9 neutron energy groups, respectively. Separating the different materials in the core enables the differential expansion of materials to be explicitly accounted for, eliminating the need for problem-specific cross-section functionalization techniques. (3) The SAM model for the core and system thermal-hydraulics analysis was updated to include 61 channels instead of just four representative ones. This enables users to obtain improved spatial resolution for sodium temperature and density scalar fields. (4) All the mesh files were created via the Multiphysics Object-Oriented Simulation Environment (MOOSE) Reactor module, eliminating all reliance on external tools for mesh creation. (5) Finally, the fuel axial expansion now leverages the HT9 and UPuZr material properties that have been validated against experimental data. The reference plant model was used to perform a full-core unprotected loss of flow (ULOF) transient calculation, including neutronics, thermal and mechanical feedback mechanisms. Future work will be devoted to further enhancements of the model. Potential improvements to the model include the addition of the control rod driveline expansion feedback and the upgrading of the support plate model so as to explicitly include 3D effects. Additionally, a Nuclear Energy Advanced Modeling and Simulation funded parallel effort has completely automated the creation of the ring-heterogeneous (RH) mesh from the fully heterogeneous (FH) geometry, thus maximizing user friendliness for the sodium fast reactor sodium-cooled fast reactor (SFR) workflow and will be incorporated in future work.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Data reduction in deterministic neutron transport calculations using machine learning

Neutron cross section matrices for fission and scattering data are required for each material, temperature, and enrichment level to calculate the neutron transport equation accurately. Here, this information can be a limiting factor when using the multigroup discrete ordinates (S N ) method when the number of energy groups is large. Machine Learning (ML) can be used to replace the need for the cross section matrices by reproducing the function that maps the scalar flux to the scattering and fission sources. Through the use of autoencoders and Deep Jointly-Informed Neural Networks (DJINN), the data storage requirements are reduced by 94% of the original data for a 618 group problem. This is accomplished while preserving the scalar flux, maintaining generality, and decreasing wall clock times.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurements of emanation of Ar-37 and Ar-39 from irradiated rocks and powders

The emanation fraction of radionuclides has been highlighted as a known source of uncertainty in the estimation of radionuclide source signatures from underground nuclear tests and other nuclear activities, particularly in the case of activation products. A system was developed at Pacific Northwest National Laboratory to quantify the emanation fraction of argon from samples ranging in particle size from powder to small rocks. Seven materials, two powders and five rock types, were irradiated with fission spectrum neutrons and the emanation fraction of 37 Ar was measured. Additional measurements were made of the 39 Ar emanation for four of these materials.

36 MATERIALS SCIENCE↗

Radial Deconsolidation and Leach-Burn-Leach of Eight As-Irradiated AGR-3/4 TRISO Fuel Compacts

Eight as-irradiated AGR-3/4 fuel compacts were subjected to destructive post-irradiation examination via radial-deconsolidation-leach-burn-leach (RDLBL) at INL. The RDLBL process deconsolidated the compacts in multiple, radial steps, followed by a final, single-step axial deconsolidation. The samples generated at each step were analyzed for isotopes of key fission products and actinides. After each deconsolidation step, the compact volume was assessed, and this was used to normalize the measured quantity of nuclides of interest to give a volumetric concentration as a function of radial position within the compact. The total inventories of measured fission products and actinides and the radial concentration profiles were compared among the eight compacts deconsolidated at INL and four other as-irradiated compacts examined at ORNL. The results were analyzed for the effects of irradiation temperature. These results will be used for comparisons with fission product transport models and as input from which fission product diffusivities can be calculated.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fusion Neutron Generator

The proposed code, named FROG (Fusion neutron Generator) is built upon the open-source particle transport Monte Carlo toolkit Geant4. Geant4 provides C++ classes that can be leveraged to build application-specific codes dealing with the transport of particles through matter. Geant4-based codes are applied in high-energy particle physics experiments, medical applications, shielding, and space applications for example. The FROG code allows the user to define the geometry of a neutron converter device shaped as a hollow cylinder, where a neutron breeding material such as lithium deuteride (LiD) is cladded by two concentric cylinders. Such neutron converter is then placed inside a regular nuclear fission reactor, where thermal neutrons will react with the neutron breeder material (typically, Lithium 6), and through a series of reactions, will generate high-energy neutrons – neutrons whose kinetic energy are around 14 MeV. The hollowed central portion can hold a specimen that will be bombarded by high-energy neutrons created inside the neutron breeding material. Figuratively speaking, this type of device transforms neutrons from thermal (~0.625 eV) to fusion (~14 MeV) energies and is sometimes termed “fusion-to-thermal neutron converters” in the literature. The code consists of C++ source file compiled and linked to generate an executable. The user can select the dimensions of the converter (radius, length, and thickness of the breeder material), the breeder material type, the cladding material, and the specimen material that will be activated or irradiated. As input, the neutron flux for a specific location inside a reactor, for instance, positions in ATR, is required. As output, the code predicts the number of high-energy neutrons produced, the total neutron flux and fluence as well as its detailed spectrum. The physics involved in such device is very complex, as it requires modeling neutron transport, light-ion (tritons) transport, as well as fusion reactions. The Geant4 toolkit provides the required physical models.

Martin, NicholasP. [Idaho National Laboratory (INL↗

Development of an In Situ Fission Gas Release Instrument for Fuel Sample Irradiations in the High Flux Isotope Reactor

Experimental measurement of gaseous fission product release with respect to temperature and burnup is a critical aspect of understanding nuclear fuel performance, validating predictive models, and qualifying new fuels. To measure this phenomenon in real-time, Oak Ridge National Laboratory has developed an instrument for measuring in situ fission gas release from small-scale fuel samples irradiated in the High Flux Isotope Reactor (HFIR). The instrument uses a continuous flow of Heover the fuel samples to sweep gaseous fission products from a sealed capsule in the HFIR Be reflector to an instrument station adjacent to the reactor. The instrument station houses two high-purity germanium (HPGe) detectors that measure decay gamma rays from fission products passing through a room temperature dwell chamber placed over the detector crystal. The sealed capsules in the reactor are designed to modulate fuel sample temperatures between 700 and 1,100°C by changing the Ar/He gas mixture surrounding the capsules during irradiation. N-type thermocouples are incorporated into the capsule housing to record real-time fuel temperatures. The capsules are heated primarily by prompt gamma rays emitted from the HFIR core with minimal heat contributions from fission in the fuel samples to minimize temperature gradients in the specimens for separate-effects characterization of the material. This paper describes modeling of time-dependent nuclear heating and fission product formation in fuel samples, thermal characteristics of the in-core capsules, and expected gaseous fission product gamma spectra at the HPGe instrument station.

Mulligan, Padhraic L [ORNL] (ORCID:000000025826540↗

Phase-field simulations of intergranular fission gas bubble behavior in U 3 Si 2 nuclear fuel

U 3 Si 2 is a potential accident-tolerant fuel that shows promise due to its high thermal conductivity and higher uranium density relative to UO 2 . However, its swelling and fission gas release behavior in light water reactor (LWR) conditions is relatively unknown. To provide mechanistic insight and determine parameters for engineering-scale fuel performance modeling of pellet-form U 3 Si 2 , phase-field simulations of the growth, interconnection, and venting of intergranular fission gas bubbles were performed. The fractional coverage of the grain boundary and the fraction of bubble area that is vented were calculated as a function of time. From the simulation data, the fractional grain boundary coverage at saturation, an important parameter needed in engineering-scale modeling of swelling and fission gas release, was determined. Multiple simulations were run to determine the uncertainty in the calculated value. Finally, the effect of model assumptions and input parameters that are not well known was evaluated. Simulation results are compared to related theoretical and computational work. Based on the simulation results, a value of 0.60 for the fractional grain boundary coverage at saturation is recommended for U 3 Si 2 fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High-fidelity photoneutron detection via neutron activation analysis

To interdict illicit radioactive sources and prevent nuclear terror, governments have deployed portal monitor systems at ports of entry. Such portal monitors rely upon the detection of spontaneously-emitted radiation signatures, however, detection scenarios become more challenging for highly enriched uranium, which emits relatively few spontaneous radiation signatures. Photon active interrogation techniques can augment current cargo inspection scenarios and improve detection capabilities for illicit nuclear material. A high-energy photon interrogation source can induce photofission in nuclear material, producing strong radiation signatures for detection. Prompt fission signals are of specific interest because prompt neutrons are greater than 99% of the fission signal. When using detectors capable of spectroscopy, e.g., pulse shape discrimination-capable organic scintillators, the intense interrogating source often will cause pulse pile-up, degrading particle classification. In this work, we demonstrate photoneutron detection via neutron activation of aluminum and iron. The experiments rely upon nuclear reactions that can only be induced by neutrons, and are robust against pile-up, thereby providing high-confidence neutron rates. In this work, we apply neutron activation analysis for the detection of high-energy neutrons produced by high-energy photon irradiation; the depleted uranium sample was irradiated with a 9-MeV bremsstrahlung beam. We find that the irradiated depleted uranium produced an aluminum activation flux of 1.77 × 10 5 n cm –2 s –1 and an iron-56 activation flux of 1.05 × 10 5 n cm –2 s –1 . Furthermore, the ability to detect radioactivity induced by neutrons created in (, n) and photofission reactions demonstrates a new approach for photon active interrogation to identify nuclear materials.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗