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DOE OSTI2023

Modeling, analysis, and optimization of complex nuclear processes and facilities via computational methods: The HALEU process case study

Improving and adapting industrial systems to timely meet changing programmatic and market demands is an important goal to achieve, including when operating and maintaining complex nuclear processes and facilities. However, changes to these complex systems are costly, particularly when they are already in place and bounded to stringent requirements and constraints such as when handling radioactive material and contaminated equipment. These conditions often exist when treating spent nuclear fuel remotely within shielded nuclear radiation chambers, commonly referred as hot cells, to condition nuclear material and/or fabricate products for utilization in other nuclear enterprises such as in the manufacture of advanced nuclear fuel. The illustrative case considered here is the production of high assay low enriched uranium (HALEU) products supporting the deployment of advanced nuclear reactors. For the HALEU program, resources invested were and are being systematically analyzed so that these investments are maximized in a facility that is nearly 60 years old. A methodology that has effectively enabled optimized and improvements in the Spent Fuel Treatment (SFT) program, and consequently the HALEU program, involves discrete event simulation as addressed in this article. Here, the quantification of multiple productivity metrics, including material processing rates, cycle times, bottlenecks, number of material transfers as well as equipment, workstation, and material handling utilization, has resulted in a myriad of diverse discoveries and data-informed decisions regarding process layout and constituent, labor levels and schedules, selection of new process units, storage needs, and other critical process configurations. This article describes such a computational capability being applied for decision-making, illustrates its application to an actual process and program, provides illustrative results, and argues how computational methods for the modeling, analysis, and optimization of complex processes and facilities does lead to informed decisions derived from data and not only from intuition.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2025

Modeling a Thermal-Spectrum LEU-fueled Molten Salt Reactor Co-fueled with Thorium in SCALE 6.3.1 and Serpent-2

Interest in the development of advanced nuclear fission reactors for commercial electricity production has risen in recent years, with Generation IV reactor designs offering numerous advantages in safety, efficiency, fuel cycle sustainability, and waste management. In particular, thorium-fueled molten salt reactors (MSRs) are considerably promising for enhancing fuel cycle sustainability in their ability to breed fissile 233U fuel from thorium, a presently untapped and widely abundant resource. A novel MSR fuel cycle concept, the ”Sourdough” refueling and waste management strategy, has previously been demonstrated with a traditional uranium-based fuel cycle in a thermal-spectrum MSR operating with low enriched uranium (LEU) fuel with favorable neutronic performance. However, the ability to use this unique fuel cycle approach with thorium-based molten salt fuels has not yet been studied. In this work, the Sourdough fuel cycle was implemented in a small, thermal-spectrum MSR fueled with high assay low enriched uranium (HALEU) and fertile 232Th for breeding 233U fuel. Relevant neutronic data, including fuel and isothermal temperature feedback behavior, was studied using the SCALE 6.3.1 and Serpent-2 code systems, and keff data was measured during simulated depletion at 400 MWth. The Sourdough fuel cycle concept is shown to perform favorably with a thorium-fueled MSR model, thus warranting further study into its use in other MSR designs.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Two Delayed Critical 7-Inch-Diameter Interacting Enriched (93.14) Uranium Metal Cylinders without Moderator and Reflector

This report documents very accurately the configuration and the materials for experiments with two unmoderated, unreflected, interacting, coaxial, highly enriched, 7-in.-diameter, uranium metal cylinders performed at the Oak Ridge Critical Experiments Facility (ORCEF) in April 1963 and described in logbook E-19 associated with experiments in the East cell of ORCEF. The information is sufficiently accurate that it can be used as the basis for preparation of benchmarks for International Criticality Safety Benchmark Program (ICSBEP) at Idaho National laboratory. The thickness of the cylinders was varied and the spacing between them was adjusted to achieve a delayed critical configuration. The average enrichment of the uranium metal was 94.15 wt. % 235 U. The heights of the 7-in.-diameter, equal-height cylinders varied from 2 5/8 to 3 1/4 inches. All interacting cylinders were assembled coaxially with their flat faces parallel and their combined masses varied between 62 and 76 kilograms of HEU metal. The data from these six experiments described are judged to be acceptable for use as criticality safety benchmark experiments for the ICSBEP and EURATOM’s Nuclear Energy Agency nuclear criticality safety benchmark program, once the uncertainty analysis is completed. Based on previous ICSBEP benchmarks with this enriched uranium metal at ORCEF, it is expected that the uncertainties in k eff could be as low as ± 0.0002.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2020

Two Delayed Critical 15-Inch-Diameter Interacting Enriched (93.14) Uranium Metal Cylinders without Moderator and Reflector

This report documents very accurately the configuration and the materials for experiments with two unmoderated, unreflected, interacting, coaxial, highly enriched, 15-in.-diameter, uranium metal cylinders performed at the Oak Ridge Critical Experiments Facility (ORCEF) in May to Aug 1963 and described in logbook E-19 and E -20 associated with experiments in the East cell of ORCEF. Measurements were also performed in April and May of 1965 and described in logbooks E-22 and E-23 The information is sufficiently accurate that it can be used as the basis for preparation of benchmarks for International Criticality Safety Benchmark Program (ICSBEP) at Idaho National laboratory. The thickness of the cylinders was varied and the spacing between them was adjusted to achieve a delayed critical configuration. The average enrichment of the uranium metal was 94.14 wt. % 235 U. The heights of the 15-in.-diameter, equal-height cylinders varied from 1-5/8 to 3.0-inches. All interacting cylinders were assembled coaxially with their flat faces parallel and their combined masses varied between 182 and 325 kilograms of HEU metal. The data from these 12 experiments described would be acceptable for use as criticality safety benchmark experiments for the ICSBEP and EURATOM’s Nuclear Energy Agency nuclear criticality safety benchmark program, once the uncertainty analysis is completed. Based on previous ICSBEP benchmarks with this enriched uranium metal at ORCEF, it is expected that the uncertainties in k eff could be as low as ± 0.0002.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Three Delayed Critical 15-Inch-Diameter Interacting Enriched (93.14) Uranium Metal Cylinders Without Moderator and Reflector

This report documents very accurately the configuration and the materials for experiments with three unmoderated, unreflected, interacting, coaxial, highly enriched, 15-in.-diameter, uranium metal cylinders performed at the Oak Ridge Critical Experiments Facility (ORCEF) in August and September 1963 and described in logbook E 20 associated with experiments in the East cell of ORCEF. The information is sufficiently accurate that it can be used as the basis for preparation of benchmarks for International Criticality Safety Benchmark Program (ICSBEP) at Idaho National laboratory. The thickness of the cylinders was varied and the spacing between them was adjusted to achieve a delayed critical configuration. The average enrichment of the uranium metal was 94.14 wt. % 235U. The heights of the 15-in.-diameter, equal-height cylinders varied from 1-1/8to 2.00 inches. All interacting cylinders were assembled coaxially with their flat faces parallel and their combined masses varied between 182 and 325 kilograms of HEU metal. The data from these six experiments described are judged to be acceptable for use as criticality safety benchmark experiments for the ICSBEP and EURATOM’s Nuclear Energy Agency nuclear criticality safety benchmark program, once the uncertainty analysis is completed. Based on previous ICSBEP benchmarks with this enriched uranium metal at ORCEF, it is expected that the uncertainties in measured keff could be as low as ± 0.0002.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Extraction of Neptunium, Plutonium, Americium, Zirconium, and Technetium by Di-(2-Ethylhexyl)- Iso -Butyramide (DEH i BA) at High Metal Loadings

Increased focus on carbon neutral energy has generated a resurgence of interest in nuclear power, and in particular advanced reactors which are likely to utilize high assay low enriched uranium (HALEU). This in turn could increase the economic attractiveness of recovering still partially enriched uranium from used nuclear fuel. Concomitant to development of advanced reactors, advanced reprocessing schemes should be developed which address the disadvantages to well established reprocessing schemes. The present study focuses on using di-(2-ethylhexyl)-iso-butyramide (DEHiBA) under high metal loading conditions for the reprocessing of used nuclear fuel. The elements examined in the study include the dominant transuranic actinides (Np, Pu, Am) as well as the often-problematic Tc and Zr. Further, by increasing the concentration of the extractant from the more commonly reported 1.0 M – 1.5 M, the extraction of hexavalent actinides is substantially increased, while maintaining effective rejection of tri, tetra, and pentavalent actinides, particularly in the presence of high loadings of uranium. In conclusion, the extraction of Zr by 1.5 M DEHiBA is noted to be negligible by comparison to tributyl phosphate (TBP), however the coextraction of Tc with U is observed to be nominally twice the quantity that is extracted by TBP indicating a need for effective Tc management.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

FAST Irradiations, Postirradiation Examinations, and Modeling of U-Mo for Light Water Reactor Applications

Many next generation light water reactor (LWR) concepts, such as mobile small modular reactors, are seeking to use smaller core dimensions than conventional reactor types. Smaller reactor cores require an increase in fissile material to maintain reactivity. For non-proliferation purposes, enrichment increases are limited to less than 20% (high assay low enriched uranium, [HALEU]) and so higher uranium density fuels than UO 2 must be considered. To this end, uranium-molybdenum alloys were tested using the Fission Accelerated Steady-state Test (FAST) approach. The experiment test matrix is focused on identifying the temperature transition between low swelling and high fission gas retention to break away swelling and low fission gas retention. This paper documents the results of irradiation tests and post-irradiation examinations (PIE) including neutron radiography, rodlet profilometry, fission gas collection analysis, and optical metallography. The results of these tests showed that unconstrained U-Mo fuels (solid, Na-bonded rodlets) have a swelling threshold between 400-450°C with minimal fission gas release below this point. Higher temperature solid fuel showed microstructural zoning with small pore networks while lower temperature solid fuels have a uniform microstructure with large pore networks. U-Annular Mo fuels where swelling had some self-constraint imposed upon it, were shown to have much reduced swelling compared to their solid counterparts as well as very low fission gas release for irradiation temperatures up to 500°C. These initial results show that the use of U-Mo in constrained fuel geometries could be used as a high uranium density HALEU fuel for LWRs.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

A Robust Processing Approach for Producing Highly Loaded Dispersion Fuels

A robust fabrication method, resulting in higher yields, to produce highly loaded U3Si2-Al dispersion fuels for converting research reactors from a high enriched to a low enriched uranium fuel needs to be developed. To reliably produce a highly loaded dispersion fuel, process changes need to be implemented where the traditional approach has experienced challenges and poor yields. The present work describes the key changes needed. Parts of the work were done with uranium silicide and parts were completed with a representative silicide surrogate. The major deviations from traditional fabrication methods are associated with a refinement in particle size distribution, method for compacting to achieve complex shapes, and welding of the aluminum picture frame used to encapsulate the fuel compact. Methods for rolling and arc melting are also discussed. By using the methods described within, fabricating a highly loaded dispersion fuel that can meet stringent fuel homogeneity and geometry requirements at higher yields and lower costs may be possible.

U3Si2, HFIR, dispersion fuel, Uranium, Research Re↗

NASA NTRSDate not supplied

Centrifugal Nuclear Thermal Rocket Challenges and Potential

The Centrifugal Nuclear Thermal Rocket (CNTR) is a liquid fueled fission propulsion concept designed to heat propellant to 5000 K prior to expansion through a nozzle. A specific impulse up to 1800 s may be achieved using hydrogen propellant, and a specific impulse up to 1000 s may be achieved using more storable propellants such as methane, ammonia, or propane. The high uranium density of the liquid metallic uranium or liquid uranium carbide fuel will help enable compact engines suitable for missions such as fast (<15 month) round trip human Mars missions or high delta-V missions in cislunar space. Long term applications of the CNTR could include the advanced exploration and utilization of the solar system through direct use of in-situ volatiles as propellant. Challenges associated with the CNTR are numerous. Centrifugal force is used to retain the liquid fuel in rotating fuel cylinders, and rotational velocities up to 5000 rpm may be required. Propellant flow must be directed such that all structures and moderators in the core are adequately cooled prior to the propellant entering the liquid fuel and being heated to 5000 K. The rotating fuel cylinder wall (RFCW) must have an inner surface designed to be compatible with liquid uranium metal or uranium carbide fuel up to at least 1500 K, and that inner surface may also need to be textured to help maintain acceptable wall temperatures. Propellant must flow radially inward through the RFCW while fuel is simultaneously contained. The RFCW should ideal-ly be made from a material with low neutron absorption to help minimize engine mass and facilitate the use of High Assay Low Enriched Uranium (HALEU) fuel in the system. The drive system for the rotating fuel cylinders must support all phases of operation. This paper will discuss computational and experimental research being conducted to address some of the challenges associated with the CNTR, and will also note potential mission benefits from the CNTR.

Michael G. Houts↗

NASA NTRSDate not supplied

Strategy for Developing Technologies for Megawatt-class Nuclear Electric Propulsion Systems

In late fiscal year 2020, the Space Nuclear Propulsion (SNP) project began the process of formulating an investment strategy to support development of the technologies required for a high-power (megawatt-class) nuclear electric propulsion (NEP) system capable of performing human-scale missions. This activity was initiated concurrent with several high-level studies and assessments were either under way or had just concluded. Studies of human-scale Mars missions have been performed several times over the past two decades. One of the most recent studies examined opposition-class human Mars missions to occur in the late 2030s timeframe [1,2]. The mission architecture assumed a hybrid NEP/chem-propelled vehicle that used a high specific impulse (Isp) NEP-system and a liquid oxygen (LOx)-liquid methane high thrust chemical stage (two 110 kN (25 klbf) thrust, 365 s Isp engines) for maneuvers performed to enter and exit gravity wells. Trajectory analyses performed in this study showed that such a mission could be performed with 2-4 MWe directed into the electric propulsion system (operating for 20,000+ hours), with the large range representing different opposition-class Mars mission opportunities and permutations on the trajectory design, concept of operations, and technology choices. In 2020, the NASA Engineering and Safety Center (NESC) performed a study to evaluate the maturity of the different technologies required for nuclear propulsion systems [3]. The executive summary of this report provided the following top-level conclusions: • “The majority of critical technologies for… NEP/Chem… systems are relatively immature” • “TRLs [technology readiness levels] in the literature are often overestimated” • “The majority of critical technologies… for NEP/Chem… systems are at a relatively high level of advancement degree of difficulty (AD2 > 4) for maturation, requiring a dual development approach” • “The proper assessment of baseline TRL and AD2 values and the estimation of requirements and resources required for advancement have been consistent issues for NEP,” • “Non-advocate reviews should occur at the start of a technology program and at all key milestones.” In 2021, the National Academies of Science, Engineering, and Medicine (NASEM) issued a separate report [4] identifying the “primary technical and programmatic challenges, merits, and risks for maturing space nuclear propulsion technologies of interest to a future human Mars exploration mission.” That work contained several important findings, including: • “Developing a MWe-class NEP system for the baseline mission would require increasing power by orders of magnitude relative to NEP system flight- or ground-based technology demonstrations completed to date.” • “Subscale in-space flight testing of NEP systems cannot address many of the risks and potential failure modes associated with the baseline mission NEP system. With sufficient M&S [modeling & simulation] and ground testing, including modular subsystem tests at full scale and power, flight qualification requirements can be met by the cargo missions that will precede the first crewed mission to Mars. Fully integrated ground testing may not be required.” • “As a result of low and intermittent investment over the past several decades, it is unclear if even an aggressive program would be able to develop an NEP system capable of executing the baseline mission in 2039.” These efforts motivated the SNP project to investigate the technologies available for a megawatt-class high power nuclear electric propulsion system. That system is illustrated schematically in Figure 1 and is comprised of five separate top-level critical technology elements (CTEs). 1. Nuclear Reactor – Thermal power source for the system, utilizing high-assay low enriched uranium (HALEU) as the nuclear fuel. Reactor radiation shielding is also included in this CTE. 2. Power Conversion – Operates as a thermodynamic cycle, accepting nuclear reactor thermal power as an input and converting it to mechanical power. 3. Power Management and Distribution (PMAD) – Accepts as an input mechanical power from the power conversion system, which is used to generate electrical power. The PMAD system also distributes the generated electrical power to all other parts of the spacecraft, including the high-power EP system. The PMAD system may also perform duties such as isolation, fault detection, and power transformation/rectification for different spacecraft systems, including the thrusters. 4. Electric Propulsion (EP) – Accepts as an input electrical power, which is used to accelerate a propellant to high speeds to produce thrust. This system includes the power processing unit (PPU), which converts the power it receives to the correct current and voltage required by the thrusters, and the propellant storage and feed systems, which contain and meter the flow of propellant to the thrusters. 5. Thermal Management (Radiators/Heat Rejection) – The cold side of the thermodynamic power conversion cycle, accepts thermal power from the power conversion system and radiatively rejects that heat to space. In this paper, we describe the SNP project formulation and investment strategy that aims to accomplish the research and development required to advance the technology readiness for each CTE. The strategy relies heavily upon experimental testing supported by modeling and simulation to yield realistic assessments of the technologies, which in turn will be used to inform future NEP system-level design decisions and any potential technology downselects.

Kurt A Polzin↗

DOE OSTI2024

DoD Symposium Presentation

TRISO fuel, or TRi-structural ISOtropic, is a ceramic based nuclear fuel capable of operating at high temperatures (up to 1600°C). The fuel, consisting of uranium oxycarbide (UCO) fuel kernels, is coated with three layers of carbon and ceramic (dense silicon carbide) materials to capture and contain radioactive fission products. BWXT, located in Lynchburg, VA, has perfected the manufacturing techniques to produce this fuel and is currently the only US company licensed to produce this irradiation-tested fuel. BWXT is currently producing fuel in support of a demonstration reactor scheduled for startup on the INL site in 2025. The first fuel delivery, estimated at 200 kilograms High Assay Low Enriched Uranium, is targeted for the end of CY2024.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2021

Yttrium Hydride Post Irradiation Examination Plan

The overarching goal of the Department of Energy Office of Nuclear Energy (DOE-NE) microreactor program is to develop technologies for the deployment of civilian microreactors by stakeholders1. Microreactors are expressed as advanced transportable nuclear reactors operating at low power (<20MWth) but high temperatures (>600°C), as well as plug-and-play and inherently safe designs. One prerequisite of a microreactor is the compactness, so that a truck can transport the reactor under safe conditions with the current road infrastructure1,2. The compactness of these reactors likely can be attainable by use of solid components for the essentials of the nuclear core, such as fuel, core heat removal components, reflectors, and moderators. Among these essentials, where fuel enrichment must remain < 20% to meet High Assay Low Enrichment Uranium criteria (HALEU), the largest contribution to the compactness is offered by use of solid moderators which benefit from light atomic weight elements, such as hydrogen, carbon, and beryllium2. Among these, hydrogen-bearing materials, such as metal hydrides, are superior to other options from the lowest critical mass standpoint. Noting that, factors other than critical mass should be considered for a specific reactor design. Yttrium- or zirconium-based metal hydrides have been down-selected due to their neutronic performance. In addition to the neutronic perspective, maintaining hydrogen within the metal hydride is important at the high operating temperatures proposed by advanced reactors. Yttrium hydride (YHx) is, therefore, a proposed moderator material that offers better hydrogen retention at higher operating temperatures than zirconium hydrides due to higher retention and thermal stability of hydrogen in the metal3. The irradiated materials properties of metal hydrides, in this case YHx, must be assessed for the qualification of these moderators. Material testing and inspection processes must illustrate that the effects of dimensional and property changes on thermophysical and mechanical properties do not cause any significant changes on the microreactor safety, and the moderating power is maintained within design limits. Thus, the effect of irradiation on the thermophysical and mechanical properties must be determined. This post-irradiation examination (PIE) plan specifically aims to determine these properties for YHx following Advanced Test Reactor (ATR) irradiation.

99 GENERAL AND MISCELLANEOUS↗

DOE OSTI2022

PLN-6268 Yttrium Hydride Post Irradiation Examination Plan

99 GENERAL AND MISCELLANEOUS↗

DOE OSTI2022

Towards a Benchmark Experiment with the Compact Nuclear Power Source

The Compact Nuclear Power Source (CNPS) was a high-assay low enriched uranium (HALEU) tristructural isotropic (TRISO)-fueled, graphite-moderated microreactor constructed in 1987 at Los Alamos National Laboratory. The reactor, conceived as a power source for short-range radar stations, was designed to be "walk-away safe," and was cooled by heat pipes and ambient air. Though the project was formally cancelled after the fuel and moderator material had been received, its potential to meaningfully advance the body of critical and integral data was evident, and critical experiments with a mock-up of the reactor proceeded at TA-18 until its disassembly in 1991. The reflector and some components of the core would later go on to see service as part of the New Production Reactor Modular High-Temperature Gas-Cooled Reactor (NP-MHTGR) critical experiments. In light of the progress made by groups like Westinghouse and X-Energy towards contemporary graphite-moderated microreactors, the system remains an attractive candidate for the basis of a benchmark experiment even today. Uncertainties remain, however, in some features of the system–inconsistencies in the dimensions and composition of the reactor’s components as described in literature and implemented in current computational models. The identification, quantification, and to the extent possible, the minimization of these uncertainties is a crucial task on the path towards creating a benchmark based on the CNPS system. The present work seeks to initiate this process with a survey of available documentation and improvements to the accuracy of CNPS neutronics models.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRSDate not supplied

Affordable Development Strategy for NEP Nuclear Systems

One nuclear electric propulsion (NEP) reactor systems under consideration is a hydride moderated thermal spectrum reactor fueled by high assay low enriched uranium (HALEU). While such a reactor is expected to yield the lightest HALEU reactor design, its development challenges grow exponentially with increasing mission demands, most notably power output, specific weight of the overall system (which may require operation at temperatures exceeding 1200 K), service lifetime, and human-rated reliability. Two of the greatest cost drivers are full-powered nuclear demonstrations and extensive material development campaigns, so it is important to consider options that can minimize the need for or complexity of such tasks. This paper discusses a structured framework being developed for assessing how NEP design choices, such as materials selection, neutronic features, and heat-removal technologies, can translate into project risk and how project performance goals can be traded with development cost.Reactors operating at high temperatures often require cutting-edge heat transfer technologies and creep-resistant materials. Use of new materials in high temperature reactors brings additional complication beyond those common to any new space materials development campaign. For example, such materials may not possess necessary neutronic cross-sectional or neutronic irradiation data. Similarly, use of new materials may significantly influence core neutronics; in some extreme cases, neutronic reactivity feed-back of certain new materials can vary during their service life as radiation damage impacts the scattering cross-section. In an affordable development approach, high fidelity modeling and simulation tools are used to identify and characterize potential ‘knees-in-the-curves’ in the relationship that exists between the mission characteristics and the project risk. Of particular significance is use of modern uncertainty management and variance reduction methods to perform gap analyses that feed into phenomena identification and ranking tables (PIRT) commonly used to communicate nuclear readiness levels. Model-based measurements techniques are used to design sub-scale experiments as a substitute to minimize orcompletely eliminate the need for nuclear demonstrations.This paper will describe the approach and present preliminary results. It will lay the groundwork for developing a set of metrics that can be broadly characterized as system nuclear readiness levels and advancement degree of difficulty for nuclear systems. Equally importantly, a goal of this paper is to initiate a dialogue among stakeholders on what is the sufficient level of maturity that is required for launching a demonstration unit.

Dasari V Rao↗

DOE OSTI2026

Nuclear Security Risks for HALEU Fuels

There is growing interest in high-assay low-enriched uranium (HALEU) for use in advanced nuclear reactors as a high-energy fuel source. The primary objectives of this report are to identify the security risks that directly result from HALEU and to identify the gaps and challenges it presents from a theft and sabotage perspective. This study focuses on HALEU security risks for the front end of the fuel cycle and includes a review of the supply chain, fuel fabrication, and transport for terrestrial reactors.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Nuclear Data and Benchmarking Program: Nuclear Data Performance Assessment for Advanced Reactors

Over the last several Evaluated Nuclear Data File (ENDF)/B releases, many updates have been introduced to the nuclear data libraries that can significantly change computational results. These changes can be particularly important for advanced reactor concepts, which are not as thoroughly investigated as those used in light water reactor (LWR) systems. Therefore, a performance assessment of the ENDF/B libraries using the SCALE 6.2.3 code package was conducted under the auspices of the U.S., Department of Energy Office of Nuclear Energy (DOE-NE). The following systems relevant to the advanced reactor community were chosen as subject for investigation in this report: sodium cooled fast reactor systems, graphite moderated high temperature gas-cooled reactors, and several molten salt reactor models. At first, the similarity of the integral performance of the ENDF/B-VII.1 and ENDF/B-VIII.0 nuclear data libraries caused by compensating errors in important differential data was demonstrated. In calculations for a shipping container of high-assay low enriched uranium, the data of individual isotopes were systematically swapped between the two ENDF/B libraries. An eigenvalue difference of up to 450 pcm was found due to the use of 235 U and 238 U from one library and 1 H and 16 O from the other library. This clearly demonstrates a cross-correlation between reaction data sets of different isotopes within a library that should be reported in the evaluations. For sodium-cooled fast reactor (SFR) fuel assemblies, significant eigenvalue (k inf ) differences (200– 450 pcm) were found between calculations using the 2011 ENDF/B-VII.1 data and 2018 ENDF/B-VIII.0 data. These differences were mainly caused by updates of 238 U and 239 Pu neutron cross sections. Results from the multigroup (MG) calculations further revealed that the group structure of the applied MG library strongly influences the MG bias due to the importance of an appropriate energy resolution of the resonances in higher energy ranges. The application of previously used MG libraries requires new verification for advanced reactor simulation in comparisons with reference continuous-energy calculations. Nuclear data uncertainty analyses of these SFR systems resulted in eigenvalue uncertainties between 1,400 and 1,800 pcm, which are three to four times higher than corresponding uncertainties in light water reactor (LWR) systems. The main contributor to this uncertainty was found to be inelastic scattering on 238 U, which shows an uncertainty of up to 50% in the fast energy range. Other important contributors are the scattering reactions of 56 Fe and 23 Na which have so far not appeared in LWR analysis. Since the largest contribution to the eigenvalue uncertainty of SFR systems is coming from scattering reactions, it is expected that uncertainties in the angular scattering distributions also have a significant impact. Those uncertainties are, however, not available for the majority of nuclides, and the capabilities to determine sensitivities to this data are currently underdeveloped. For two graphite moderated high temperature gas-cooled reactor (HTGR) benchmarks, only the ENDF/BVII. 1 calculations resulted in consistent eigenvalues (k eff ) with the corresponding experimental measurements. Eigenvalue differences of about 1,000 pcm were found between the 2006 ENDF/B-VII.0 data and the 2011 ENDF/B-VII.1 data, primarily due to an updated carbon capture cross section in the thermal energy range in the later ENDF/B release. The ENDF/B-VIII.0 eigenvalue was larger than the ENDF/B-VII.1 eigenvalue by about 300 pcm mainly due to updates in multiple 235 U neutron cross sections, with offsetting updates in the 238 U cross sections. With ENDF/B-VIII.0, graphite can be modeled as perfect crystal or with two different porosities. The choice of the graphite evaluation can have a significant influence of the eigenvalue. For a HTGR benchmark, maximum eigenvalue differences as high as 650 pcm due to different porosities were observed. More detailed studies of the impact of the porosity are necessary while considering that the graphite porosity can vary between the used materials and changes as a function of neutron fluence. xii The uncertainty of the HTGR eigenvalues due to nuclear data uncertainties was found between 500 and 600 pcm, with the top contributor being the neutron multiplicity of 235 U. A gap in the form of missing uncertainties in graphite thermal scattering data, that might have significant impact on HTGR reactors, was identified. This gap is being investigated by the DOE-NE Nuclear Data and Benchmarking Program, as documented in a separate report The fast spectrum molten salt reactor calculations revealed similar comparisons as for the SFR assemblies. The eigenvalue uncertainties were significantly influenced by inelastic scattering on 238 U, while the impact of angular scattering distributions is unknown. For the graphite and zirconium hydride moderated system, eigenvalue uncertainties of up to 700 pcm were observed, requiring in depth analyses of the cross sections and corresponding uncertainties of the included materials. In general, it was observed that the flux spectra of the various molten salt reactor systems show significant differences, even between a fresh state and a depleted state. The choice of the energy group structure of MG calculations is therefore highly relevant; the applicability of previously used MG libraries needs to be verified. Due the unavailability of pin power measurements of advanced reactor systems, pin power calculations with both ENDF/B-VII.1 and VIII.0 data were performed for a light water reactor and compared to corresponding measurements. Both calculations show good agreement with the measurements. A comparison between the ENDF/B-VII.1 and VIII.0 results revealed small differences, mostly in the range of about 0.2%.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2024

Superoxide Radicals in Uranyl Peroxide Solids: Lasting Signatures Identified by Electron Paramagnetic Resonance Spectroscopy

Abstract U(VI) peroxide phases (studtite and meta‐studtite) are found throughout the nuclear fuel cycle and exist as corrosion products in high radiation fields. Peroxides are part of a family of reactive oxygen species (ROS) that include hydroperoxyl and superoxide species and are produced during alpha radiolysis of water. While U(VI) peroxides have been thoroughly investigated, the incorporation and stability of ROS species within studtite have not been validated. In the current study, electron paramagnetic resonance (EPR) spectroscopy was used to identify the presence of free radicals within a series of U(VI) peroxide samples containing depleted, highly enriched, and natural uranium. Density functional theory calculations indicated that the predicted EPR signals matched well with a superoxide (O 2 − ⋅) species incorporated into the studtite structure, confirming the presence of ROS in the material. Further analysis of samples that were synthesized between 1945 and 2023 indicated that there is a correlation between the radical signal and the product of specific activity multiplied by age of the sample.

Scherrer, Sarah K.↗