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Initial Fracture Propagation Modeling of Graphite Components with Grizzly

Graphite has historically been extensively used in power reactor cores and will be used in multiple types of advanced reactors currently under development. These graphite structural components can experience significant stresses due to nonuniform volumetric strains induced by irradiation and thermal expansion, which can lead to fracture. Robust tools for predicting fracture initiation and propagation in graphite structural components in nuclear reactors are important for evaluating component integrity, developing design standards, and interpreting experimental results to characterize graphite performance. The U.S. Department of Energy’s Nuclear Energy Advanced Modeling and Simulation program has been developing degradation models for other structural components in nuclear reactors within the Grizzly and BlackBear codes. This report documents an effort to develop initial capabilities for modeling graphite fracture within these codes, building on prior efforts to model fracture in other materials. Major elements of this effort include developing a new system for modeling fracture nucleation and growth in two dimensions using the extended finite element method and incorporating a damage and plasticity model. These capabilities are applied here to model a representative graphite component and a splitting disc experiment used to obtain tensile strength.

36 MATERIALS SCIENCE↗

Status memorandum on ORNL support of vendor irradiation capsule design and ASME irradiation code development and new ASTM test standard development activities

This report is in submission of completion of the Level 4 milestone number M4TG-24OR0501111 within the larger Advanced Reactor Technologies Gas Cooled Reactor program at Oak Ridge National Laboratory (ORNL). The focus of this year’s efforts is to continue support of industry needs related to the development of future industry-funded irradiation programs. At ORNL these efforts included the development of a generalized three-dimensional CAD model of an irradiation creep capsules for graphite, cost estimates of the expansion of the Materials Irradiation Facility (MIF), involvement with ASTM D02.F0 “Manufactured Carbon and Graphite Products” and the ASME Boiler and Pressure Vessel Code, and publication of papers supporting these efforts. This report will document the status of these activities.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

In-situ ion irradiation of fission products in a spent UO 2 fuel

This study investigates the behavior of fission gas bubbles and five metal precipitates (5MPs) (Mo, Ru, Rh, Tc, Pd) in spent uranium dioxide (UO 2 ) fuel under various ion irradiation doses, temperatures, and flux conditions. Utilizing in-situ ion irradiation and advanced transmission electron microscopy, we analyzed the evolution of fission gas bubbles and 5MPs in UO 2 samples from the Belgium Reactor 3 (BR-3). Our findings reveal significant shrinkage of fission gas bubbles and 5MPs with increasing irradiation dose, accompanied by a decrease in pair density. We demonstrate that ion irradiation induces a homogeneous re-solution process where individual atoms are ejected from bubbles and precipitates, leading to their dissolution and subsequent re-precipitation in the matrix. In conclusion, this study provides critical insights into the dynamic behavior of fission products under irradiation, facilitating the development of predictive models and contributing to the optimization of nuclear fuel performance and safety.

Fission products↗

In-situ ion irradiation of a spent UO2 fuel: evolution of fission products and nanograins with radiation dose

This study investigates the behavior of fission gas bubbles, five metal precipitates (5MPs) (Mo, Ru, Rh, Tc, Pd) and nanograins in spent uranium dioxide (UO2) fuel under various ion irradiation doses, temperatures, and flux conditions. Utilizing in-situ ion irradiation and advanced transmission electron microscopy, we analyzed the evolution of fission gas bubbles, 5MPs and nanograins in UO2 samples from the Belgium Reactor 3 (BR-3). Our findings reveal significant shrinkage of fission gas bubbles and 5MPs with increasing irradiation dose, accompanied by a decrease in pair density. The study also reveals nanograin coarsening under irradiation. We demonstrate that ion irradiation induces a homogeneous re-solution process where individual atoms are ejected from bubbles and precipitates, leading to their dissolution and subsequent re-precipitation in the matrix. This study provides critical insights into the dynamic behavior of fission products and nanograins under irradiation, facilitating the development of predictive models and contributing to the optimization of nuclear fuel performance and safety.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Considerations for Hydride Moderator Readiness in Microreactors

The emergence of microreactor technology has helped to drive supporting nuclear materials qualification and acceptance processes. One essential component in these small reactors is a solid moderator, which typically consists of metal hydride and cladding. While the behavior and performance of metal-hydride moderators go back to early advanced reactor development for nuclear-powered aviation and space propulsion, there remains a knowledge gap in the understanding of hydrogen transport–related phenomena and irradiation performance for hydride moderators. This impacts the acceptance/qualification of hydride moderators for microreactors. The goal of this technical note is to lay out a potential path forward for advanced moderator qualification and acceptance for designers and developers of microreactors. The proposed approach has benefited from a model microreactor core with the design parameters of a hydride moderator. Based on the model core and design parameters, a simple chart was developed for the major challenges of hydride moderators where potential incidents, causes, effects, and resolutions are described. The relation between the offered resolutions and the maturity of the metal-hydride moderator technology was emphasized using technological readiness. Technological readiness levels (TRLs) were clustered to three sets: physical phenomena related, reactor irradiations, and system demonstration. Some essential needs to fill the knowledge gaps are discussed for physical phenomena–related TRLs. For reactor irradiations, the importance of identifying goals and priorities is stressed to reach certain TRLs. For system demonstration, it is noted that metal-hydride moderator qualification must comply with the overall microreactor design.

36 MATERIALS SCIENCE↗

Accelerated Irradiation Testing and Post-Irradiation Characterization: U.S.-Based Capabilities for Advanced Nuclear Systems and Radioisotope Production

Irradiation experiments and post-irradiation examinations, together referred to as irradiation testing (IRT), are prerequisites for nuclear fuel and material qualification for the deployment of new and advanced reactors, as well as radioisotope production, thereby ensuring regulatory compliance. Qualified research and test reactors (RTRs) and testing facilities are essential to enable IRT to verify performance and safety under prototypical reactor conditions. In the past, qualification of new fuels or structural materials required about 20 years. Synergist strategies, advanced tools, and qualified methods are needed to greatly reduce this timeframe of IRT and radioisotope production. This study, termed accelerated-IRT, focuses on identifying gaps and leveraging U.S.-based RTRs and material testing capabilities, leveraging the preliminary evaluation and qualification of selected RTRs to provide a generic as well as specific-case solution paths forward, ensuring adherence to stringent regulatory standards. Furthermore, IRT and radioisotope production utilizing qualified RTRs necessarily includes modeling and simulation to support the design (i.e. neutronics, thermal, and structural aspects) and manufacturing of irradiation test specimens, vehicles, capsules, apparatuses, and flow loops. In addition, IRT can be improved by applying advanced manufacturing techniques and in-pile sensors and instrumentation, as discussed in this study.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Irradiation Damages of Structural Materials under Different Irradiation Environments

For the advancement and development of nuclear systems used in heavy irradiation environments such as fusion DEMO reactors, fission reactors, fast reactors, and accelerator driven target systems, it is necessary to fully understand the changes of mechanical properties and the other properties of the materials induced by irradiation and to clarify the synergistic effect of displacement damage and helium generation. In this study the mechanical property changes and microstructural development induce by displacement damage and helium production have been mainly examined in austenitic stainless steels, 316FR and type304, and ferritic/martensitic steel, HCM12A, irradiated at around 550oC in JRR-3M reactor and/or JOYO fast reactor. At 550°C, 316FR steel was superior to 304 steel in terms of the amount of ductility and strength with respect to irradiation resistance. It is noteworthy that at 550 °C as well as room temperature, the higher fracture strength of the 316FR steels is a remarkable result. It is found that helium atoms strongly influenced on creep lifetime of the irradiated austenitic stainless steel, 316FR. It was found that the ratio of creep rupture time is slightly lower than the lower limit of previous study’s Miyaji and co-workers in the region from 0.01 appm to 1 appm. It is also found that the lower limit of reduction ratio of creep rupture time (irradiation specimen to unirradiation one) does not decrease linearly with the helium production above 10 appm up to about 33 appm. dpa enhanced the reduction of creep lifetime. Recent R&D of high-energy accelerator driven target systems used under heavy irradiation environment is also introduced and discussed for high radiation resistance materials such as Ti alloys with very high number density of nano size precipitate, which have been studying under RaDIATE collaboration, from points of view of irradiation damage and materials development.

radiation damage, structural alloys, neutron irrad↗

Development of Refractory Alloys and Refractory Coatings for Advanced Nuclear Reactors

The next generation of nuclear reactors will benefit from materials that enable operation at higher temperatures (>500°C), higher irradiation doses (up to 200 displacements per atom (dpa)), and the use of more corrosive and reactive coolants. This work package represents the first experimental steps towards a longer-term effort to develop refractory materials for nuclear energy applications which will enable operation under these conditions. Specifically, this work package focuses on additive manufacturing of refractories as both a refractory liner coating deposited onto the interior surface of a metallic tubular backbone and as bulk refractory alloys. During fiscal year 23 (FY23), several refractory metal coating systems and bulk alloys were examined and selected using a decision criteria matrix. The refractory metal coating systems included molybdenum, tungsten, and zirconium as refractory coatings on backbones of either carbon-carbon (C/C) or silicon carbide-silicon carbide (SiC/SiC) ceramic matrix composites. The bulk refractory alloys included C-103, WTa, and WNiFe as bulk alloys. During FY24 additional bulk refractory alloys and metallic backbones were evaluated using the decision criteria matrix based on input from the AMMT leadership team. These included 316 SS and 316H SS for the metallic backbones and Mo-La, Ta, and Nb1Zr as bulk refractory alloys. The primary focus for the FY24 effort was placed on establishing the capabilities to deposit refractory coatings based on the results of the scoring in the decision criteria matrix and finalizing the additively manufactured TZM studies which were incorporated into the AMMT program from the microreactor program. Further efforts were dedicated to establishing the capabilities to additively manufacture down-selected bulk refractory alloys.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Capability Needs for Irradiated and Radioactive Materials Research (Ad hoc Committee Summary Report)

It is essential for the U.S. nuclear energy community to have access to world-leading equipment suitable for conducting research on both nuclear fuels and structural materials, including neutron irradiated–and therefore activated–materials. To address future research infrastructure requirements to support the DOE-NE mission, the Office of Reactor Fleet and Advanced Reactor Deployment established an ad hoc committee to gather information on potential capability gaps for radioactive materials and radiation effects research. This document summarizes the discussions of the committee addressing the high-level challenges in irradiated and radioactive materials research and the capabilities needed to address these challenges. After considering the various needs, the committee agreed on the four top-level targets and priority capability gaps.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

AGC-2 Graphite Preirradiation Data Analysis Report

This report describes the specimen loading order and documents all preirradiation examination material property measurement data for graphite specimens contained within the Second Advanced Graphite Capsule (AGC 2) irradiation capsule. The AGC 2 capsule is the second in six planned irradiation capsules comprising the Advanced Graphite Creep (AGC) test series. The AGC test series is used to irradiate graphite specimens in order to garner quantitative data necessary for predicting the irradiation behavior and operating performance of new nuclear grade graphites. This testing will ascertain the in service behavior of the graphite for pebble bed and prismatic very high temperature reactor designs. Similar to the First Advanced Graphite Capsule (AGC 1) preirradiation examination report, material property tests were conducted on specimens from 18 nuclear grade graphite types. However, AGC 2 tested an increased number of specimens (i.e., 512) prior to loading them into the AGC 2 irradiation assembly. All AGC 2 specimen testing was conducted at Idaho National Laboratory from July 2009 to August 2010. This report also details the specimen loading methodology for graphite specimens inside the AGC 2 irradiation capsule. The AGC 2 capsule design requires “matched pair” creep specimens that have similar dose levels above and below the neutron flux profile mid plane. This provides similar specimens with and without an applied load. Analysis in this document utilizes the neutron flux profile calculated for the AGC 2 capsule design, the capsule dimensions, and the size (i.e., length) of the selected graphite specimens to create a stacking order that produces “matched pairs” of graphite specimens above and below the AGC 2 capsule elevation mid point, thus providing specimens with similar neutron dose levels.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Irradiation enhanced diffusion and diffusional creep in U₃Si₂

U₃Si₂ is a candidate as an advanced fuel for light water reactors (LWRs). Compared to UO₂, there are significant data gaps for the thermophysical and thermomechanical properties of U₃Si₂. Atomic scale simulations can help fill in those gaps, while also providing a more mechanistic understanding of the material properties. Creep is an important property for fuel performance as it influences the pellet-cladding gap, which in turn affects the temperature of the fuel (a key parameter in many other aspects of fuel behavior). In this work, we employed a DFT-informed cluster dynamics framework to predict point defect concentrations in U₃Si₂. The concentrations, diffusivities, and volumes of these defects were used to develop a diffusional creep model based on bulk (Nabarro-Herring) and grain boundary (Coble) diffusion processes. It was found that irradiation enhanced Nabarro-Herring creep is dominant at low temperatures, while Coble creep dominates for high temperatures. The model compares well against available experimental data and has been implemented in BISON. A demonstration case using simple power profiles has been carried out, showing that negligible creep occurs due to the low temperatures experienced by U₃Si₂, a consequence of its high thermal conductivity.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Report on the Integration of Experimental and Modeling Data for Initial Equivalence Study of Microstructural Evolution in Irradiated LPBF 316SS

Advanced materials and manufacturing technologies are poised to improve the safety and design characteristics of nuclear technologies and meet US energy, environmental, and economic needs. In particular, metal additive manufacturing (AM) provides an opportunity to produce novel materials and component geometries, but their use is not without hurdles arising from the inherent microstructure variability that can result from the layer-by-layer build approach. Given the greater possible microstructure variability in AM materials—and the dearth of materials test reactors—it is impractical to rely solely on neutron irradiation studies to produce data for materials qualification for every possibility. This work within the Advanced Materials and Manufacturing Technologies (AMMT) Environmental Effects technical area contributes to the rapid qualification framework by developing a science-driven framework for the accelerated qualification of materials for nuclear environments. A key product of the Environmental Effects technical area of the AMMT program is the Licensing Approach with Ions and Neutrons (LAIN). This approach recognizes that whether using existing materials in new environments, newly developed materials tailored for these environments, or new manufacturing methods, the traditional decades-long approach for materials qualification does not facilitate rapid deployment. In FY 2023, the AMMT program presented a conceptual framework of specific steps to fulfill several technical challenges associated with qualifying materials for performance in radiation environments on an accelerated time frame informed by the state of the art in materials science and a review of the current regulatory landscape. The objective of this section of the Environmental Effects technical area is to critically evaluate and refine the proposed qualification framework presented under AMMT by integrating the research results of the neutron irradiations, the ion irradiations, and modeling efforts. These ongoing efforts span across Argonne National Laboratory (ANL), Idaho National Laboratory (INL), and Oak Ridge National Laboratory (ORNL) and are closely coordinated.

36 MATERIALS SCIENCE↗

Influence of Irradiation-induced Microstructural Defects on Thermal Transport in Single Crystal Thorium Dioxide

Microstructural defects formed as a result of fission fragment damage are known to drastically alter thermal conductivity, a fuel property that governs the efficiency of a nuclear reactor. A fundamental understanding of radiation-induced effects on thermal transport is critical for the development of advanced fuels. Ion-irradiation has widely been used to simulate the effects of neutron-irradiation by seeding atomic-to-nanoscale defects of controllable size and density. In this work, we investigate the influence of microstructural defects, induced by ion-irradiation, on the thermal properties of single crystal thorium dioxide samples grown using the hydrothermal technique. The samples were irradiated using 2 MeV protons at room temperature. A laser-based modulated thermoreflectance technique was used to measure the thermal diffusivity and conductivity within the damaged ThO2 region. The experimentally measured thermal properties were compared with Boltzmann Transport Equation predictions, to determine the impact of various defect types on the thermal properties of ThO2.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Development and formulation of physics based metallic fuel models and comparison to integral irradiation data

Metallic fuel has an important historical significance in the development of nuclear reactors and continues to be relevant to the progression of advanced test and power reactors. A number of models, ranging from empirical to mechanistic, have been developed and implemented in various fuel performance codes to describe U-Zr and U-Pu-Zr fuel and typical fast reactor cladding materials. One challenge of using these models to simulate fuel performance is the inevitable tangling of coupled phenomena that can cloud proper implementation, calibration, and eventual utilization of new models. Here in an effort to provide a baseline capability that will facilitate the use of advanced models, new capabilities have been implemented into the fuel performance code BISON specific to metallic fuel simulations, ranging from materials properties, fission gas release and swelling calculations, coolant channel models, and cladding correlations. These models have been applied to the X441/X441A EBR-II experimental assembly data, a set of irradiated metallic UPuZr fuel rods of varying pin designs. The models implemented in BISON are able to capture the general trend of the expected response of the fuel and cladding to irradiation in EBR-II, especially when considering the spread in experimental measurements and the uncertainties inherited from the historical material models. Ultimately, the models outlined here provide the baseline capabilities on which new models can build upon in order to improve the prediction of metallic fuel performance simulations in off-normal designs or operations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Ab-initio informed cluster dynamics simulation of self- and Xe diffusivity in uranium mononitride under irradiation

Uranium mononitride (UN) is one of the ceramic nuclear fuel alternatives to oxide fuels considered for light water reactor and advanced reactor designs, as it presents significant advantages such as high uranium density (better economics) and high thermal conductivity and melting point (increased safety). Self- and fission gas diffusivities need to be better understood, given that they influence key fuel performance phenomena like swelling and fission gas release. Recently, radiation enhanced diffusivity was investigated in UN by means of cluster dynamics simulations relying on empirical potential-based parameterizations, the reliability of which highly depends on the interatomic potential accuracy. Here, in this work, we refine this approach by determining, using ab-initio calculations, the properties of defect clusters containing vacancies, self-interstitials and Xe impurities. We also consider larger clusters than previous studies. The obtained dataset (formation enthalpies, entropies, and migration barriers) is used to parameterize a cluster dynamics model of mobile clusters, and to calculate the defect cluster concentrations under irradiation. This gives us access to the radiation enhanced self- and fission gas diffusivities. Although the resulting diffusivities are close to the values reported in the literature, we find important qualitative differences in the diffusion mechanisms. Capturing the correct mechanisms is crucial to properly describe the chemistry and fission rate dependence of the model.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Advanced Test Reactor Neutron Dosimetry Report - 173B

Results of neutron dosimetry measurements in ATR for cycle 173B-1&2 are presented. Cobalt and nickel wires were installed in numerous irradiation locations for the duration of the cycle. The specific activity of these wire segments can be used in conjunction with the presented cycle history information to determine the thermal- and fast-neutron fluence rates for each irradiation position during the cycle using the referenced standard test methods.

173B↗

NON-DESTRUCTIVE POST IRRADIATION EXAMINATION OF FIRST CYCLE ACCIDENT TOLERANT AND ADVANCED ZIRCONIUM ALLOY HIGH BURNUP FUEL RODS

Post irradiation examination (PIE) of accident tolerant fuel concepts and high burnup uranium dioxide advanced zirconium alloy clad fuel contribute to near term nuclear industry goals of enhancing light water reactor safety and economics. Westinghouse is developing chromium coated zirconium alloy cladding as an accident tolerant fuel option for current pressurized water reactors. Examination of high burnup fuel further augments the technical foundation for extending the peak rod average burnup limits beyond the current regulatory limit of 62 MWd/kgU. Seven fuel rods were received at the Oak Ridge National Laboratory Irradiated Fuel Examination Facility. This includes three chromium coated zirconium alloy fuel rods and four high burnup advanced zirconium alloy fuel rods. Six of the seven rods were fueled with standard uranium dioxide while one of the chromium coated rods contained Westinghouse’s ADOPT fuel. The overall hot-cell PIE plan and some PIE results have been presented previously. This paper focuses on the additional non-destructive examination and fission gas release. Highlights from visual examination of these rods are presented. The chromium coating showed little to no visual change following irradiation. Observations of the axial burnup trends in the fuel rods are derived from full rod axial gamma-ray scans with additional observations related to local fission product migration. The axial dimensional changes of the seven rods are evaluated. As expected, creep down had not yet occurred in the chromium coated rods, and the maximum diameter strain in the high burnup advanced zirconium alloy cladding was less than 0.5%. Finally, the steady state fission gas release for these rods was measured ranging from 4.1% to 17.6% which matched expectation from literature. These fuel rods now await further destructive examination.

Harp, Jason↗

FY2022 Progress Report for Advanced Re-fabrication/Re-instrumentation Capability Development

In support of performing follow-on irradiation experiments with previously irradiated materials, the Halden Reactor Project developed unique and state of the art capabilities to refabricate and re-instrument previously irradiated materials. Such materials were used in in-pile tests at the Halden reactor, and out-of-pile tests for example using furnaces as a heat source. The decision to close the Halden Reactor Project results in the loss of this refabrication and re-instrumentation capability. As a result, the United States (U.S.) Department of Energy (DOE) has determined to develop refabrication and re-instrumentation capability at the unique shielded facilities at Idaho National Laboratory (INL). The development of refabrication capability has been completed and demonstrated. This report focuses on the complementary aspects of reinstrumentation and the progress to-date. Halden spent nearly 30 years developing both refabrication and re-instrumentation. Collaboration with Halden is allowing Idaho National Laboratory (INL) to develop this capability much more rapidly. In FY-21 the results include development of the capability to drill annular center holes in ceramic UO2 fuel pellets, development of fuel rod end caps with feedthroughs for centerline instrumentation inside the rodlet, The procurement of both fuel drilling and welding demonstration equipment from Halden, evaluation of surface thermocouple attachments to support better understanding of temperature measurement uncertainties, and finally, the conceptual design of a new shielded enclosure where advanced refabrication and re-instrumentation equipment can be housed. In FY-22, the results include; Completing set up of the drilling and welding modules procured from Halden, and early experimental trials using that equipment.; Completing set up of an out-of-cell circumferential weld system to allow for further weld development to take place and support fabrication of fuel for fresh fuel experiments.; Evaluation of the Hot Fuel Examination Facility (HFEF) infrastructure to support future installation of advanced re-fabrication/re-instrumentation equipment, specifically related to necessary infrastructure for cryo-drilling.; Developments in dry-drilling alternative. Including experimental studies showing cordierite is the most suitable surrogate for UO 2 for performing drilling studies. That drilling performance is enhanced when a fuel-clad bonding condition is simulated.; Conceptual design completed for attaching surface thermocouples to irradiated fuel in support of TWIST capsule experiments. The authors would like to thank the numerous colleagues at INL and Halden who provided support in accomplishing this work. Their support both material and intellectual is invaluable in advancing the state of the art and establishing the capabilities for refabrication and re-instrumentation at INL.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗