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At least 181 records · Page 10

An integrated statistical-thermodynamic model for fission gas release and swelling in nuclear fuels

Here, we propose a new model for burst fission gas release induced by microcracking in ceramic nuclear fuels such as uranium dioxide. The model stipulates that the densities of defects in the fuel material, such as microcracks and fission gas bubbles on grain boundaries, evolve in accordance with the second law of thermodynamics. Central to the model is the notion of an effective temperature, conjugate to the configurational entropy of the fuel material, and directly linked to the burnup. The model predicts that microcracking, driven by the internal stress state of the fuel material, reduces the bubble storage capacity of grain boundaries, and accounts for burst fission gas release during rapid temperature transients that simulate power transients, reactor startup, and loss-of-coolant accident conditions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Electron microscopy data on irradiation effects in glassy carbon, nuclear graphite, pyrolytic carbon, and carbon fibers

Glassy carbon, a monoatomic allotrope of carbon, is a candidate material for components in fission nuclear power systems due to its radiation tolerance. This article presents comprehensive electron microscopy data revealing the effects of neutron and electron irradiation on glassy carbon. For comparison, additional data are provided for pyrolytic graphite and carbon fibers, materials that exhibit similar structural behavior under irradiation. In situ electron irradiation experiments further illustrate the real-time microstructural evolution of glassy carbon during exposure. The dataset is organized into five parts: (1) transmission electron microscopy (TEM) micrographs of as-received and neutron-irradiated glassy carbon; (2) TEM micrographs of neutron-irradiated graphite; (3) TEM micrographs of unirradiated and irradiated carbon–carbon composites; (4) TEM micrographs of pyrolytic carbon specimens in both conditions; (5) scanning transmission electron microscopy (STEM) micrographs of as-received and neutron-irradiated glassy carbon and (6) in situ electron irradiation data of a glassy carbon particle. These datasets provide valuable insights into radiation-induced structural changes in carbon-based materials relevant to nuclear applications.

36 MATERIALS SCIENCE↗

Peer Review of X441A Fission Gas Release Data

The purpose of this document is to demonstrate completion of the independent peer review for the fission gas release measurement of fuel pins irradiated in the Experimental Breeder Reactor-II (EBR-II) as part of the X441A experiment. The specific data reviewed includes reported plenum volume and pressure from the measurement from the fuel pins. Fraction percent of fission gas release is derived in part from these measurements but is excluded from the data reviewed.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Redistribution of radionuclides in irradiated AGR-1 UCO TRISO fuel after 1800 °C safety testing

Release of radionuclides from intact tristructural-isotropic (TRISO) coated particle fuel at normal and accident conditions is a primary metric of fuel performance. The distribution of fission products and actinides in the TRISO layers of individual particles provides insight on radionuclide transport and release behavior and was determined using scanning electron microscopy analysis. Particles were isolated from an irradiated fuel compact (AGR-1 Compact 4-4-2) and analyzed as-irradiated or after individual particle safety-testing at 1800 °C for 650 h. Particles were selected for comparison based on their remaining 110mAg fission product inventory. These comparisons corroborated the observation that the 110m Ag inventory is a marker for relative irradiation temperature based on observed radionuclide distribution in the SiC layer. The comparison also indicated that the in-pile behavior influences the fission product and actinide species interactions with the TRISO layers during high temperature exposure after irradiation. The analysis confirms both palladium and uranium diffusion, as well as other species, are active in the UCO TRISO fuel system at 1800 °C and that palladium transport is active at lower temperatures relative to uranium. While diffusion across the SiC layer was observed, the intact nature of the SiC layer after the 1800 °C, 650-h exposure indicates the SiC layer maintained its functionality as a fission product barrier by mitigating release of radionuclides at beyond accident margin temperatures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fundamental Phenomena and Applications of Swift Heavy Ion Irradiations

This review concentrates on the specific properties and characteristics of damage structures generated with high-energy ions in the electronic energy loss regime. Irradiation experiments with so-called swift heavy ions (SHIs) find applications in many different fields, with examples presented in ion-track nanotechnology, radiation hardness analysis of functional materials, and laboratory tests of cosmic radiation. The basics of the SHI-solid interaction are described with special attention to processes in the electronic subsystem. The broad spectrum of damage phenomena is exemplified for various materials and material classes, along with a description of typical characterization techniques. This review also presents state-of-the-art modeling efforts that try to account for the complexity of the coupled processes of the electronic and atomic subsystems. Lastly, a brief discussion at the end of this review on SHI phenomena induced by fission fragments in nuclear materials will highlight the relevance of energetic ion irradiation in nuclear technology applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Interlayers and associated systems, devices, and methods

Embodiments related to interlayers (e.g., interlayers comprising a transition metal oxide, a transition metal oxynitride, and/or a transition metal nitride) and associated systems, devices (e.g., photovoltaic devices), and methods are disclosed. In some embodiments, a system for exciton transfer includes a substrate including an inorganic semiconductor. An interlayer may be disposed on the substrate, and a layer including a material that undergoes singlet exciton fission when exposed to electromagnetic radiation may be disposed on the interlayer. The interlayer may be disposed between the substrate and the layer. In some embodiments, a method for manufacturing a system for exciton transfer involves depositing an interlayer onto a substrate that includes an inorganic semiconductor. The method may also include depositing a layer including a material that undergoes singlet exciton fission when exposed to electromagnetic radiation onto the interlayer.

Baldo, Marc A.↗

Refining a Novel Process Monitoring Method to Safeguard Continuously Cycling Designs Using Isotopic Ratios

In advanced reactor (AR) designs, a common feature is continuous chemical processing and circulation of the nuclear material. This work bridges a significant measurement gap in safeguarding reactors with circulating fuel or continuous refueling by leveraging and building on the isotope ratio method first developed by our team under an FY21 Advanced Reactors International Safeguards Engagement (ARISE) project (Uribe et al. 2021). In circulating fuel designs, the radioisotope inventory changes from traditional effects (e.g., radioactive decay, fission) but also includes material transport due to pressure and temperature gradients. Such designs may also require regular or continuous additions or removals during operation, which significantly increases the rate of inventory change compared to traditional pressurized water reactor (PWR)s. Thus, directly tracking the nuclear inventory is ineffective since the isotopes are continuously added and removed. The isotope ratio method instead focuses on detecting changes to the input and output flows of radioisotopes. Previous work showed that for well-chosen pairs of isotopes, the isotopic ratio provides a sensitive and lasting indicator of deviation from normal conditions (e.g., startup, shutdown, diversion). The isotope ratio method is a process monitoring method with potential for application in for forward-looking approaches to International Atomic Energy Agency (IAEA) safeguards. The original process monitoring method was developed for a specific case—the decay tank of a thorium-fueled molten salt breeder reactor. In this expanded work, we explored other types of reactors and processes with nonstationary (e.g., flowing) nuclear material, which are difficult to safeguard with traditional methods because of the transient nature of the systems. The goal of the present work is to generalize the isotope ratio method for use in processes with continuously flowing nuclear material. All continuous processes have an average time for isotopes to be replaced in the system. The isotope ratio method works by choosing radioisotopes with half-lives both above and below the processing time. The present work seeks to explore which isotopes are suitable for the method by simulating the nuclear inventory, radioisotope emissions, and detector responses for several classes of advanced reactors. While the method can in principle be applied to other processes (e.g., enrichment or reprocessing facilities), the present work limits scope to ARs with continuously flowing fuel. Section 2 details the mathematics supporting the isotope ratio method, and Section 3 introduces the representative ARs selected for this work. Section 4 discusses how each reactor was analyzed, and Section 5 showcases the results for each representative reactor. Finally, Section 6 provides concluding remarks and suggests pathways for further analysis.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Understanding grain refinement and intergranular gas bubble evolution in U-10Mo fuel using phase-field modeling

Monolithic U-10Mo fuel undergoes significant microstructural changes in the form of grain refinement and gas bubble formation during burnup, which degrades its mechanical properties. In this talk, I present a phase-field model for microstructure evolution in U-10Mo developed using the Multiphysics Object-Oriented Simulation Environment (MOOSE) framework. Simulations demonstrate that grain refinement initiates at pre-existing grain boundaries (GBs) to eliminate the lattice distortion energy caused by the accumulation of self-interstitial loops. By employing an equation of state for xenon gas, we simulate the evolution of gas bubbles in the polycrystal microstructure. Large, interconnected bubbles are found to form along the triple junctions. The effects of defect production rate, diffusivities and GB mobility on the microstructure evolution are systematically studied. Homogenization is employed on the microstructures to obtain effective elastic constants and diffusivity as a function of fission density. The simulations provide critical insights on microstructure and property degradation in U-10Mo fuel.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Demonstrate Viability of Accelerated Fuel Qualification Approaches

This presentation summarizes the research under LDRD grogram, Demonstrate Viability of Accelerated Fuel Qualification Approaches. It is demonstrated that the fabrication process of uranium carbide fuel has been developed and neutronic, thermal and hydraulic analysis have been conducted for the Fission Accelerated Steady-state Testing (FAST). This program provides basis of expansion of FAST as an efficient platform to broad nuclear fuels.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Improved Fuel Particle and Compact Matrix Fission Product Release Prediction with Improved Mass Transfer Model

This study was motivated by the need to incorporate more physics-based mass transfer models in BISON in order to improve fuel particle and compact matrix fission product release prediction. This document details the integration of new modeling capabilities in BISON, including (1) development of sorption mass transfer models; improvement of thermal contact model by adding neon to the gas gap inventory, (3) implementation of PCEA and IG-110 graphite thermal models, (4) validation using Advanced Gas Reactor (AGR)-3/4 compact and capsule rings data. These new capabilities have been shown to enforce the desired physics with satisfactory accuracy. BISON’s predictions of fission product release of AGR-3/4 compacts compare favorably with PARFUME and the concentration profiles across capsule rings show reasonable trend to the experiment measurement.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Spatial separation of triplet excitons drives endothermic singlet fission

Molecules that undergo singlet fission, converting singlet excitons into pairs of triplet excitons, have potential as photovoltaic materials. The possible advantages of endothermic singlet fission (enhanced use of photon energy and larger triplet energies for coupling with common absorbers) motivated us to assess the role of exciton delocalization in the activation of this process. Here we report the synthesis of a series of linear perylene oligomers that undergo endothermic singlet fission and have endothermicities in the range 5-10 kBT at room temperature in solution. We study these compounds using transient spectroscopy and modelling to unravel the singlet and triplet dynamics. We show that the minimal number of coupled chromophores needed to undergo endothermic singlet fission is three, which provides sufficient statistical space for triplet excitons to separate and avoid annihilation - and a subsequent fast return to the singlet state. Our data additionally suggest that torsional motion of chromophores about the molecular axis following triplet-pair separation contributes to the increase in entropy, thus lengthening the triplet lifetime in longer oligomers.

14 SOLAR ENERGY↗

In situ high-temperature 3D imaging of the damage evolution in a SiC nuclear fuel cladding material

Silicon carbide (SiC)-based nuclear fission fuel rod cladding has been considered as one of the possible designs for accident tolerant fuels. It is in the form of a SiC fibre reinforced SiC matrix composite tube (SiC f -SiC m ) with monolithic SiC outer and/or inner coating layers. This study focuses on the deformation and fracture processes in this material using in situ X-ray micro-computed tomography (XCT) at room temperature (RT) and 1200 °C in an inert gas environment in a C-ring compression loading configuration. Prior to testing, local properties and residual stresses were characterised using nanoindentation and Raman spectroscopy since they can impact the mechanical behaviour of the material. The 3D strain distribution, crack formation and propagation processes including the toughening mechanisms (e.g., crack deflection, micro-cracking, crack bridging and bifurcation) are investigated in the coating and underlying composites at RT and 1200 °C. There is no particular sequence which toughening mechanism occurs first – this is very different from the conventional toughening theory in ceramic-matrix composites under uniaxial tension loading. Indeed, no evidence of fibre pull-out or fibre fracture was observed in this SiC f -SiC m nuclear cladding material in the current C-ring compression configuration. The correlation between local measurements and bulk mechanical behaviour are discussed.

3D imaging↗

AGR TRISO Fuel Fission Product Release Data Summary

Knowledge of fission product retention in and release from TRISO fuel under normal and off-normal conditions is needed for reactor safety analyses. This is important for coated-particle fuel used in high-temperature reactors relying on the functional containment strategy. Data on the release and retention of key fission products (e.g., Ag-110m, Cs-134, Eu-154, and Sr-90) in AGR UCO TRISO fuels have been summarized in this report, and empirical relationships with respect to time and temperature were developed. This included fission product accumulation in the OPyC and compact graphitic matrix during irradiation, release from compacts during irradiation, and release during post-irradiation safety testing at temperatures from 1600-1800°C. The frequencies of SiC failure and TRISO coating failure from irradiation and post-irradiation safety testing were also summarized as they have bearing on the quantities of Cs release from the fuel. In a forthcoming publication, a framework for combining and using these empirical relationships as part of a source term analysis will be presented.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Evaluations of Silicon Carbide Temperature Monitors

The effect of irradiation on materials properties is an important field of study for materials usage in both fission and fusion systems for energy production. Neutron flux and energy spectrums are well understood; however, the irradiation temperature can be more difficult to determine. Since the early 1960s, Silicon Carbide (SiC) has been used as a passive post-irradiation temperature monitor because the irradiation defects anneal out above the irradiation temperature. Irradiation temperature is determined by measuring a property change after isochronal annealing or during a continuously monitored annealing process. There are many properties that may be measured including electrical resistivity, bulk density, dimensions, thermal diffusivity, or lattice spacing. Electrical resistivity is accepted as a robust measurement technique; however, such method is time-consuming since the steps involved must be performed in a serial manner. The use of thermal expansion from continuous dilatometry is an automated process requiring minimal setup time. As part of a Nuclear Science User Facilities (NSUF) project, low dose silicon carbide monitors were irradiated in the BR2 material test reactor at SCK, Belgium, and were then evaluated at the Idaho National Laboratory (INL) High Temperature Test Laboratory (HTTL) to determine their peak temperature achieved during irradiation. The technical significance of this work was that the monitors were irradiated to a dose that was significantly less than recommended in published literature. This paper will discuss the evaluation processes available at HTTL and the performance of the low dose silicon carbide temperature monitors.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Impact of grain boundary and surface diffusion on predicted fission gas bubble behavior and release in UO 2 fuel

In this work, we quantify the impact of grain boundary (GB) and surface diffusion on fission gas bubble evolution and fission gas release in UO 2 nuclear fuel using simulations with a hybrid phase field/cluster dynamics model. Here, we begin with a comprehensive literature review of uranium vacancy and xenon atom diffusivity in UO 2 through the bulk, along GBs, and along surfaces. In our model we represent fast GB and surface diffusion using a heterogeneous diffusivity that is a function of the order parameters that represent bubbles and grains. We find that the GB diffusivity directly impacts the rate of gas release via GB transport, and that the GB diffusivity is likely below 104 times the lower value from Olander and van Uffelen. We also find that the surface diffusivity impacts bubble coalescence and mobility, and that the bubble surface diffusivity is likely below 10 -4 times the value from Zhou and Olander.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Cluster dynamics simulation of xenon diffusion during irradiation in UO 2

Diffusion of fission gas in UO 2 nuclear fuel impacts several important performance metrics, such as fission gas release, swelling, and thermal conductivity. Current empirical models of fission gas release have significant uncertainty, some of which derives from the bulk diffusion rate and its dependence on, for example, fuel chemistry and irradiation. In this work, we have applied the previously-developed Free Energy Cluster Dynamics (FECD) methodology in the code Centipede to calculate xenon cluster concentrations in UO 2 under intrinsic (high temperature) and irradiation-enhanced (intermediate temperature) conditions in order to develop a model of the xenon diffusion coefficient based on the atomic scale mechanisms responsible for transport. While the diffusion mechanism for xenon in UO 2 is adequately described by the Xe + U 2 O vacancy cluster for intrinsic conditions, a similar process is not capable of capturing measured in-pile fission gas diffusivity at intermediate temperatures. Therefore, a different diffusion mechanism must dominate under this regime. Using calculated atomistic data, we have shown that irradiation-enhanced diffusion at intermediate temperatures occurs via the larger Xe + U 4 O y vacancy clusters, which have lower migration barriers and increase in concentration by several orders of magnitude compared to intrinsic conditions. This mechanism is enabled by the increased uranium vacancy concentration under irradiation due to Frenkel pair production. In addition, the fast migration of uranium interstitials with two attached oxygen interstitials lowers the total uranium interstitial concentration through reactions with sinks. This allows the extended defects, such as Xe + U 4 O y vacancy clusters, to maintain high concentrations by limiting annihilation with attached vacancies. Furthermore, predictions using the Xe + U 4 O y diffusion mechanism are in good agreement with experiment, albeit with some differences in the Arrhenius slope, which we believe may be related to either experimental or model parameter uncertainty. Lastly, an analytical expression suitable for application in fuel performance simulations was derived to capture the predictions of the Centipede simulations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

AGR-5/6/7 Final Release-to-Birth Ratio Data Analysis

AGR-5/6/7 is the last of a series of Advanced Gas Reactor (AGR) experiments conducted in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) in support of development and qualification of tristructural isotropic (TRISO) low-enriched fuel for use in the high-temperature gas cooled reactor (HTGR). AGR configuration and irradiation conditions are based on prismatic HTGR technology that is distinguished primarily through the use of helium coolant, a low-power-density ceramic core capable of withstanding very high temperatures, and TRISO-coated particle fuel. The AGR tests provide valuable irradiation-performance data to support fuel process development, qualify fuel for normal operation and accident conditions, and support development and validation of fuel performance and fission-product (FP) transport models and codes. Each AGR test consists of multiple independently controlled and monitored capsules containing fuel compacts placed in a graphite cylinder shrouded by a steel shell. Release-to-birth ratios (R/B) for fission-gas isotopes released from each capsule are calculated from release rates, measured by germanium detectors in the Fission Product Monitoring System (FPMS) installed downstream from each capsule, and birth rates calculated using numerical models of FG generation. The R/Bs are a critical measure of the ability of the fuel kernel, the particle coating layers, and the compact matrix to retain fission-gas atoms, preventing their release into the sweep-gas flow, and the impact of initially defective particles and/or particle-coating failures that occur during irradiation. For fission-gas isotopes, particle failure is defined as failure of all coating layers, allowing gaseous fission atoms to escape from a particle. During the first five cycles (162B ? 165A), R/Bs were stable in the 10-8?10-6 range, and no in-pile particle failures were observed, based on the gross gamma counts. The maximum R/B value of around 2 ? 10-6 for Kr-85m resulted from the presence of as-fabricated exposed kernels (based on the high exposed kernel fraction), the dispersed uranium, and high fuel particle temperatures in Capsule 1. Comparison of capsule-measured R/Bs from these early cycles to predictions using the previously developed AGR R/B model demonstrated FG release from the AGR-5/6/7 TRISO fuel was comparable to that of previous experiments. In addition, the Kr-85m R/B per-exposed-kernel values are comparable to R/B values obtained in AGR-3/4 irradiation experiment and four irradiation experiments performed during 1980s: (1) HRB-17/18, (2) COMEDIE-BD1, (3) HFR B1, and (4) HRB-21. In contrast, all measured R/B values are lower than predictions by the commonly used Richards and German models, which are intentionally conservative. A large number of in-pile particle failures occurred in Capsule 1 by the end of Cycle 166A. During the final four cycles (166A ? 168A), apparent damage to the Capsule 1 gas line appeared to cause FG leakage from that capsule into the other four capsules, resulting in an increase in fission gas (FG) detected in the effluent for all capsules. Isolation of the Capsule 1 gas line during the last three cycles also prevented measurement of its FG release. Thus, R/Bs in all capsules after Cycle 166A are highly uncertain because of undefined amount of leakage from Capsule 1, especially for long-lived isotopes. A few hundred in-pile particle failures were estimated for Capsule 1 before the end of Cycle 166A, but the total number of failures is unknown due to the lack of FG release data in the later cycles. Based primarily on evidence from the gross gamma counts during Cycle 168A, approximately 15 particles failed in Capsule 3 and four particles failed in Capsule 2. In-pile failures in Capsule 3 were anticipated because this capsule was designed to operate beyond the HTGR normal operating temperature range. In contrast, no in-pile failures were identified in the top two capsules (4 and 5) based on the absence of the typical spikes in gross gamma counts and low failure estimates using the AGR model, developed in INL/EXT-14-32970, for R/B of the short-lived isotopes (Kr-89 and Xe-137) with minimal leakage from Capsule 1.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗