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At least 19 records

Micro-tensile Properties of Fueled Irradiated AGR-2 TRISO-coated Particle Buffer, IPyC, and SiC Interlayer Regions

Tristructural isotropic (TRISO) coated nuclear fuel particles are proving to be a versatile fuel form for new reactor designs. Understanding the bounding strength and failure mode of each coating interface is important to both fuel quality evaluation and failure prediction. A mechanism of key significance is failure of the silicon carbide (SiC) layer to retain fission products due to incomplete tearing of the buffer layer. This is a two-step mechanism involving both mechanical failure in the buffer and inner pyrolytic carbon (IPyC) layers and degradation of the SiC layer through palladium silicides at the IPyC-SiC interface. However, the mechanical properties of TRISO particle coating layers have yet to be fully characterized due to the small dimension of TRISO fuel particles and high radioactivity. To investigate this mechanism, in situ micro-tensile properties of the buffer, IPyC, SiC, buffer-IPyC, and IPyC-SiC interlayer regions of fueled TRISO particles have been tested at both as-fabricated and irradiated conditions. Determination of the mechanical properties of these TRISO particle regions will lead to a better understanding of the SiC layer failure mechanism and enable progress towards TRISO fuel qualification.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Anisotropic temperature-dependent elastic constants and thermal conductivities of TRISO particle coatings

Tristructural isotropic (TRISO) particles show great promise as a candidate fuel for use in several next-generation high-temperature nuclear reactor designs due to their structural integrity and fuel performance at high temperatures and burnups. Computational codes exist that can simulate TRISO fuel performance characteristics and failure probabilities under extreme conditions which require knowledge of the TRISO coatings’ thermophysical properties. The thermophysical descriptions of the TRISO particle's layers (i.e., buffer, pyrolytic carbon, and silicon carbide) currently used in fuel performance codes, however, assume that many of these properties are constant with respect to temperature or texture. In this paper, we obtain the full elastic stiffness tensors of the carbon and silicon carbide layers, which have transversely isotropic symmetry. Additionally, the calculated elastic properties of each of the coating layers are in remarkable agreement with the current models at room temperature and correct orientations. Additionally, the textured 3C-SiC layer was found to exhibit novel auxetic behavior above 1500 °C. The anisotropic temperature-dependent thermal conductivities of the carbon layers were calculated using acoustical Grüneisen-Debye theory which are in excellent agreement with current models at room temperature and correct orientations. These texture- and temperature-dependent relationships can be incorporated into the thermophysical description of TRISO particles in order to more accurately model fuel performance and failure probabilities under extreme conditions in forthcoming high-fidelity computational simulations.

36 MATERIALS SCIENCE↗

Advanced Electron Microscope and Micro Analysis of TRISO coated Particles: FY2020 Overview

Objectives Understanding Effects of Irradiation on TRISO layers Fission product chemistry and behavior in UCO kernel Identify and Understand Fission Product Transport Mechanisms in TRISO Coated Particles Outcomes and Impact Impact on Performance Improve Predictive Behavior Modeling Kernel Behavior: Release from kernel; release from whole particle Known Fission Product Transport Mechanisms

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Thermal properties measurement of TRISO particle coatings from room temperature to 900 °C using laser-based thermoreflectance methods

The thermal properties of tristructural isotropic (TRISO) particle coatings have been measured using laser-based thermoreflectance methods from room temperature to 900 °C. At room temperature the pyrocarbon coatings have comparable thermal conductivities below 10 W·m -1 ·K -1 , whereas the SiC coating has a thermal conductivity around 90 W·m -1 ·K -1 . The thermal diffusivities of all coatings display significant reduction with increasing temperature. Finally, the thermal conductivity of SiC decreases by more than 25% above 800 °C and the thermal conductivities of pyrocarbons increase moderately with the temperature, displaying similar changes to that of amorphous graphite at elevated temperatures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Electron Microscopic Examination of an Irradiated TRISO Coated Particle of AGR-2 Experiment: AGR2-222-RS019

The transmission electron microscopic (TEM) examination of an irradiated tristructural isotropic (TRISO) coated particle from advanced gas reactor (AGR) 2 fuel Compact 2-2-2 is presented in this report. Compact 2-2-2 refers to the compact in Capsule 2 at Level 2 of Stack 2. The examination on AGR2 222 RS019 is focused on the interface between the silicon carbide (SiC) to inner pyrolytic carbon (IPyC) layer, central part of SiC, and the interface between SiC and outer pyrolytic carbon layer. The SiC grain boundary distribution and associated fission product precipitates were characterized by scanning transmission electron microscopy (STEM) energy dispersive spectroscopy (EDS), and precession electron diffraction (PED) in the transmission electron microscope. Two separate locations on SiC layer were selected for on the basis of the intact of the buffer layer in the irradiated TRISO particle. The key observation in this particle is that the compositional nature of grain boundary precipitates is more complex near IPyC/SiC layer where Pd, Pd-Ag, Pd-U containing precipitates can be observed. However, the compositions of precipitate towards outer most region of SiC mainly contain Pd. Ag has been observed in the IPyC/SiC layer in one of the two locations. Comparison of the results to previously irradiated and analyzed, Variant 3, safety tested AGR-1 TRISO particles (AGR1-433-001 and AGR1 222-RS004) showed the grain boundary distributions have some noticeable differences. The differences in coincident site lattice grain boundary and misorientation angles are possibly inherent to the fabrication process. Neutron irradiation induced void distribution has been found to be nonuniform. A high concentration of smaller voids is found at stacking faults compared to those in the SiC matrix. Larger void sizes are observed in the SiC location that is near to the broken buffer layer. This void size variation with integrity of buffer layer can potentially affect the fission product retention. However, the average void size continuously decreases along the radius of SiC in both locations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effects of Neutron Irradiation on the Micro/Nano Scale Structure and Fission Product Distribution of TRISO Coated Particle Fuel Kernels from AGR Experiments

The Advanced Reactor Technologies (ART) Program at Idaho National Laboratory (INL) includes the Advanced Gas Reactor (AGR) fuel development and qualification program that consists of fuel fabrication, experiment irradiations, post-irradiation examination (PIE) and safety testing to assess tristructural isotropic (TRISO) fuel performance during normal irradiation and under potential accident conditions. Advanced microscopy work on selected AGR-1 and AGR-2 unirradiated and irradiated fuel specimens is performed as part of the PIE effort. PIE work on fuel from the first experiment irradiation, AGR-1, began at INL in April 2010, and AGR-2 PIE began at INL in July 2014. This work scope includes University of Florida (UF) performing advanced electron microscopy examination and analysis using facilities at the Center for Advanced Energy Studies (CAES), INL or UF’s electron microscopy facilities. Electron microscopic examination and analysis may include scanning transmission electron microscopy (STEM), transmission electron microscopy (TEM), selected area diffraction (SAD), electron energy loss spectroscopy (EELS), electron dispersive spectroscopy (EDS) and atom probe tomography (APT) on the fuel kernels of TRISO-coated fuel particles. The electron microscopy lamellae will be provided by INL and will be available at CAES or Irradiated Materials Characterization Laboratory (IMCL).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Microstructural Characterization of AGR-2 TRISO-coated Particle Buffer, IPyC, and Buffer-IPyC Interfaces

Investigating the microstructural, mechanical, and chemical behaviors of Tristructural Isotropic (TRISO) fuel particles is vital for its qualification and use in advanced reactors. Central to the study of TRISO particles is understanding the silicon carbide (SiC) layer's ability to confine fission products, with failure mechanisms linked to chemical degradation following mechanical degradation of the buffer and IPyC layers. Research has been done to quantify the micro-tensile properties of the buffer, inner pyrolytic carbon (IPyC), and buffer-IPyC interlayer regions and their interactions within both irradiated and un-irradiated TRISO particles. Techniques such as atom probe tomography (APT) and transmission electron microscopy (TEM) have also been deployed to examine microstructural defects and fission product distribution in detail. The goal is to understand layer delamination, establish connections between microstructure and mechanical attributes, and inform computational predictions of fuel performance. This work may help refine predictive models of TRISO fuel behavior and facilitating its certification for use in advanced reactors.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Determining the tensile strength of fuel surrogate TRISO-coated particle buffer, IPyC, and buffer-IPyC interlayer regions

A novel micro tensile sample fabrication technique for determining the tensile strength of the buffer, IPyC, and buffer -IPyC interlayer regions of surrogate (ZrO2) TRISO fuel particle layers was refined and implemented. Copper micro tensile samples served as baseline materials to verify the methods used. Tensile tests performed in this study, while limited in number, were analyzed using standard and Weibull statistics. As expected, the buffer layer was weakest, with an average ultimate tensile strength of 138.70 MPa, and the IPyC layer samples, were strongest, with an average ultimate tensile strength of 189.74 MPa. In the buffer -IPyC interface samples, all breaks occurred in the buffer region, though the average ultimate tensile strength of the samples, 159.80 MPa, was between the pure buffer and IPyC samples. These results suggest the interlayer region has unique properties, perhaps associated with pyrocarbon infiltration into the buffer layer during particle coating. All interlayer samples fractured within the buffer side; however, the stress strain behavior of some of these samples resembled the behavior of the IPyC layer samples. Here, the buffer and IPyC layer strengths had a normal distribution under Weibull analysis, while the interlayer region had a Rayleigh distribution. Further testing is needed to clarify both the standard and Weibull statistical results

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Understanding TRISO Coated Particle Neutron Irradiation Behavior:Evolution of Advanced Micro Analysis and Electron Microscopy Approaches

Objectives and motivation• Provide data for fuel qualification in support of reactor licensing• Establish a domestic commercial TRISO fuel fabrication capability Approach • Focus is on developing and testing UCO TRISO fuel –Develop fuel fabrication and QC measurement methods, first at lab scale and then at industrial scale –Perform irradiation testingover a range of conditions (burnup, temperature, fast neutron fluence) –Perform post-irradiation examination and safety testingto demonstrate and understand performance during irradiation and during accident conditions –Develop fuel performance modelsto better predict fuel behavior –Perform fission product transport experiments to improve understanding and refine models of fission product transport

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Micromechanical Properties of the SiC and Pyrolytic Carbon Layers in Tristructural-Isotropic Coated Particles

Tristructural isotropic (TRISO) coated particle fuel was initially developed for high temperature gas cooled reactors (HTGR) and has been proposed for several other advanced reactor concepts. The design of TRISO particles focuses on preventing the release of fission products in normal and off-normal reactor conditions. The particle design features an actinide bearing fuel kernel that is surrounded by three pyrolytic carbon (PyC) layers and a silicon carbide layer (SiC). The mechanical stability of the particle and fission product retention for both metallic and gaseous fission products depend on the SiC layer. Post irradiation examination (PIE) of TRISO fuel from the first two US DOE Advanced Gas Reactor Fuel Development and Qualification Program irradiation campaigns, AGR-1 and AGR-2, had identified a low rate of particles exhibiting cracking in the SiC layer that did not propagate across the SiC layer. While cracking in the SiC is rare for test conditions and particles associated with the AGR program, understanding the stress state and mechanical properties of the SiC and PyC layers related to particle architecture can aid predicting thermomechanical response of TRISO fuel under the prescribed operation envelope and beyond as well as aiding in the development of similar fuel concepts for other advanced reactors. The presented investigation shows the relationship of the mechanical properties and mechanical response (e.g., understanding crack propagation) of the SiC and PyC layers relative to position within the particle. Testing was conducted on the inner and outer PyC layers of TRISO particles to quantify differences in mechanical behavior.

Montoya, Katherine [ORNL] (ORCID:0000000326955086)↗

AGR-3/4 TRISO Fuel Compact Ceramography

The combined third and fourth irradiation in the Advanced Gas Reactor (AGR) program (AGR-3/4) contained tristructural isotropic (TRISO)-coated particle fuel and designed-to-fail (DTF) fuel particles. The DTF particles were only coated with highly anisotropic pyrocarbon (PyC) so they would purposely fail during the AGR-3/4 irradiation and provide a source of fission products for measurement. To observe the post-irradiation morphology of these DTF particles and the TRISO-coated particles, three AGR-3/4 compacts were mounted in epoxy, sectioned above their centerlines, and ground/polished. Three rounds of grinding/polishing and optical microscopy were performed so that the particles could be observed at multiple planes. Each compact contained approximately 1,872 TRISO particles and exactly 20 DTF particles. The three AGR-3/4 compacts examined covered a wide temperature range and featured both the hottest average irradiation temperature (1375°C) and the coldest/lowest burnup (872°C and 5.5% fissions per initial metal atom) of any compacts to undergo post-irradiation examination (PIE) in the AGR program to date. A total of 29 DTF particles were located and observed via microscopy across the three compacts. All the DTF particles observed via microscopy had completely failed PyC coatings. Some different DTF kernel and PyC morphologies were observed that have been attributed to the differences in irradiation temperature and/or burnup. At low and medium irradiation temperatures (roughly 850 to 1050°C), it appears irradiation-induced dimensional changes in the DTF PyC caused it to fracture and fold in on itself, and the kernel deformed to accommodate this PyC deformation. The extent of DTF kernel deformation to accommodate DTF PyC buckling tended to be greater for the medium-temperature fuel compared to the cold fuel. In the high-irradiation-temperature compact (1375°C), the DTF PyC layer appears to have completely reacted chemically with the kernel material. The only material surrounding the DTF particles in this hot compact resembles the compact matrix material. Observations of the TRISO-coated driver fuel particles and fuel compact graphitic matrix were also made. The TRISO particle kernels in the medium-temperature compact (1047°C), and many in the high-temperature compact (1375°C), showed morphologies consistent with what was seen in AGR-1 and AGR-2. In other TRISO particles from the high-temperature compact, a spatial gradient in the kernel appearance was evident. Here the cool side of the kernel (away from the center of the compact) had a much darker appearance (like that of the buffer and pyrocarbon). This is the first observation of this kind of kernel spatial gradient in AGR fuel. It is believed that the high irradiation temperature of that compact (an average of 1375°C) activates or accelerates an unidentified chemical reaction, and the temperature gradient within the fuel causes a sharp spatial gradient. The low-temperature/low-burnup compact also showed unique kernel morphologies where the TRISO-coated particles had clearly distinguishable oxide and carbide phases at the center of the kernel, an oxide rind surrounding this, and remnants of a carbide skin surrounding the oxide rind. These are features observed in the as-fabricated fuel that are no longer present in higher burnup fuel. Occasional gaps between the outer pyrolytic carbon (OPyC) and graphitic matrix material were observed in all compacts. Gaps were most often found in the small, matrix-filled spaces between adjacent particles. Finally, buffer morphologies in AGR-3/4 TRISO particles were like those observed in AGR-1 and AGR-2, and the buffer fracture frequencies in AGR-3/4 and AGR-2 TRISO particles were plotted versus fast neutron fluence and irradiation temperature. In AGR-3/4 the buffer fracture rate was highest (23%) for an irradiation temperature of 1047°C and a fast fluence of 5.18E25 n/m 2 . Increasing the irradiation temperature to 1375°C reduced the buffer fracture rate to 14%. Reducing the irradiation temperature to 872°C and the fast fluence by a factor of 3 reduced the buffer fracture rate to 7%. The temperature and fluence dependencies observed for AGR-3/4 buffer fracture were consistent with those observed in AGR-2. Lower fluences and/or higher temperatures significantly reduced the buffer fracture frequencies. Lower buffer fracture frequencies were also observed at lower temperatures as long as the fluence was also significantly reduced. This is believed to be due to lower fluence resulting in less irradiation-induced dimensional change (shrinkage) of the buffer, and a higher temperature promoting enhanced creep relaxation of stresses within the buffer, leading to less buffer fracture.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

TRISO Fuel’s Safety Functions, Contributions to Reactor Safety, and Necessary Safety Limits

Safety functions are the actions, passive or active, that structures, systems, and components of nuclear facility that contribute to the safety of the workers, the public, or the environment. Well-defined safety functions are the foundation of a solid safety case for a reactor. For reactors that use TRISO-coated particles, the TRISO fuel plays an important part of the safety case because of its ability to contain radionuclides in the fuel itself. This ability enables the use of a functional containment strategy for the reactor where radionuclide retention is the primary safety function supported by the safety functions of controlling reactivity control and controlling heat rejection. This paper establishes at a deeper level the role that TRISO fuel plays in each of these safety functions and associated quality assurance and testing requirements for TRISO particle manufacturing to ensure these safety functions. Safety limits necessary to protect these safety functions include: operational limits, time at temperature limits, and fission gas release activity limits. In conclusion, this approach demonstrates the role that specific aspects of TRISO fuel play in protecting the safety of workers, the public, and the environment.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Safety Testing and Destructive Examination of AGR-2 UO 2 Compact 3-1-1

Post-irradiation examination and elevated-temperature safety testing are being performed on compacts from the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s second irradiation experiment (AGR-2). The compacts in the AGR-2 irradiation experiment held either tristructural isotropic (TRISO)-coated particles containing uranium oxide fuel kernels (UO 2 ) or TRISO-coated particles containing fuel kernels with both uranium carbide and uranium oxide phases (UCO). In UO 2 TRISO particles, oxygen released by uranium fission can react with the surrounding carbon in the buffer layer to form carbon monoxide (CO). Excess CO can lead to various irradiation performance issues under certain operating conditions, such as pressure-induced fracture, kernel migration, and silicon carbide (SiC) corrosion. In UCO TRISO particles, CO formation is reduced because the chemical potential for oxidation of uranium carbide is lower than for oxidation of carbon.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Micromechanical response of SiC-OPyC layers in TRISO fuel particles

Tristructural isotropic (TRISO)–coated particle fuel is a proposed fuel for multiple advanced reactor concepts. The performance of the particle depends on whether the silicon carbide (SiC) layer remains intact to prevent the release of metallic and gaseous fission products. Mechanical fracture of the SiC layer is a potential failure mode under various fuel configurations and operating environments, including the potential transmission of matrix-originating cracks through TRISO particles. Furthermore, this study uses instrumented indentation techniques on cross-sectioned surrogate particles to examine the mechanical stability of the critical interface between SiC and the outer pyrolytic carbon (OPyC) layer. The observed behavior at the interface is rationalized by examining the radially dependent fracture behavior of the SiC layer and performing a numerical analysis to quantify the residual stresses that develop during the processing and cross-sectioning of the as-fabricated particle. Characterizing the SiC-OPyC interface of surrogate TRISO particles using nanoindentation provides unique insight into the interface's room-temperature residual stress and mechanical stability. The modeling efforts were used to investigate the experimental procedure further, and the results are presented herein to validate this fuel form's potential mechanical failure modes.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Experimental validation of the mechanistic scale-up methodology of gas–solid spouted beds using radioactive particle tracking (RPT)

The very high-temperature reactors (VHTRs) are highly ranked among candidates of Generation IV of nuclear reactors due to their high efficiency, safety, the resistance to proliferation, and reliability. The VHTRs are preferentially fueled by Tristructural-isometric (TRISO) coated fuel particles which has fuel kernels of fissile material coated by four coating layers: a porous buffer pyrolysis carbon layer (buffer PyC), an inner dense pyrolysis carbon layer (IPyC), a silicon carbide layer (SiC) and an outer dense pyrolysis carbon layer (OPyC). The heart of the operation and safety of the VHTRs significantly depends on the reliability of the coating layers of TRISO particles to retain metallic and gaseous fission products within the particles. The technique used for coating TRISO particles are gas-solids spouted beds via chemical vapor deposition (CVD). Fabrication of high-quality low-defect TRISO fuel particles fuel at larger scale spouted beds is required to support the commercialization of the VHTRs. In this work, our new developed mechanistic scale-up methodology of gas-solids spouted beds based on matching the radial profile of gas-holdup has been demonstrated and validated using radioactive particle tracking (RPT). Two spouted beds of small and larger scales were used in the study. Three sets of conditions were carried out which include the conditions of the reference case in the large scale, conditions that provide similar gas holdup radial profile to that of the reference case and conditions that provided dissimilar gas holdup radial in the small-scale spouted beds. The results confirm the validation of the scale-up methodology in terms of the dimensionless values of the spout diameter, cumulative probability distribution of the solids particles penetration into the spout, fraction of cycle time in each region of the bed, the radial profiles of the dimensionless values of the root-mean-square particle velocities and solids eddy diffusivity. Finally, the results further advance the knowledge and understanding of the gas-solids spouted beds provide deeper insight into their solids dynamics and presenting important benchmarking data for validating computational fluid dynamics codes and models. At last, procedures are established for the implementation of the new scale-up methodology.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗