Fabrication and Characterization of Driver Fuel Particles, Designed-to-Fail Fuel Particles, and Fuel Compacts for the US AGR-3/4 Irradiation Test
Explore the source record for details and available documents.
SEARCH · Search NASA
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Explore the source record for details and available documents.
The second Advanced Gas Reactor irradiation (AGR-2) featured UCO tristructural isotropic (TRISO)-coated particle fuel and, for comparison purposes, UO2 TRISO fuel. Particles from three UCO fuel compacts and one UO2 fuel compact were chosen for analysis of kernel swelling and buffer shrinkage. Both kernel swelling and buffer shrinkage are common elements of TRISO fuel performance models. More recently, the AGR program has determined that buffer shrinkage may impact the integrity of the inner pyrolytic carbon (IPyC) layer, which may impact SiC layer integrity (particularly during high-temperature heating tests). Therefore, measurements of buffer irradiation-induced shrinkage may be useful in improving existing models and developing new models that capture buffer-IPyC-SiC-fission product interactions observed in recent AGR post-irradiation examination (PIE). TRISO particles were mounted in epoxy, ground, polished, and imaged via optical microscopy in four separate iterations. Each of the four iterations revealed progressively deeper cross sections within the particles. Images collected from each iteration were analyzed for the circumferences/radii of the kernel, buffer, IPyC, and SiC. Spheres were fit to each set of measurements to generate spherical radii representative of the components of the fuel particle. From these radii, volumes were computed and compared to the as-fabricated volumes. UCO kernel swelling was similar among the three AGR-2 compacts ranging from approximately 28 to 32%. This is only slightly higher swelling than was measured in an earlier study of an AGR-1 compact. However, the burnup at which this swelling occurred in AGR-2 was lower than in AGR-1, indicating a faster swelling rate for the AGR-2 kernels for the irradiation conditions covered by these compacts. The AGR-2 UO2 kernel swelling was less, at 9.9%, comparable to other studies of UO2 kernel swelling. While AGR-2 UCO and UO2 kernels demonstrated different rates of swelling, the extent of buffer shrinkage was similar among the two fuel types, ranging from 24-28%. For comparison, a prior study showed that AGR-1 Compact 1-3-1 experienced 39% buffer shrinkage. A commonly-observed post-irradiation particle morphology is where the buffer pulls away from the IPyC (at least in some regions of the particle). Besides the possibility of the buffer degrading the IPyC when it pulls away from the IPyC, this gap is significant because it may also reduce heat transfer within the particle. Average AGR-2 buffer-IPyC gaps were similar for the UCO and UO2 particles, ranging from 22.2 to 26.0 µm. This is similar to what was measured for AGR-1 Compact 1-3-1.
PARFUME is an advanced gas-cooled reactor fuel performance modeling and analysis code. It has been developed as an integrated mechanistic code that evaluates the thermal, mechanical, and physio-chemical behavior of fuel particles during irradiation and postulated accident conditions to determine the failure probability of a population of fuel particles given the particle-to-particle statistical variations in physical dimensions and material properties that arise from the fuel fabrication process, accounting for all viable mechanisms that can lead to particle failure. The code also determines the diffusion of fission products from the fuel through the particle coating layers, and through the fuel matrix to the coolant boundary. The subsequent release of fission products is calculated at the fuel element level (release of fission products from the compact or pebble). PARFUME calculates the release fraction as the ratio of the number of atoms released from the fuel element to the amount.
Tristructural isotropic (TRISO) coated particle fuel is a promising fuel form for advanced reactor concepts such as high temperature gas-cooled reactors (HTGR) and is being developed domestically under the US Department of Energy’s Nuclear Reactor Technologies Initiative in support of Advanced Reactor Technologies. The fuel development and qualification plan includes a series of fuel irradiations to demonstrate fuel performance from the laboratory to commercial scale. The first irradiation campaign, AGR-1, included four separate TRISO fuel variants composed of multiple, laboratory-scale coater batches. The second irradiation campaign, AGR-2, included TRISO fuel particles fabricated by BWX Technologies with a larger coater representative of an industrial-scale system. The SiC layers of as-fabricated particles from the AGR-1 and AGR-2 irradiation campaigns have been investigated by electron backscatter diffraction (EBSD) to provide key information about the microstructural features relevant to fuel performance. The results of a comprehensive study of multiple particles from all constituent batches are reported. The observations indicate that there were microstructural differences between variants and among constituent batches in a single variant. Finally, insights on the influence of microstructure on the effective diffusivity of key fission products in the SiC layer are also discussed.
Coated particle fuels, such as the tristructural isotropic (TRISO) fuel particle, have been studied and developed for decades for high-temperature gas reactor (HTGR) applications because of their efficiency and relative stability under off-normal conditions. Critical to this development is a strong understanding of the relationship between fuel fabrication, properties and performance, as is how the former can be adjusted and improved to optimize the latter. Accordingly, wide-scale implementation of coated nuclear particle fuels requires thorough and robust quality assurance/quality control (QA/QC) methods for fabrication, characterization, and deployment
Tristructural isotropic (TRISO) coated particle fuel as a key fuel concept for the High Temperature Gas-cooled Reactors (HTGRs) and a candidate accident tolerant fuel (ATF) has been currently investigated under the US-DOE Advanced Gas Reactor (AGR) fuel development and qualification program. Over the past decades, extensive studies have been conducted to evaluate the fission product release, diffusion on Ag, Pd and Cd in the SiC layer and the TRISO coating system, and post-safety-test performance. However, to date, there are limited reported results on the fuel kernels’ response to irradiation with or without post irradiation high temperature annealing. To incrementally fulfill this knowledge gap extensive studies using transmission electron microscopes (TEM) and atom probe tomography (APT) were conducted on a TRISO fuel particle kernel with a 19.74% 235U enrichment, irradiated to 18.63% FIMA and subsequently subjected to post-safety testing at 1600ºC for 300 hours.. Microstructure characterizations, elemental analysis, and phase identification were conducted using conventional TEM and scanning TEM (STEM) imaging, energy-dispersive X-ray spectroscopy (EDS), selected-area electron diffraction (SAED) and atom probe tomography (APT). The following findings were made: (1) significant reconstructions and phase evolutions occurred in the irradiated and post-safety annealed fuel kernel, and its microstructure consists of two primary phases, namely a “high-Z (atomic mass)” UC phase and a “low-Z” UO phase, (2) no fission gas bubbles are identified within the fuel kernel, that can be attributed to the high temperature post safety annealing, (3) fission products Zr, Nb, Mo, Ru, Tc and Rh were found to preferentially segregate into UC phase or to form metallic precipitates, while the lanthanide fission products tend to stay in the solution of UO phase, (4) Pd was detected in the rod-shaped precipitates, (5) APT data reveals segregation of Te, Pd, and Ag at the UO and UC phase boundary, and (6) Pd is detected in both the UO and UC phases but with an enrichment in the former one.
Tristructural isotropic (TRISO) particles are considered as advanced fuel forms for a variety of fission platforms. While these fuel structures have been tested and deployed in reactors, the mechanical properties of these structures as a function of production parameters need to be investigated in order to ensure their reliability during service. Nanoindentation techniques, indentation crack testing, and half sphere crush testing were utilized in order to evaluate the integrity of the SiC coating layer that is meant to prevent fission product release in the coated particle fuel form. The results are complimented by scanning electron microscopy (SEM) of the grain structure that is subject to change as a function of processing parameters and can alter the mechanical properties such as hardness, elastic modulus, fracture toughness and fracture strength. Through utilization of these advanced techniques, subtle differences in mechanical properties that can be important for in-pile fuel performance can be distinguished and optimized in iteration with processing science of coated fuel particle production.
Particle fuel forms generally consist of a dispersion of fuel, such as tristructural isotropic (TRISO) particles, within a refractory matrix (e.g., graphite or silicon carbide). The density of matrix materials for particle fuel forms is of interest for modeling fuel form strength and thermal properties and may be specified as a quality control parameter, depending on reactor design. Some of the uncertainty associated with traditional, manual approaches can be eliminated by performing x-ray computed tomography (XCT) on the fuel forms and applying image processing methods to generate a precise count of the number of particles. This also removes the need to include determination of particle count within each individual fuel form during fabrication. Unfortunately, reconstruction artifacts from high-Z uranium-bearing kernels prevent accurate measurement of individual particle volumes using this approach, so the use of mean particle mass and volume are still necessary for computation of average fuel form matrix density. This method of using XCT to count particles in individual fuel form for determination of average matrix density was applied to three archived compacts from the Advanced Gas Reactor Fuel Development and Qualification (AGR)-1 campaign, four archived compacts with uranium carbide/uranium oxide (UCO) TRISO from the AGR-2 campaign, and three archived UO 2 -TRISO compacts from the AGR-2 campaign. The resulting density values were compared with those previously reported, showing slight changes due to uncertainties in the previously used number of particles in each of these cylindrical, graphite matrix compacts.
The AGR-1 experiment involved irradiation of 72 TRISO-coated particle fuel compacts to a peak compact-average burnup of 19.5% FIMA with no in-pile failures observed out of 3 x 105 total particles. Irradiated AGR-1 fuel compacts have been cross-sectioned and analyzed with optical microscopy to characterize kernel, buffer, and coating behavior. Six compacts have been examined, spanning a range of irradiation conditions (burnup, fast fluence, and irradiation temperature) and including all four TRISO coating variations irradiated in the AGR-1 experiment. The cylindrical specimens were sectioned both transversely and longitudinally, then polished to expose from 36 to 79 individual particles near midplane on each mount. The analysis focused primarily on kernel swelling and porosity, buffer densification and fracturing, buffer–IPyC debonding, and fractures in the IPyC and SiC layers. Characteristic morphologies have been identified, 981 particles have been classified, and spatial distributions of particle types have been mapped. No significant spatial patterns were discovered in these cross sections. However, some trends were found between morphological types and certain behavioral aspects. Buffer fractures were found in 23% of the particles, and these fractures often resulted in unconstrained kernel protrusion into the open cavities. Fractured buffers and buffers that stayed bonded to IPyC layers appear related to larger pore size in kernels. Buffer–IPyC interface integrity evidently factored into initiation of rare IPyC fractures. Fractures through part of the SiC layer were found in only four classified particles, all in conjunction with IPyC–SiC debonding. Compiled results suggest that the deliberate coating fabrication variations influenced the frequencies of IPyC fractures and IPyC–SiC debonds.
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.
Abstract not provided
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).
Generation of pressure wave by explosion of condensed phase fuel particles dispersed in gaseous oxidizer
Dynamic properties of explosion in medium consisting of condensed phase fuel particles dispersed in gaseous oxidizer
Generation of pressure wave by explosion of condensed phase fuel particles dispersed in gaseous oxidizer
During High Temperature Gas-cooled Reactor (HTGR) operation, tristructural isotropic (TRISO) coated-particle fuel undergoes irradiation-induced changes in morphology and thermomechanical properties. Experimental results from the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program show, among other things, the mechanism of gap formation between the buffer and inner pyrolytic carbon (IPyC) layers, which could be explored further via computational simulations using the Bison code. Two simulation models were developed, the debonding restricted model, where no gap formation between buffer and IPyC layers is permitted, and the debonding enabled model, where the gap between those layers is created. The inputs of the simulated models are based on the irradiation conditions from the AGR-1 experiment. The research included simulations on spherical and aspherical fuel types. Under the specific temperatures and fluences of the AGR-1 irradiation experiment, and the Bison simulations, it was concluded that the most common scenario is a gap formation along the buffer-IPyC interface, while the least possible scenario is the situation where there is no gap formation at the buffer-IPyC junction. The computational results confirmed that the sphericity of the fuel influences the thickness of the gap that occurs at the buffer-IPyC junction, in a way that with increasing aspect ratio the gap thickness increases. The results obtained for spherical and aspherical fuel are nearly identical. Finally, performed simulations match conclusions observed from the AGR-1 experiment, which as such shows that the Bison code is a good computational method for simulating the TRISO fuel. Future simulations will include the validation of performed research and comparison of the results between Bison and PARFUME codes.
In the AGR-1 irradiation experiment, 72 coated-particle fuel compacts were taken to a peak burnup of 19.5% fissions per initial metal atom with no in-pile failures. This paper discusses the first post-irradiation test of these mixed uranium oxide/uranium carbide fuel compacts at elevated temperature to examine the fuel performance under a simulated depressurized conduction cooldown event. A compact was heated for 400 h at 1600 degrees C. Release of 85Kr was monitored throughout the furnace test as an indicator of coating failure, while other fission product releases from the compact were periodically measured by capturing them on exchangeable, water-cooled deposition cups. No coating failure was detected during the furnace test, and this result was verified by subsequent electrolytic deconsolidation and acid leaching of the compact, which showed that all SiC layers were still intact. However, the deposition cups recovered significant quantities of silver, europium, and strontium. Based on comparison of calculated compact inventories at the end of irradiation versus analysis of these fission products released to the deposition cups and furnace internals, the minimum estimated fractional losses from the compact during the furnace test were 1.9 x 10-2 for silver, 1.4 x 10-3 for europium, and 1.1 x 10-5 for strontium. Other post-irradiation examination of AGR-1 compacts indicates that similar fractions of europium and silver may have already been released by the intact coated particles during irradiation, and it is therefore likely that the detected fission products released from the compact in this 1600 degrees C furnace test were from residual fission products in the matrix. Gamma analysis of coated particles deconsolidated from the compact after the heating test revealed that silver content within each particle varied considerably; a result that is probably not related to the furnace test, because it has also been observed in other as-irradiated AGR-1 compacts. X-ray imaging of selected particles was performed to examine the internal microstructure. This examination revealed variable irradiation performance of the coating layers, but sufficient statistical sampling is not yet available to identify any possible correlation to variation in individual particle fission product retention.
The structure and speciation of fission products within the SiC barrier layer of tristructural-isotropic (TRISO) fuel particles irradiated to 19.6% fissions per initial metal atom (FIMA) burnup in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) was investigated. As-irradiated fuel particles, as well as those subjected to simulated accident scenarios, were examined. The TRISO particles were characterized using synchrotron X-ray absorption fine-structure spectroscopy (XAFS) at the Materials Research Collaborative Access Team (MRCAT) beamline at the Advanced Photon Source. The TRISO particles were produced at Oak Ridge National Laboratory under the Advanced Gas Reactor Fuel Development and Qualification Program and sent to the ATR for irradiation. XAFS measurements on the palladium and silver K-edges were collected using the MRCAT undulator beamline. Analysis of the Pd edge indicated the formation of palladium silicides of the form Pd x Si (2 ≤ x ≤ 3). In contrast, Ag was found to be metallic within the SiC shell safety tested to 1700 °C. To the best of our knowledge, this is the first result demonstrating metallic bonding of silver from fissioned samples. Knowledge of these reaction pathways will allow for better simulations of radionuclide transport in the various coating layers of TRISO fuels for next generation nuclear reactors. In conclusion, they may also suggest different ways to modify TRISO particles to improve their fuel performance and to mitigate potential fission product release under both normal operation and accident conditions.