Adam Bratten

Tristructural isotropic (TRISO) fuel particles, developed for use in high‐temperature gas‐cooled nuclear reactors, can be subjected to oxidizing environments in off‐normal accident scenarios. In this study, surrogate TRISO fuel particles were oxidized at 1000–1350°C for 4 h in 20 kPa water vapor atmosphere balanced with ultrahigh‐purity helium gas. The oxide scale morphology and thickness were studied via scanning electron microscopy, focused ion beam, and transmission electron microscopy. The oxide thickness increased as the oxidation temperature was increased. Although the oxide scale at 1000°C was completely amorphous, pockets of crystalline oxide were observed on particles oxidized at 1200 and 1300°C. Kinetic analysis was performed to deduce the oxidation mechanism by determining the apparent activation energy using linear regression analysis. The oxidation mechanism was consistent for temperatures from 1000 to 1200°C with an activation energy of 412.4 ± 8.8 kJ/mol. The activation energy then dropped to approximately 201 ± 7.1 kJ/mol for temperatures 1200–1350°C. Therefore, there is a change in oxidation mechanism at ∼1200°C. This change is attributed to the existence of a network of significant bubbles in the oxide layer at higher temperatures, which serve as rapid diffusion pathways for the transport of oxidants from the surface to the SiC/SiO₂ interface, instead of relying on the bulk diffusion through the SiO₂ layer at lower temperatures where only small bubbles are present along the SiC/SiO₂ interface.

A novel additive manufacturing approach is herein reported for manufacturing high mechanical strength continuous carbon fiber‐reinforced silicon carbide (C_f/SiC) composite materials. Continuous carbon fibers were coated with polycarbosilane (PCS) using a colloidal evaporative deposition process and then coextruded with high solid content SiC ink. The zeta potential of the SiC ink was adjusted to optimize the printing ability of the suspension. During sintering, small SiC grains and whiskers were generated in the gaps in and around the PCS‐coated carbon fibers, which led to the improved flexural strength and density of the composites. Meanwhile, the PCS coating on the surface of the carbon fibers prevented the carbon fibers from reacting with SiO gas generated by reactions between the SiC matrix and SiO₂ and sintering additives (Al₂O₃ and Y₂O₃), effectively preserving the structural integrity of the carbon fibers. Compared to the SiC specimens containing uncoated carbon fibers, the density of the specimens fabricated with coated carbon fibers was increased from 2.51 to 2.85 g/cm³, and the strength was increased from 190 to 232 MPa.

Surrogate tristructural‐isotropic (TRISO)‐coated fuel particles were oxidized in 0.2 kPa O₂at 1200–1600°C to examine the behavior of the SiC layer and understand the mechanisms. The thickness and microstructure of the resultant SiO₂layers were analyzed using scanning electron microscopy, focused ion beam, and transmission electron microscopy. The majority of the surface comprised smooth, amorphous SiO₂with a constant thickness indicative of passive oxidation. The apparent activation energy for oxide growth was 188 ± 8 kJ/mol and consistent across all temperatures in 0.2 kPa O₂. The relationship between activation energy and oxidation mechanism is discussed. Raised nodules of porous, crystalline SiO₂were dispersed across the surface, suggesting that active oxidation and redeposition occurred in those locations. These nodules were correlated with clusters of nanocrystalline SiC grains, which may facilitate active oxidation. These findings suggest that microstructural inhomogeneities such as irregular grain size influence the oxidation response of the SiC layer of TRISO particles and may influence their accident tolerance.

The oxidation behavior of matrix‐grade graphite in air‐ or steam‐ingress accident scenarios is of great interest for high‐temperature gas reactors (HTGRs). In this study, the microstructures of two variants of matrix‐grade graphite based on the German A3‐3 and A3‐27 formulations were characterized with scanning electron microscopy (SEM), transmission electron microscopy (TEM), and Raman spectroscopy, and correlated to oxidation behavior observed through thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). Through TEM imaging and selected area electron diffraction (SAED), a higher volume fraction of partially graphitized carbon was identified in the A3‐3 type graphite than in the A3‐27 type. This structure is believed to have contributed to the accelerated oxidation exhibited by A3‐3 in the chemical reaction‐controlled oxidation regime.