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Lu, Kathy

Publications and source records attributed to Lu, Kathy.

In-situ TEM study of Kr ion irradiation tolerance of SiFeOC nanocomposite

Here, in this work, ion irradiation of polymer derived SiFeOC nanocomposite was carried out using 1.2 MeV Kr ions at room temperature and 600°C. The starting composite was composed of Fe 3 Si, SiC, SiOC, SiO 2 , and graphitic C. In-situ TEM investigations show uniform distribution of nano-crystalline Fe 3 Si and SiC phases in the amorphous SiOC matrix. During ion irradiation, the SiOC bulk microstructure and interfaces between Fe 3 Si or SiC crystallites and the SiOC matrix remain defect-free and demonstrate outstanding ion irradiation resistance. At room temperature, the crystalline domains are stable up to 2 dpa. At 600°C, Fe 3 Si crystallites are more stable than SiC; SiC crystallites are stable up to 4 dpa while the Fe 3 Si crystallites are stable up to 10 dpa. These crystallites also coalescence and amorphize simultaneously during ion irradiation. The exceptional tolerance to defect formation and irradiation of the SiFeOC nanocomposite provides important guidance to developing irradiation resistant fuels for advanced gas cooled reactors.

36 MATERIALS SCIENCE↗

In-situ microstructure observation of oxidized SiC layer in surrogate TRISO fuel particles under krypton ion irradiation

In accidental scenarios of high temperature gas-cooled reactors, both oxidation of and irradiation to the SiC layer in tri-structural-isotropic (TRISO) fuel particles can change the microstructure and integrity of the fuel elements. Here, in the present study, microstructure and defect evolution in the oxidized SiC layer of surrogate TRISO fuel particles under 1.2 MeV krypton ion irradiation was observed by in-situ transmission electron microscopy. The SiC layers oxidized in water vapor at 1200 °C were irradiated azt room temperature and 800 °C and at damage levels of 0.28–11.2 dpa, respectively. SiC and SiO 2 were found to still be in their crystal structures at the damage level of 11.2 dpa at 800 °C, while SiC was observed to have been amorphized at only 0.56 dpa irradiation at room temperature. The defect number density at 800 °C was an order of magnitude lower than that in the sample irradiated at room temperature. Also, crystalline SiO 2 had higher radiation resistance compared to SiC. A defect reaction rate theory was utilized to understand the fundamental defect evolution process and irradiation resistance difference.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effects of processing temperature on the corrosion and tribocorrosion resistance of perhydropolysilazane-derived coatings on AISI 304 steel

Ensuring a highly corrosion and erosion resistant surface is critical to the reliability and structural integrity of steel canisters for long-term nuclear waste storage in corrosive environments. In this work, perhydropolysilazane (PHPS)-derived coating has been successfully applied to enhance the pitting and tribocorrosion resistance of 304 stainless steels in 0.6 M NaCl solution. Two types of coatings were synthesized on the stainless steel substrate by crosslinking PHPS at room temperature or 600 °C, resulting in different mechanical and corrosion performance. Further, Raman spectra revealed that Si-O bonds were generated in the coating crosslinked at room temperature after corrosion, while absent in that pyrolyzed at 600 °C. In tribocorrosion tests, both coatings were protective to the steel substrate, with the protective effect being more pronounced in the 600 °C pyrolyzed coating. Overall, the PHPS-derived coating synthesized at 600 °C exhibited better protection for steel in wear and corrosion coexisting environments than those synthesized at room temperature.

36 MATERIALS SCIENCE↗

Polysiloxane coatings on microspheres based on Multiphase Flow with Interface Exchange-Discrete Element Modelling

Polysiloxane coatings on yttria stabilized zirconia (YSZ) microspheres of 500 μm were simulated in a spout fluidized bed coater using Multiphase Flow with Interface Exchange-Discrete Element Modelling (MFiX-DEM). In this work, two different coater configurations were developed to study the influence of gas velocity and its distribution on particle dynamics. The presence of the Wurster tube not only enhances the distribution but also increases the overall residence time of the particles. Investigations were also carried out with different Wurster tube positions (normal, 10% and 20% lowered from its initial position). Among these, 20% lowered Wurster tube position demonstrated the most effective coating process. The effects of gas inlet pressure on the average gas velocity and the distribution of particles were analyzed. More than 97% of the particles can be retained. The derived results, including average gas velocity, particle retention percentage, and distribution of particles with gas velocity, are being used to guide the experimental work in obtaining defect-free coatings for YSZ microspheres.

36 MATERIALS SCIENCE↗

SiOC coatings on yttria stabilized zirconia microspheres using a fluidized bed coating process

In this study, defect-free SiOC coatings were prepared on yttria stabilized zirconia (YSZ) microspheres by a fluidized bed coating process. Effects of the rheological properties of the coating solution on the coating process were elucidated. An impact regime diagram was constructed, which demonstrated that the coating mechanisms were collision/impact. During the fluidized bed coating, longer spouted time resulted in wider dispersion, longer residence time, and more circulatory motion of particles; the fluid distributed more uniformly throughout the column, as demonstrated in our Multiphase Flow with Interface eXchange (MFiX) simulations. Two-step pyrolysis in Ar achieved complete coating layers, which were comprised of SiOC, SiO 2 , SiC, and graphite. The two stage mass loss during the pyrolysis corresponded to simultaneous reactions due to depolymerization and hydrocarbon loss from 400 to 600°C. Carbon cluster size in the pyrolyzed samples was calculated to be 25 ± 2 Å. In conclusion, this work provides a new method for producing SiOC coatings on micron spheres, with nuclear TRISO fuel particles as the application.

42 ENGINEERING↗

Oxidation behaviors of matrix-grade graphite during water vapor ingress accidents for high temperature gas-cooled reactors

Water ingress into cores of high temperature gas-cooled reactors (HTGRs) can cause serious safety problems in graphitic components, especially for matrix graphite, which is more vulnerable than nuclear graphite. Here in this study, oxidation behaviors of a matrix-grade graphite, ARB-B1, were investigated under simulated water ingress accidental conditions. The oxidation tests were conducted in water vapor/helium mixed atmospheres at elevated temperatures up to 1200 °C. Oxidation rates and activation energy were evaluated by mass loss measurements. The activation energy was 121.5 kJ/mol in the considered temperature range, indicating only one oxidation regime-in-pore diffusion assisted by cracks. The cracks originated from the fabrication process, acting as penetration paths for the oxidant, played an important role in the oxidation behaviors. Ungraphitized binder oxidation occurred at all temperatures, while apparent oxidation of filler particles started from 1100 °C. Moreover, oxidation effects on compressive properties and hardness of the matrix graphite were discussed in terms of oxidized microstructures. This first detailed study on matrix graphite oxidation in water vapor provides important kinetics knowledge and microstructural and mechanical data for accidental scenarios of HTGRs as well as for development of new matrix graphite materials.

36 MATERIALS SCIENCE↗

Water vapor oxidation of SiC layer in surrogate TRISO fuel particles

Under accidental conditions for high temperature gas-cooled reactors (HTGR), the SiC layer in tri-structural-isotropic (TRISO) fuel particles can be exposed to water vapor. In this study, oxidation behaviors of surrogate TRISO fuel particles were investigated in a He-20 vol% water vapor mixed atmosphere at temperatures up to 1600 °C. The growth of the crystalline oxide passivation layer with cracks and pores followed a parabolic law with time, where the maximum was 2.3 μm at 1600 °C. The oxide layer and the SiC surface under the oxide became flattened with increasing temperature, as a function of the silica viscosity and the diffusion path of water vapor. Volatilization of the oxide layer was analyzed using a mechanistic model that an inert gas in oxidizing atmospheres could influence the magnitude of volatilization. The fracture load and strength of the oxidized and thinned SiC layer were numerically estimated to decrease from 2.27 to 1.69 N and from 317 to 299 MPa, respectively, with the SiC thickness decrease from 35 to 32 μm. This prediction indicates that the oxidized SiC layer should retain fission products. Additionally, the mechanical integrity of each layer in the TRISO fuel particle after oxidation was evaluated. The results in this work provide important data for the safety analysis of accidental scenarios in HTGRs.

36 MATERIALS SCIENCE↗

Microstructural evolution of a silicon carbide-carbon coated nanostructured ferritic alloy composite during in-situ Kr ion irradiation at 300°C 450°C

This work focuses on irradiation behaviors of a novel silicon carbide and carbon coated nanostructured ferritic alloy (SiC-C@NFA) composite for potential applications as a cladding and structural material for next generation nuclear reactors. The SiC-C@NFA samples were irradiated with 1 MeV Kr ions up to 10 dpa at 300 and 450 °C. Microstructures and defect evolution were studied in-situ at the IVEM-Tandem facility at Argonne National Laboratory. The effects of ion irradiation on various phases such as α-ferrite matrix, (Fe,Cr) 7 C 3 , and (Ti,W)C precipitates were evaluated. The α-ferrite matrix showed a continuous increase in dislocation density along with spatial ordering of dislocation loops (or loop strings) at >5 dpa. The size of the dislocation loops at 450 °C was larger than that at 300 °C. The nucleation and growth of new (Ti,W)C precipitates in α-ferrite grains were enhanced with the ion dose at 450 °C. This study provides new insight into the irradiation resistance of the SiC-C@NFA system.

(FeCr)(7)C-3↗

Effects of transition metals on the evolution of polymer-derived SiOC ceramics

This work focuses on catalytic graphitization from different metals, iron (Fe), cobalt (Co), and nickel (Ni), for inducing carbon growth in silicon oxycarbides (SiOCs) during the pyrolysis. Fe, Co, and Ni-modified SiOCs were synthesized by pyrolysis to 900, 1100, and 1300 °C respectively in Ar. The transition metals induced the formation of the corresponding metal silicides, β-SiC, and graphitic carbon with the catalytic activity in the order of Fe > Co > Ni, in agreement with the activation energy calculation based on the carbon types and amounts. Lateral growth of turbostratic carbon followed a 2D grain growth process and its point-like defect density decreased based on the catalytic order of the transition metals, with SiOC/Fe having the lowest defect density. Quantitative analysis of the XPS results with Rietveld refinement illustrated that the phase separation of SiOC is more dominant than local carbothermal reduction between SiO 2 and C in the SiOC/M (M = Ni, Co, or Fe) systems. Understanding the catalytic graphitization effect of Ni, Co, and Fe on polymer derived ceramics offers new strategies in increasing high-temperature phase amounts and thus creating novel materials for heterogeneous catalysis, magnetic, and other applications.

36 MATERIALS SCIENCE↗

High temperature oxidation behaviors of bulk SiC with low partial pressures of air and water vapor in argon

Oxidation behaviors of bulk SiC at 1000–1400 °C in Ar-20 vol% H 2 O-10 vol% air were investigated. The thickness of the passivation oxide layer showed a parabolic increase with time. Dense and uniform layers formed below 1200 °C, whereas pores and cracks were observed at higher temperatures. An analytical model was proposed to estimate the oxide layer growth and SiC mass loss rate. The SiC layer should be effective in retaining the fission products after oxidation by excessive water and air. This work is the first detailed study of SiC layer oxidation during loss of coolant accidents (LOCA) for HTGRs.

36 MATERIALS SCIENCE↗

Water vapor oxidation behaviors of nuclear graphite IG-110 for a postulated accident scenario in high temperature gas-cooled reactors

Water leakage in accidental conditions of high temperature gas-cooled reactors is one of the most critical problems that can compromise the integrity of different nuclear components. In this study, oxidation behaviors of nuclear graphite IG-110 in water ingress accidental conditions were investigated. Mass loss and oxidation rates were evaluated after oxidation tests at temperatures up to 1400 °C in an Ar-20 vol% H 2 O mixed atmosphere. The activation energy decreased from 318.6 to 148.9 kJ/mol with temperature, indicating two different oxidation regimes. The cross-sections of the oxidized samples were systematically characterized. The corresponding logarithmic porosity profiles showed a temperature dependency. Pore formation moved toward near-surface regions with increasing temperature and preferential binder oxidation, with filler particle degradation. Furthermore, oxidant concentration profiles and oxidation depths were estimated using a theoretical model and compared with the experimental results. This work provides important benchmark data and safety analysis guidance for the accident scenario in high temperature gas-cooled reactors.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗