Influence of temperature, oxygen partial pressure, and microstructure on the high-temperature oxidation behavior of the SiC Layer of TRISO particles

Visharad Jalan; Adam Bratten; Meng Shi; Tyler Gerczak; Haiyan Zhao; Jonathan D. Poplawsky; Xiaoqing He; Grant Helmreich; Haiming Wen

doi:10.1016/j.jeurceramsoc.2024.116913

Influence of temperature, oxygen partial pressure, and microstructure on the high-temperature oxidation behavior of the SiC Layer of TRISO particles

Visharad Jalan, Adam Bratten, Meng Shi, Tyler Gerczak, Haiyan Zhao, Jonathan D. Poplawsky, Xiaoqing He, Grant Helmreich, Haiming Wen

Research output: Contribution to journal › Article › peer-review

4 Scopus citations

Abstract

Tristructural isotropic (TRISO)-coated fuel particles are designed for use in high-temperature gas-cooled nuclear reactors, featuring a structural SiC layer that may be exposed to oxygen-rich environments over 1000 °C. Surrogate TRISO particles were tested in 0.2–20 kPa O₂ atmospheres to observe the differences in oxidation behavior. Oxide growth mechanisms remained consistent from 1200–1600 °C for each P_O₂, with activation energies of 228 ± 7 kJ/mol for ₂0 kPa O₂ and 188 ± 8 kJ/mol for 0.2 kPa O₂. At 1600 °C, kinetic analysis revealed a change in oxide growth mechanisms between 0.2 and 6 kPa O₂. In 0.2 kPa O₂, oxidation produced raised oxide nodules on pockets with nanocrystalline SiC. Oxidation mechanisms were determined using Atom probe tomography. Active SiC oxidation occurred in C-rich grain boundaries with low P_O₂, leading to SiO₂ buildup in porous nodules. This phenomenon was not observed at any temperature in 20 kPa O₂ environments.

Original language	English
Article number	116913
Journal	Journal of the European Ceramic Society
Volume	45
Issue number	2
DOIs	https://doi.org/10.1016/j.jeurceramsoc.2024.116913
State	Published - Feb 2025

Funding

The MATLAB script used to measure the oxide thickness in the cross section micrographs was developed by Grant Helmreich at ORNL. This study was financially supported by the Nuclear Energy University Program (award number DE-NE0008753) under the Office of Nuclear Energy of the U.S. Department of Energy. H. M. Wen also acknowledges the U.S. Nuclear Regulatory Commission Faculty Development Program (award number NRC 31310018M0044). SEM, FIB, and STEM work was supported by the University of Missouri Electron Microscopy Core \u201CExcellence in Electron Microscopy\u201D award. APT research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. The authors would like to thank James Burns for assistance in performing APT sample preparation and running the APT experiments. The authors would like to thank Dr. John Hunn and the DOE-NE Advanced Gas Reactor Fuel Development and Qualification Program for fabrication of and providing access to the surrogate TRISO particles.

Keywords

Atom probe tomography
Electron microscopy
Oxidation
Silicon carbide
TRISO particle

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10.1016/j.jeurceramsoc.2024.116913

Cite this

Jalan, V., Bratten, A., Shi, M., Gerczak, T., Zhao, H., Poplawsky, J. D., He, X., Helmreich, G., & Wen, H. (2025). Influence of temperature, oxygen partial pressure, and microstructure on the high-temperature oxidation behavior of the SiC Layer of TRISO particles. Journal of the European Ceramic Society, 45(2), Article 116913. https://doi.org/10.1016/j.jeurceramsoc.2024.116913

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title = "Influence of temperature, oxygen partial pressure, and microstructure on the high-temperature oxidation behavior of the SiC Layer of TRISO particles",

abstract = "Tristructural isotropic (TRISO)-coated fuel particles are designed for use in high-temperature gas-cooled nuclear reactors, featuring a structural SiC layer that may be exposed to oxygen-rich environments over 1000 °C. Surrogate TRISO particles were tested in 0.2–20 kPa O2 atmospheres to observe the differences in oxidation behavior. Oxide growth mechanisms remained consistent from 1200–1600 °C for each PO2, with activation energies of 228 ± 7 kJ/mol for 20 kPa O2 and 188 ± 8 kJ/mol for 0.2 kPa O2. At 1600 °C, kinetic analysis revealed a change in oxide growth mechanisms between 0.2 and 6 kPa O2. In 0.2 kPa O2, oxidation produced raised oxide nodules on pockets with nanocrystalline SiC. Oxidation mechanisms were determined using Atom probe tomography. Active SiC oxidation occurred in C-rich grain boundaries with low PO2, leading to SiO2 buildup in porous nodules. This phenomenon was not observed at any temperature in 20 kPa O2 environments.",

keywords = "Atom probe tomography, Electron microscopy, Oxidation, Silicon carbide, TRISO particle",

author = "Visharad Jalan and Adam Bratten and Meng Shi and Tyler Gerczak and Haiyan Zhao and Poplawsky, \{Jonathan D.\} and Xiaoqing He and Grant Helmreich and Haiming Wen",

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AU - Jalan, Visharad

AU - Bratten, Adam

AU - Shi, Meng

AU - Gerczak, Tyler

AU - Zhao, Haiyan

AU - Poplawsky, Jonathan D.

AU - He, Xiaoqing

AU - Helmreich, Grant

AU - Wen, Haiming

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N2 - Tristructural isotropic (TRISO)-coated fuel particles are designed for use in high-temperature gas-cooled nuclear reactors, featuring a structural SiC layer that may be exposed to oxygen-rich environments over 1000 °C. Surrogate TRISO particles were tested in 0.2–20 kPa O2 atmospheres to observe the differences in oxidation behavior. Oxide growth mechanisms remained consistent from 1200–1600 °C for each PO2, with activation energies of 228 ± 7 kJ/mol for 20 kPa O2 and 188 ± 8 kJ/mol for 0.2 kPa O2. At 1600 °C, kinetic analysis revealed a change in oxide growth mechanisms between 0.2 and 6 kPa O2. In 0.2 kPa O2, oxidation produced raised oxide nodules on pockets with nanocrystalline SiC. Oxidation mechanisms were determined using Atom probe tomography. Active SiC oxidation occurred in C-rich grain boundaries with low PO2, leading to SiO2 buildup in porous nodules. This phenomenon was not observed at any temperature in 20 kPa O2 environments.

AB - Tristructural isotropic (TRISO)-coated fuel particles are designed for use in high-temperature gas-cooled nuclear reactors, featuring a structural SiC layer that may be exposed to oxygen-rich environments over 1000 °C. Surrogate TRISO particles were tested in 0.2–20 kPa O2 atmospheres to observe the differences in oxidation behavior. Oxide growth mechanisms remained consistent from 1200–1600 °C for each PO2, with activation energies of 228 ± 7 kJ/mol for 20 kPa O2 and 188 ± 8 kJ/mol for 0.2 kPa O2. At 1600 °C, kinetic analysis revealed a change in oxide growth mechanisms between 0.2 and 6 kPa O2. In 0.2 kPa O2, oxidation produced raised oxide nodules on pockets with nanocrystalline SiC. Oxidation mechanisms were determined using Atom probe tomography. Active SiC oxidation occurred in C-rich grain boundaries with low PO2, leading to SiO2 buildup in porous nodules. This phenomenon was not observed at any temperature in 20 kPa O2 environments.

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KW - Electron microscopy

KW - Oxidation

KW - Silicon carbide

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Influence of temperature, oxygen partial pressure, and microstructure on the high-temperature oxidation behavior of the SiC Layer of TRISO particles

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