In-Situ TEM study of microstructural evolution in proton irradiated single crystal UO2 under high-temperature annealing
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Microcrystalline CeO 2 , ThO 2 , and UO 2 were irradiated with 198 MeV 132 Xe ions to the same fluence at temperatures ranging from 25°C to 700°C then characterized by synchrotron X-ray diffraction and X-ray absorption spectroscopy. All samples retain crystallinity and their nominal fluorite-type phase at a fluence of 1.5x10 13 ions/cm 2 . Both CeO 2 and ThO 2 display defect-induced unit cell expansion after irradiation at room temperature (~0.15% and ~0.10%, respectively), yet as irradiation temperature increases, the maximum swelling produced decreases to ~0.02%. Alternatively, UO 2 shows an initial contraction in unit cell parameter (approximately -0.05%), for room temperature irradiation most likely related to irradiation-enhanced annealing or irradiation-induced oxidation. At higher temperatures (above 200°C), UO 2 begins to swell, surpassing its unit cell parameter prior to irradiation (~0.05%), an effect which could be attributed to minor reduction in uranium oxidation state in vacuum. However, while CeO 2 irradiated at room temperature undergoes partial reduction, both UO 2 and ThO 2 exhibit no measurable change in cation oxidation state as evidenced by X-ray absorption spectroscopy. All samples display a decrease in irradiation-induced heterogeneous microstrain as a function of increasing irradiation temperature.
Slides for presentation at AFC review meeting 12/14/21
Here, the use of fluorination as a rapid separation technique for quantification of trace-mass, short-lived isotopes is illustrated. Single crystal 238 UO 2 was exposed to a 14 MeV neutron source to produce mixed fission and activation products. Selective removal of trace volatile fluorides from non-volatile ones produced two results of interest. A decrease in background produced better detection and quantification of select analytes across the gamma spectrum. Second, at the very low burnup condition described, the volatility behaviors of common isotopes were altered relative to their well-established behaviors in higher burnup metal and metal oxide fuels.
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Analysis of fission gas bubbles (FGBs) in light-water reactor (LWR) fuel is needed to improve the understanding and predictive capability of fuel evolution under normal- and transient conditions. One of the most important parameters of a FGB is the pressure of the gas, primarily Xe, inside it. Bubble volume and location (inter- vs. intragranular) are important considerations as well. However, experimental analysis of such bubbles is challenging due to their small size and embedded nature, and usefulness of the data requires large numbers be analyzed. This paper proposes a method to measure the pressure of Xe bubbles using X-ray spectrum imaging (XSI) in scanning transmission electron microscopy (STEM). From X-ray generation and instrumental parameters, the number of Xe atoms yielding a given number of Xe L-series X-ray counts is estimated, and then from the estimated volume of the bubble the Xe density is estimated, which can then be converted to pressure via an equation-of-state. We apply the method to XSI datasets from high burnup (HBu) fuel from North Anna 1 reactor in as-irradiated and post-LOCA-test conditions and find Xe pressures in the FGBs clustered around 1 GPa.