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Hurley, David

Publications and source records attributed to Hurley, David.

Accelerated thermal property mapping of TRISO advanced nuclear fuel

TRistructural ISOtropic (TRISO) fuel is a leading-edge nuclear fuel form representing a departure from the more traditional nuclear fuel forms utilized in the reactor fleet of today. Rather than a monolithic fuel pellet of uranium dioxide, integral fuel forms containing TRISO fuel are composed of thousands of microencapsulated uranium-bearing fuel kernels and individually coated with multiple layers of pyrolytic carbon and silicon carbide. These multilayered ceramic coatings serve as an environmental barrier to ensure radioactive and chemically reactive fission products are contained within the reactor fuel elements, but also participate in the transfer of heat generated in the nuclear fuel to the coolant – the primary purpose of a nuclear reactor. Since traditional thermal property measurement techniques, such as laser flash analysis, would be unable to resolve the thermal properties of the individual TRISO coating layers, a simplified frequency-domain thermoreflectance technique has been developed to rapidly map the thermal properties of TRISO particles. Using this technique, the thermal properties of TRISO particles have been mapped from room temperature up to 1000 °C to examine the spatial variation and temperature-dependency of the thermal properties within each layer. Additionally, spatial-domain thermoreflectance was used to examine the anisotropy of the thermal properties for each layer at different locations within a single TRISO particle, and across multiple TRISO particles to assess the intra- and inter-particle uniformity of thermal properties, respectively. To elucidate the underlying causes for the measured variations in thermal properties, scanning electron microscopy and Raman spectroscopy were used to examine variations in microstructure and chemical bonding within the different coating layers. Results from this work are then compared with previous examinations of TRISO fuel particles and microstructurally driven mechanisms for the variations in the measured thermal properties of the different carbonaceous layers are discussed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Microstructure characterization of electric field assisted sintering (EFAS) sintered metallic and ceramic materials using local thermal diffusivity measurement

Electric Field Assisted Sintering (EFAS, also referred to as spark plasma sintering) is a powerful technology for the consolidation of powder materials. The high heating rate during the sintering process is critical for minimizing energy consumption, but it can also cause microstructure heterogeneities in sintered parts, such as spatially varied porosity. The examination of localized porosity usually requires the use of a scanning electron microscope with a carefully prepared surface. In this paper, photothermal radiometry is used to measure local thermal diffusivity and extract localized porosity of EFAS-sintered parts by using a percolation-threshold model. Applying this approach, we identified the radial position-dependent porosity variation in EFAS parts, which is likely formed due to the large temperature gradient during the sintering process. This approach has a unique advantage because it can measure samples with minimal or no surface preparation, enabling the possibility of in situ characterization in EFAS with proper system modification. Necessary modifications on the measurement approach for EFAS deployment and in situ characterization are also discussed.

36 MATERIALS SCIENCE↗

Local measurement of bulk thermal diffusivity using photothermal radiometry

Here, an experimental methodology using photothermal radiometry is developed for the accurate measurement of bulk thermal diffusivity of nuclear fuels and materials irradiated to high doses. Under these conditions, nuclear fuels, such as uranium oxide, and moderator materials, such as graphite, become friable, which requires characterization techniques that can accommodate irregularly shaped fragments. Photothermal radiometry, a good candidate for this application, involves locally heating a sample by using a laser and measuring the temperature field by monitoring blackbody radiation. The interaction volume for this study, less than a millimeter, is carefully chosen to sample a statistically significant number of large-scale structural features, such as pores and gas filled bubbles, and is small enough that the sample fragments can be treated as a thermal half-space. The thermal diffusivity standards considered in this study cover a range of thermal diffusivities representative of both fresh and spent nuclear fuels. We also consider a sample having a porous microstructure representative of large-scale structures found in materials irradiated to high doses. Our measurement methodology circumvents complex thermal wave models that address optical diffraction, nonlinear transfer function associated with blackbody radiation, and finite sample size effects. Consequently, the large measurement uncertainty associated with modeling these effects can be avoided. While the emphasis here is on nuclear fuels and materials, this measurement approach is well suited to measure thermal transport in a variety of technologically important materials associated with advanced synthesis techniques. Examples range from small, exotic single crystals grown using hydrothermal growth techniques to additively manufactured components having complex geometries.

36 MATERIALS SCIENCE↗

Magnetic, transport and thermal properties of δ-phase UZr 2

Here, polycrystals of hexagonal δ-phase UZr 2 have been synthesised and studied by means of heat capacity, magnetic susceptibility, magnetisation, electrical resistivity, magnetoresistance, thermoelectric power, thermal conductivity measurements, for the first time, at temperatures from 1.8 to 300 K and in magnetic fields up to 8 T. The weak temperature dependence of the magnetic susceptibility and the small value of both Seebeck (0.75 μV/K at room temperature) and of the Sommerfeld coefficient (13.5 mJ mol –1 K –2 ) point to 5f-electrons in this material having a delocalised nature. The electrical resistivity and magnetoresistance indicate the presence of significant electronic disorder in δ-UZr 2 , consistent with the disorder in its crystal structure. Density functional theory calculations have been performed and compared to experimental results.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effect of Atmospheric Organics on Bioavailable Fe Lifetime in the Oceans

The deposition of atmospheric aerosols is an important supply pathway of soluble iron (sol-Fe) to the global oceans influencing marine ecosystem processes and climate. Previous studies have shown that natural and anthropogenic acidic trace gases, when mixed with mineral dust, can lead to production of sol-Fe, leading to considerable increase in dust-Fe solubility. Recent studies have further highlighted the importance of atmospheric organic compounds/ligands in the production of sol-Fe during atmospheric transport and transformation of mineral aerosols. However, the actual scope of this aerosol sol-Fe for stimulating the primary productivity in the oceans is determined by both: the total atmospheric fluxes of sol-Fe and the lifetime of sol-Fe after its deposition to the ocean. In this study several atmospheric organic ligands were investigated for their effect on the lifetime of sol-Fe after mixing with seawater. Organic ligands were selected based on their abundance in the marine boundary layer and rainwater and their ability to form bidentate complexes with Fe. The results reveal that the tested organics had minor influence on Fe(II) lifetime in seawater. However, results also show that some organic acid considerably extended the lifetime of colloidal and aqueous Fe(III). Using these results we simulate aerosol sol-Fe lifetime in the ocean for different mineral dust deposition events in the presence and the absence of atmospheric organic ligands. The calculations suggest that when a large dust plume is assumed to contain Fe(II) alone, less than 15% of aerosol sol-Fe gets complexed with marine organic ligands. However, this fraction increases to over 90% when atmospheric Fe is allowed to bond with atmospheric organic acids prior to deposition to the oceans. Calculations also show that for the conditions when seawater organic ligands get titrated by Fe released from dust aerosol particles, retention of sol-Fe in the ocean depends on surface ocean mixing, i.e., replenishing rates for Fe-bonding ligands from below. This study suggests that in future ocean biogeochemistry models more attention should be devoted to better quantification of the role of atmospheric organic acids in the lifetime of aerosol sol-Fe after its deposition to the ocean and the improvements of upper ocean turbulence parameterizations.

Oceans↗