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At least 19 records

Hydrogen effects on thermal diffusivity and electrical resistivity of zircaloy cladding

Thermal diffusivity measurements on Zirconium-based cladding materials have historically been a challenge due to the difficulty to measure on specimens with curved geometries, including nuclear grade Zircaloy cladding materials. Here, in this work, we first used laser flash analysis method and four-probe configuration method to measure the thermal diffusivity and electrical resistivity of Zircaloy tubes respectively, which show good agreement with Zircaloy plates in this work, as well as previously published data. The consistent results proved the applicability of the laser flash analysis setup and four-probe configuration method for investigating thermal diffusivity and electrical resistivity of Zircaloy tubes. We further investigated the hydrogen effect on thermal diffusivity and electrical resistivity of Zircaloy. Hydrogen plays significant roles in the thermal diffusivity of Zircaloy, which depends on the hydrogen concentration. For higher hydrogen contents (1130 and 1820 wppm in this work), where phase transformation (α-Zr + δ-hydride → α-Zr + β-Zr) occurs at 567 °C, thermal diffusivity decreases as a function of temperature at the α-Zr + δ-hydride phase regime, while increase at higher temperature at the α-Zr + β-Zr phase regime. For low hydrogen concentration, where hydride dissolved into α-Zr matrix phase at higher temperature, the thermal diffusivity is lower than non-hydrided Zircaloy-4 with similar temperature-dependent trends. Such observation demonstrates the hydrogen effects on reducing thermal diffusivity of α-Zr phase. Hydrogen increases the electrical resistivity of Zircaloy. Similar to thermal diffusivity results, the phase transformation causes a reversal of temperature-dependent trends in electrical resistivity results in Zircaloy-4 with higher hydrogen contents.

36 MATERIALS SCIENCE↗

Report summarizing demonstration of thermal conductivity measurement methods for coated zirconium cladding

Thermal diffusivity measurements on Zirconium-based cladding materials have historically been a challenge due to the difficulty to measure on specimens with curved geometries, including nuclear grade Zircaloy cladding materials. In this work, we first used Laser Flash Analysis methods to measure the thermal diffusivity of Zircaloy tubes, which show good agreement with Zircaloy plates in this work, as well as previously published data. The consistent results proved the applicability of the Laser Flash Analysis setup for investigating thermal diffusivity of Zircaloy tubes. We further investigate the hydrogen effect on thermal diffusivity of Zircaloy tubes. Hydrogen plays significant roles in temperature dependent thermal diffusivity trends of Zircaloy tube. For low hydrogen concentration, where hydride dissolved into single phase α-Zr at higher temperature, thermal diffusivity is relatively unchanged at low temperature at two phase regions (α-Zr and δ-hydride), and it increases as a function of temperature at single phase α-Zr region. For high hydrogen concentration, where phase transformation (α-Zr + δ-hydride → α-Zr + β-Zr) occurs at 567 °C, thermal diffusivity decreases as a function of temperature below 567 °C before the transformation (α-Zr and δ-hydride), while increase at higher temperature after the transformation (α-Zr and β-Zr).

36 MATERIALS SCIENCE↗

A model to separate conduction and radiation in high temperature laser flash measurements for semi-transparent materials

Laser flash analysis (LFA) is a widely used technique in the scientific and industrial communities for measuring the thermal diffusivity and conductivity of materials. However, traditional fitting methods based solely on heat conduction do not account for radiation heat transfer in transparent and semi-transparent materials, which becomes significant at high temperatures. In this study, we have developed a coupled radiation-conduction model that considers the optical properties of materials to accurately extract thermal diffusivity from LFA measurements. We conducted LFA measurements on fused silica glass samples of varying thicknesses and within the temperature range of 25 to 1000 °C and fitted the data with the model. Since the coupled model requires optical properties as input parameters, which are often unavailable for new materials, we have also proposed a modified transparent model. Compared to the coupled model, results from the modified transparent model generally overestimate thermal conductivity, but the errors are acceptable in silica glass with small thickness. Here, we also investigated the applicability of the modified transparent model with materials of different optical properties.

14 SOLAR ENERGY↗

Fabrication and thermophysical properties of UO 2 -UB 2 and UO 2 -UB 4 composites sintered via spark plasma sintering

Uranium dioxide (UO 2 ) composites with uranium diboride (UB 2 ) and uranium tetraboride (UB 4 ) have been proposed as advanced fuel candidates due to their high thermal conductivity, high melting point, high fissile density and their ability to incorporate a built-in burnable poison by tailoring the targeted 10 B/ 11 B ratio. As such, it is important to assess the fabrication, and thermal and micromechanical properties of such composites. In this work, UO 2 -UB 2 and UO 2 -UB 4 samples with boride phase fractions of 5, 15 and 30 wt% were fabricated to high densities (above 95 % theoretical density) via spark plasma sintering (SPS). This enabled sintering at relatively low temperatures and short timescales. SPS also aided in maintaining the target phase fractions of the samples as reactions between the constituent phases were suppressed due to the short timescales and reducing environment during sintering. Here, thermal diffusivity measurements from 299 to 1273 K were conducted through laser flash analysis (LFA). The diffusivity increased as a function of boride weight fraction, and UB 2 additions increased the thermal diffusivity of the composites more than UB 4 additions. Assessment of the LFA results indicated in-situ reactions between the UO 2 and boride phases that suppress the thermal diffusivity occur above 800 K for all samples. Oxidation of the boride phase was proposed as the underlying reaction. This was supported by thermodynamic assessments from the literature, as well as microstructural, crystallographic, and nanoindentation characterization performed on these samples.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High-temperature thermal conductivity measurements of macro-porous graphite

Graphite is a unique material for high temperature applications and will likely become increasingly important as we attempt to electrify industrial applications. Here, we investigate the thermal properties of low-quality, macro-porous graphite to determine the tradeoff between quality and thermal performance. We use laser flash analysis (LFA) to measure the thermal diffusivity of graphite at high temperatures. Due to the large pores in the graphite samples preventing uniform laser flash heating, we first apply a thick coating to achieve the required flat, parallel surfaces for LFA measurements. We then develop a methodology to extract properties of the sample from the diffusivity measurements, based on finite element modeling of a variety of sample/coating interface profiles. Validating the methodology against a reference sample demonstrates a mean absolute percentage error of 8.5%, with potential improvement with better sample characterization. We show low-quality graphite has a thermal conductivity of ~10 W/m/K up to 1000 °C, which is an order of magnitude lower than high-quality graphite, but contributions from photon conductivity may result in higher conductivities at higher temperatures. Overall, we demonstrate an approach for measuring thermal properties of macro-porous materials at high temperatures, and apply the approach to measuring thermal conductivity of porous graphite, which will aid in the design of hightemperature systems for cost-competitive decarbonization.

Verma, Shomik↗

Viability of Miniature Discs in LFA-427

Miniature disc samples pose challenging measuring conditions for laser flash analysis. With reductions in signal from lower radiosity and lower half-rise times from low thicknesses, optimal selections of coatings and laser parameters are critical in a successful measurement. This report explains the methodology in successfully measuring two different material types—metals and ceramics—in proper coating selection, laser parameters, and post analysis for each material, as well as applying it to un-irradiated uranium samples of each type (U-metal, UO 2 ). This was done through a combination of analysis techniques combining automatic commercial methods (Neztech) and manual methods for correcting laser pulse impact aberrations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Review of thermophysical property methods applied to fueled and un-fueled molten salts

Recent investigation into designs of molten salt reactors (MSR) requires accurate data of candidate salts. Review of the literature shows lacking thermophysical (TP) property data for coolants and fuel-bearing salts of Advanced High Temperature Reactors (AHTR). Measurement uncertainties of current data are even more deficient, and this affects ongoing research where MSR modeling and testing are being performed. Melting temperature, viscosity, density, specific heat capacity, and thermal and electrical conductivity measurements are often not arranged together or discussed in great detail, especially for fuel-bearing salts. Raw data from key findings spanning over 70 years for LiF, LiF-BeF 2 , LiF-NaF-KF, KCl-MgCl 2 , KF-ZrF 4 , and NaF-KF-MgF 2 have been organized and presented here. Brief description of methods used to obtain these results, in addition to the TP data of some of these salts as fuel carriers, has also been discussed. Thermal conductivity data are particularly weak due to older, high-error measurement techniques. More recent measurement systems to evaluate salt thermal conductivity show promise for obtaining consistent absolute values. This work concludes that measurement systems such as transient hot-wire method, forced Rayleigh scattering, and laser flash analysis provide the most promise to fill these data gaps and reduce current uncertainty in thermal conductivity measurements of both fueled and un-fueled molten salts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Thermal conductivity measurement using modulated photothermal radiometry for nitrate and chloride molten salts

Molten salts are being used or explored for thermal energy storage and conversion systems in concentrating solar power and nuclear power plants. Thermal conductivity of molten salts is an important thermophysical property dictating the performance and cost of these systems, but its accurate measurement has been challenging, as evidenced by wide scattering of existing data in literature. The corrosive and conducting nature of these fluids also leads to time consuming sample preparation processes of many contact-based measurements. Here, in this work, we report the measurement of thermal conductivity of molten salts using a modulated photothermal radiometry (MPR) technique, which is a laser-based, non-contact, frequency-domain method adopted for molten salts for the first time. By unitizing the advantages of front side sensing of frequency-domain measurements and the vertical holder orientation, the technique can minimize the natural convection and salt creeping effects, thus yielding accurate molten salt thermal conductivity . The MPR technique is first calibrated using standard molten materials including paraffin wax and sulfur. It is then applied on measuring pure nitrate salts (NaNO 3 and KNO 3 ), solar salt (NaNO 3 –KNO 3 mixture), and chloride salt (NaCl–KCl–MgCl 2 ). The measurement results are compared with data from literature, especially those obtained from laser flash analysis (LFA). Our results demonstrate that the MPR is a convenient and reliable technique of measuring thermal conductivity of molten salts. Accurate thermal conductivity data of molten salts will be valuable in developing the next-generation high-temperature thermal energy storage and conversion systems.

14 SOLAR ENERGY↗

Thermophysical properties of high-density, sintered monoliths of yttrium dihydride in the range 373–773 K

Yttrium dihydride is a promising nuclear reactor moderator for high-temperature, thermal micro-reactors due to its ability to retain hydrogen to high temperatures while having a relatively low impact on neutron economy. However, it is difficult to fabricate yttrium dihydride in high-density, near net-shape monoliths for moderator applications due to challenges associated with the hydrogen absorption process. Here, high-density monoliths of yttrium dihydride were prepared by powder metallurgical methods. The lattice strain and thermal expansion coefficient were measured using neutron diffraction of powders of directly-hydrided yttrium, while the molar heat capacity and thermal diffusivity of sintered yttrium dihydride were measured using differential scanning calorimetry (DSC) and laser flash analysis (LFA), respectively. The molar heat capacity of yttrium dihydride was also calculated using density functional theory (DFT) for comparison. These parameters were used to then calculate the thermal conductivity and resistivity of yttrium dihydride as a function of temperature. The thermophysical properties of materials produced by both methods were observed to be consistent with the values from literature for yttrium dihydride. Due to the novelty of producing yttrium dihydride by powder metallurgical methods, this result indicated that the sintered monoliths were of high quality and that powder metallurgy is a viable method for large-scale production of yttrium dihydride monoliths for nuclear reactor moderator applications.

36 MATERIALS SCIENCE↗

Enhancing thermal conductivity of UO 2 with the addition of UB 2 via conventional sintering techniques

We report that uranium dioxide has been the primary fuel type used in light water reactors for more than 40 years and proven to be reliable and robust. However, the Fukushima-Daiichi nuclear accident has motivated new work evaluating fuels with characteristics promoting accident tolerance, including enhanced thermal conductivity. Recently, additives have been investigated to increase thermal conductivity, but research has been largely focused on non-fissile additions. This study investigated the use of fissile additives to not only increase the thermal conductivity but also increase the uranium loading. Uranium diboride was chosen as the additive for this study due to its promising corrosion behavior as well as its significantly higher thermal conductivity at 573 K (25 Wm -1 K -1 ) when compared to UO 2 (7 Wm -1 K -1 ). Uranium diboride powder was fabricated via the arc melting technique and a ball milling process prior to mixing with UO 2 in a 90/10 wt% UO 2 /UB 2 ratio. Green bodies were made using a uniaxial die and subjected to a traditional pressureless sintering technique at 2073 K in argon. Sintered samples were analyzed via laser flash analysis for thermal diffusivity and differential scanning calorimetry for specific heat capacity in order to calculate thermal conductivity. The samples displayed an increase of 36-55% in thermal conductivity between 323 K and 1273 K when compared to the benchmark samples (pure UO 2 ) as reported in open literature.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

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↗

Optical properties enhancement of thermal energy media for consistently high solar absorptivity

This study aimed to evaluate the optical properties of particles intended for use as thermal energy absorbers in generation 3 concentrated solar power systems. Their characterization involved UV–Vis NIR measurements with an integrating sphere for solar absorptivity, while a reflectometer was employed to measure thermal emittance. By combining absorptivity and emittance data, the solar absorption efficiency was calculated. Laser flash analysis, differential scanning calorimetry, and thermogravimetric analysis were utilized to determine thermal conductivity and specific heat. The solar absorptivity of the particles was initially measured at 0.90. After exposure to air at 1000 °C, it decreased to 0.73. However, following a reduction process, the particle recovered absorptivity of 0.90. The thermal aging and recovery were repeated multiple times, consistently achieving an absorptivity of 0.90. The thermal conductivity of the particles ranged from 0.50 to 0.88 W/(m-K). Solar absorptivity was found to be influenced by the types of iron oxide present in the particles. Particles with a predominance of hematite exhibited decreased solar absorptivity, while those containing magnetite, wüstite, and iron showed increased absorptivity. The estimated cost of the developed particles was more than ten times lower than that of current products. Given that component costs significantly impact the levelized cost of electricity (LCOE), this price reduction corresponded to an 8 % decrease in LCOE compared to other products. The low-cost thermal energy media show great promise for contributing to a reduced LCOE in the third generation of concentrating solar power systems.

14 SOLAR ENERGY↗

High-Temperature Thermophysical Property Measurement of Proposed Gen3 CSP Containment Materials

Abstract The US Department of Energy (DOE) has sponsored an initiative to improve the thermal efficiency of Concentrating Solar Power (CSP) systems. To approach parity with conventional fossil fuel-based electricity generation, the operating temperature of the CSP power cycle must exceed 700°C with integrated thermal energy storage. The materials used to house this high-temperature heat transfer media must be thermally stable and corrosion resistant. However, the temperature-dependent thermophysical properties of commonly used containment materials (nickel alloys and alumina-based firebricks) are either not well known or poorly understood. In this report, the high-temperature thermal properties of thirteen (13) candidate containment materials proposed by the CSP community are tested using laser flash analysis and differential scanning calorimetry.

Brankovic, Sonja A.↗

Fabrication and Characterization of Candidate Alloys for Advanced LEU Fuel Concepts

A set of novel uranium-based alloys has been proposed for use in advanced LEU fuel systems. This study seeks to develop methods to fabricate single-phase alloys and evaluate the compatibilities of the alloys for use in composite fuel systems. The as-cast microstructure of each alloy was characterized via scanning electron microscopy (SEM), and candidate alloys were further down-selected for homogenization and interaction testing. The U 22 Zr 20 Nb 58 alloy was successfully fabricated as a single-phase system, as demonstrated via X-ray diffraction (XRD) and SEM. The thermal and mechanical properties of the U-Nb-Zr alloy were further assessed via differential scanning calorimetry (DSC), laser flash analysis (LFA), and Vickers’ micro-hardness testing. This alloy also demonstrated improved compatibility with fuel candidate alloys from conventional matrix materials and may be a viable option for use in advanced fuel systems.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Characterization of Aluminum Metal Powders for Plutonium-238 Program

As part of radioisotope thermoelectric generator (RTG) production for power sources in deep space exploration, Oak Ridge National Laboratory (ORNL) produces plutonium-238 ( 238 Pu). To produce 238 Pu, neptunium-237 ( 237 Np) targets are fabricated at ORNL and subsequently irradiated at the High Flux Isotope Reactor (HFIR) at ORNL and the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). Specifically, current flowsheets utilize neptunium dioxide ( 237 NpO 2 ) targets. Aluminum (Al) powder is blended with 237 NpO 2 target material to improve thermal conductivity during irradiation. The current composition of 237 NpO 2 /Al pellets (i.e., cermets, or ceramic–metallics) is 20% 237 NpO 2 , 70% Al, and 10% void space. Al powders utilized by the 238 Pu program are high-fired under vacuum before blending into targets. The primary objective of this work is to measure the physical, chemical, and thermal properties of Al before and after the high-firing process. Properties of interest include the morphology, surface texture, particle size, crystal phase(s), and thermal conductivity of the material. These properties are measured with existing materials characterization equipment at ORNL, including powder x-ray diffraction (pXRD), scanning electron microscopy (SEM) with energy-dispersive spectroscopy (EDS), laser flash analysis (LFA), and thermogravimetric analysis (TGA). A secondary objective of this work is to compare the Al powders before and after the high-firing procedure to determine the effects of high-firing on chemical, physical, and thermal properties and to determine the efficacy of the high-firing process.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Property Measurements of NaCl-UCl 3 and NaCl-KCl-UCl 3 Molten Salts (Rev.1)

Thermochemical and thermophysical property values of several salt compositions of interest are needed by molten salt reactor (MSR) developers to design, license, and operate their reactors. Thermochemical and thermophysical properties being measured at Argonne include thermal transitions, phase behavior, heat capacity, density, volumetric thermal expansion of the liquid phase, thermal diffusivity, thermal conductivity, and viscosity. Several properties of eutectic compositions in the ternary NaCl-KCl-UCl 3 and binary NaCl-UCl 3 systems that may be used by MSR developers as fuel bearing salts are being measured. A 65.8 mol % NaCl–34.2 mol % UCl 3 mixture and a near-eutectic mixture of 50.9 mol % NaCl–24.4 mol % KCl–24.7 mol % UCl 3 were synthesized and the thermochemical properties of the mixtures were measured by using differential scanning calorimetry (DSC). The measured transition temperatures were compared to transition temperatures predicted using two models. A thermodynamic model of the binary NaCl-UCl 3 system was constructed using data in the Molten Salt Thermal Properties Database–Thermochemical Version 2.0 (MSTDB-TC V2.0). A ternary NaClKCl-UCl 3 system model constructed at Argonne and was described in a previous report. These comparisons can be used to validate the models. Thermophysical property values of molten salts are needed to model how salt retains and transfers heat in an MSR system. These property values are essential to the entire MSR design because molten salt is used as both the fuel and the coolant material in a salt fueled reactor. Heat capacity of the synthesized NaCl-UCl 3 and NaCl-KCl-UCl 3 salt mixtures was measured by using DSC and thermal diffusivity was measured by using laser flash analysis (LFA) at temperatures spanning the typical operating range of an MSR.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Property Measurements of NaCl-UCl 3 and LiF-NaF-KF Molten Salts Doped with Surrogate Fission Products

Knowing thermophysical and thermochemical property values of salts over the expected range of operating temperatures is essential to modeling and simulation efforts that support the commercialization of molten salt reactor (MSR) technologies. Salt properties being measured at Argonne include thermal transitions, phase behavior, heat capacity, density, surface tension, volumetric thermal expansion, thermal diffusivity, thermal conductivity, and viscosity. The properties of several salts of interest including NaCl-UCl 3 and LiF-NaF-KF (FLiNaK) have been measured at Argonne and reported previously. These property measurements are suitable for use in evaluating reactor performance during startup and the early operating life of the reactor. The physical and chemical behavior of the fuel salt is altered by the buildup of fission products and the resulting changes in heat transfer and other properties must be understood by reactor developers. This report summarizes melting behavior, heat capacity, and thermal diffusivity values that were measured for mixtures of FLiNaK and NaCl-UCl 3 salts that have been doped with surrogate fission products. Additional heat capacity measurements were also performed on a separate mixture of FLiNaK without dopants. Measured properties are suitable for incorporation into the Molten Salt Thermal Properties Database–Thermochemical (MSTDB–TC) and the Molten Salt Thermal Properties Database–Thermophysical (MSTDB–TP) to support the development of MSRs. Salts were prepared by doping eutectic mixtures of NaCl-UCl 3 and FLiNaK with surrogate fission products. These salts were prepared for use in salt spill experiments being performed at Argonne and were subsequently used for thermal property measurements. Thermal transitions and heat capacities were measured by using differential scanning calorimetry (DSC) and thermal diffusivity was measured by using laser flash analysis (LFA) at temperatures spanning the typical MSR operating range. The measured property values of the doped salts were compared to measured property values of salts without fission products to quantify the effects of the doped fission products.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Postirradiation Examination of HFIR-Irradiated Yttrium Hydrides

The US Department of Energy Microreactor Program is developing compact, high-temperature microreactors that require robust neutron moderators. Known for its high hydrogen retention and structural stability, YH x is a leading candidate for this purpose. As part of an ongoing evaluation, Oak Ridge National Laboratory conducted post-irradiation examinations on YH x specimens irradiated in the High Flux Isotope Reactor under the legacy Transformational Challenge Reactor program, focusing on their structural integrity, hydrogen retention, and thermal properties. The post-irradiation examination campaign primarily examined specimens from two irradiation campaigns, covering a range of hydrogen-to-yttrium atomic ratios (H/Y), neutron damage levels (0.1–2 displacements per atom), and targeted irradiation temperature of 600°C. The investigations included electron microscopy, high-energy x-ray diffraction, laser flash analysis, differential scanning calorimetry, and SiC thermometry analysis.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗