Thermal transport properties of hafnium hydrides and deuterides

The thermal conductivities of δ′-, δ-, δ+ε-, and ε-phase hafnium hydrides and deuterides with various hydrogen isotope concentrations (HfH_x, 1.48 ? x ? 2.03; HfD_x, 1.55 ? x ? 1.94) were evaluated within the temperature range of 290-570 K from the measured thermal diffusivity, calculated specific heat, and density. The thermal conductivities of δ′-, δ-, δ+ε-, and ε-phase HfH_x and HfD_x are independent of the temperature within the range 300-550 K and are in the range 0.15-0.22 W/cm K and 0.17-0.23 W/cm K, respectively; these values are similar to and lower than the observed thermal conductivities of α-phase Hf. The experimental results for the electrical resistivities of δ′-, δ-, δ+ε-, and ε-phase HfH_x and HfD_x and the Lorenz number corresponding to the electronic conduction, obtained from the Wiedemann-Franz rule, indicated that heat conduction due to electron migration significantly influences the thermal conductivity values at high temperatures. On the other hand, heat conduction due to phonon migration significantly affects the isotope effects on the thermal transport properties.     

Molecular dynamics calculations of heat conduction in actinide oxides under thermal gradient

Thermal conductivities of UO₂, PuO₂ and (U_0.8,Pu_0.2)O₂ have been investigated by non-equilibrium molecular dynamics (NEMD) simulation between 300 K and 2000 K. The thermal conductivity was directly calculated by the temperature gradient on the system according to Fourier's law in NEMD simulation. The thermal conductivity obtained from the NEMD simulation decreases with a decrease of the supercell size, which means the phonon scattering occurs at the system boundaries in the microsystem. In addition, the present NEMD simulation, as well as previous EMD simulation studies, clearly shows that the Umklapp process causes the decrease of thermal conductivity at high temperatures. When comparison is made with literature data, the calculated results obtained from the relatively small supercell are in good agreement with the measured ones for the above actinide dioxides.     

Thermal Conductivity of UO2-BeO Pellet

Beryllium oxide(BeO)-doped (0.3, 0.6, 0.9, 1.2 and 13.6 wt%) UO₂ pellets were fabricated to evaluate the effects of BeO precipitate shape on thermal conductivity. Precipitate distributions were of two types: BeO precipitated almost continuously along a grain boundary (designated BeO continuous type) and spherical BeO randomly dispersed within the matrix (designated BeO dispersed type). Thermal diffusivity was measured by a laser flash method and thermal conductivity was evaluated. The thermal conductivity increased with the BeO content. The thermal conductivity of the BeO continuous type was higher than that of the BeO dispersed type at lower temperatures, while their difference became smaller at higher temperatures. The thermal conductivities of UO₂-1.2 wt% BeO at 1,100K were higher than that of UO₂ by about 25 % for the BeO continuous type and by about 10 % for the BeO dispersed type. The thermal conductivities of both types were expressed by a semi-empirical equation as a function of volume fraction and shape of the BeO precipitates.     

Thermal conductivity of BaPuO3 at temperatures from 300 to 1500 K

Polycrystalline specimens of barium plutonate, BaPuO₃, have been prepared by mixing the appropriate amounts of PuO₂ and BaCO₃ followed by reacting and sintering at 1600 K under the flowing gas atmosphere of dry-air. The sintered specimens had a single phase of orthorhombic perovskite structure and were crack-free. The Debye temperature of BaPuO₃ was determined from the sound velocity and lattice parameter measurements. The elastic moduli were also determined from the longitudinal and shear sound velocity. The thermal conductivity of BaPuO₃ was calculated from the measured density at room temperature, literature values of heat capacity, and thermal diffusivity measured by a laser flash method in vacuum. The thermal conductivity of BaPuO₃ was roughly independent of the temperature and was almost the same magnitude as that of BaUO₃. This was markedly lower than the conductivities of other perovskite type oxides and was about one-tenth that of UO₂ around room temperature. The temperature dependence of the thermal conductivity of BaPuO₃ was found to be quite similar to that of BaUO₃.     

Atomistic modeling of the vibrational and thermodynamic properties of uranium dioxide, UO2

Modeling the thermal properties of uranium oxide is of immense interest to the nuclear industry. UO₂ belongs to the family of superionic conductors whose solid-state diffusion coefficients at high temperatures are comparable to that of liquids. We report lattice dynamics and molecular dynamics studies carried out on oxide UO₂ in its normal as well as superionic phase. Lattice dynamics calculations have been carried out using shell model in the quasiharmonic approximation. The calculated equilibrium structure, elastic constants, bulk modulus, phonon frequencies and specific heat are in excellent agreement with the reported experimental data. Pressure variation of the phonon dispersion and equation of state have also been predicted. Molecular dynamics simulations have been carried out to study the diffusion behavior and the thermodynamic properties in UO₂. The diffusion constant of O in UO₂ has been determined. The pair correlation functions, O-U-O bond angle and thermal amplitude of vibration for the oxygen atom provide a microscopic picture of the local structure thereby throwing light on the gradual increase in the disorder of the oxygen sub-lattice which is a signature of superionic transition. The calculated transition temperature of UO₂ is 2300 K, which compares well with experimental value of about 2600 K.     

Thermal conductivity evaluation of high burnup mixed-oxide (MOX) fuel pellet

The thermal conductivity formula of fuel pellet which contains the effects of burnup and plutonium (Pu) addition was proposed based on the Klemens’ theory and reported thermal conductivities of unirradiated (U, Pu) O₂ and irradiated UO₂ pellets. The thermal conductivity of high burnup MOX pellet was formulated by applying a summation rule between phonon scattering parameters which show the effects of plutonium addition and burnup. Temperature of high burnup MOX fuel was evaluated based on the thermal conductivity integral which was calculated from the above-mentioned thermal conductivity formula. Calculated fuel temperatures were plotted against the linear heat rates of the fuel rods, and were compared with the fuel temperatures measured in a test reactor. Since both values agreed well, it was confirmed that the proposed thermal conductivity formula of MOX pellets is adequate.     

Thermal Diffusivities and Thermal Conductivities of UO2-Gd2O3

Thermal diffusivities of samples of UO₂ and UO₂ doped with 3, 5, 7 and 10 w/0 Gd₂O₃ were measured over the temperature range of 298~2,023 K by a laser flash method. Then thermal conductivities were calculated from them. The thermal conductivity decreased with increasing Gd₂O₃ content at low temperatures, while it was independent of Gd₂O₃ content at high temperatures. An expression of the thermal conductivity was proposed for (U, Gd)O₂ solid solution as a function of Gd₂O₃ content and temperature by applying Klemens' model.     

Thermal Conductivity Measurements on UO2+x from 300 to 1,400 K

In order to evaluate the thermal conductivity of oxidized fuel pellets of leaker fuel rods, UO_2+x samples with x between 0.00 and 0.20 were prepared by an oxidation or a sintering method. Sample thermal diffusivities were measured by using a laser flash method from 300 to 1,400 K and their thermal conductivities were evaluated from multiplying the thermal diffusivities by the sample densities and the specific heat capacities derived from the literature. The thermal conductivities of UO_2+x were decreased with increasing hyperstoichiometry and they were expressed as a function of their hyperstoichiometry using the concentration of U⁵⁺ formed with the excess interstitial oxygen atoms.     

Thermal conductivity and thermal expansion of hot-pressed trisodium uranate (Na3UO4)

Thermal conductivity and thermal expansion of Na₃UO₄ prepared by two different reaction processes were determined over a temperature range of 20–1000°C. Compositional differences in the samples resulting from the different reaction processes have a pronounced effect on thermal expansion and on thermal conductivity below 500°C. Above 500°C, these compositional differences in the thermal conductivities decrease.     

Simulation of ion-track ranges in uranium oxide

Direct comparisons between statistically sound simulations of ion-tracks and published experimental measurements of range densities of iodine implants in uranium dioxide have been made with implant energies in the range of 100–800 keV. Our simulations are conducted with REED-MD (Rare Event Enhanced Domain-following Molecular Dynamics) in order to account for the materials structure in both single crystalline and polycrystalline samples. We find excellent agreement between REED-MD results and experiments for polycrystalline target materials.     

Calculation of thermal neutron self-shielding correction factors for aqueous bulk sample prompt gamma neutron activation analysis using the MCNP code

In this work thermal neutron self-shielding in aqueous bulk samples containing neutron absorbing materials is studied using bulk sample prompt gamma neutron activation analysis (BSPGNAA) with the MCNP code. The code was used to perform three dimensional simulations of a neutron source, neutron detector and sample of various material compositions. The MCNP model was validated against experimental measurements of the neutron flux performed using a BF₃ detector. Simulations were performed to predict thermal neutron self-shielding in aqueous bulk samples containing neutron absorbing solutes. In practice, the MCNP calculations are combined with experimental measurements of the relative thermal neutron flux over the sample’s surface, with respect to a reference water sample, to derive the thermal neutron self-shielding within the sample. The proposed methodology can be used for the determination of the elemental concentration of unknown aqueous samples by BSPGNAA where knowledge of the average thermal neutron flux within the sample volume is required.     

Compositional analysis of atom beam co-sputtered metal-silica nanocomposites by Rutherford backscattering spectrometry

Metal:SiO₂ (metal: Ni, Ag, Au) nanocomposite films of different compositions have been prepared by atom beam co-sputtering. The estimation of composition of films is done theoretically using sputtering yield and relative area of metal and SiO₂. The sputtering yields used for estimation of composition are calculated by three theoretical methods: Monte Carlo simulations (SRIM code), Sigmund’s theory and Sigmund’s theory modified by Anderson and Bay. Rutherford backscattering spectrometry (RBS) is also used to analyze the composition of the nanocomposite films. RUMP simulations of RBS data are performed. The errors in theoretical calculations and RBS results are estimated. It is found that SRIM is more appropriate for Ni:SiO₂ nanocomposite films, while modified Sigmund’s theory based method is better for Ag:SiO₂ and Au:SiO₂ nanocomposite films. The possible sources of errors in theoretical methods with respect to experimental (RBS) results are also discussed.     

Isotope Effects on Thermal Conductivity of Boron Carbide

The isotopically enriched disk samples of ¹⁰B₄ ¹²C, (¹⁰B_0.75 ¹¹B_0.25)₄ ¹²C, (¹⁰B_0.20 ¹¹B_0.80)₄ ¹²C, ¹⁰B₄ ¹³C, ¹⁰B₄ (¹²C_0.50 ¹³C_0.50), ¹¹B₄ (¹²C_0.50 ¹³C_0.50), ¹¹B₄ ¹²C, ¹¹B₄ ¹³C and natural ⁿB₄ ⁿC were prepared by the spark plasma sintering method. The thermal diffusivity for each sample was measured by the laser flash method over the temperature range from 290 to 1,450 K. The isotope effects on the thermal conductivities, which were calculated from the measured thermal diffusivities, the heat capacity for natural B₄C and densities, were discussed in terms of the phonon-velocity and the scattering probability of phonon by isotopic impurity. The thermal conductivity decreased only with increasing the mean mass of boron. In the single-atom model, the phonon-velocity decreases with increasing the mass of atoms. The thermal conductivity obtained in this study was seen to be independent on the scattering probability of phonon by isotopic impurity, but to depend on the phonon-velocity. Isotope effects are thought to be difficult to detect in polycrystalline boron carbide.     

Pu-breeding feasibility in PWR

This study addresses the issue of alternative pathways for breeding plutonium in a 900 MWe three loop thermal pressurized water reactor (PWR), either fueled with uranium fuel (3.5% U-235) or with mixed fuel (20% MOX). During the operation of a nuclear reactor the in-core neutron flux and the ex-core neutron flux are monitored with flux detectors. At the places where those detectors operate, the guide thimbles and the vessel wall, respectively, the neutron flux can be used to irradiate material samples. This paper investigates whether it would be possible to produce plutonium by breeding it at the walls of a PWR vessel and/or in the guide thimbles. The neutron flux in the reactor and the corresponding multi-group spectra are estimated with Monte Carlo simulations for different positions at the vessel wall of a PWR operating with either UO₂ or MOX. Then the irradiation of fresh uranium samples at the vessel wall and in the guide thimbles are calculated and the isotopic composition of the irradiated samples are determined. The minimum irradiation period and the necessary minimum amount of fresh uranium to breed different grades of plutonium are derived.     

Thermal conductivities of hypostoichiometric (U, Pu, Am)O2−x oxide

The thermal conductivities of (U_0.68Pu_0.30Am_0.02)O_2.00−x solid solutions (x = 0.00-0.08) were studied at temperatures from 900 to 1773 K. The thermal conductivities were obtained from the thermal diffusivities measured by the laser flash method. The thermal conductivities obtained experimentally up to about 1400 K could be expressed by a classical phonon transport model, λ = (A + BT)⁻¹, A(x) = 3.31 × x + 9.92 × 10⁻³ (mK/W) and B(x) = (−6.68 × x + 2.46) × 10⁻⁴ (m/W). The experimental A values showed a good agreement with theoretical predictions, but the experimental B values showed not so good agreement with the theoretical ones in the low O/M ratio region. From the comparison of A and B values obtained in this study with the ones of (U,Pu)O_2−x obtained by Duriez et al. [C. Duriez, J.P. Alessandri, T. Gervais, Y. Philipponneau, J. Nucl. Mater. 277 (2000) 143], the addition of Am into (U, Pu)O_2−x gave no significant effect on the O/M dependency of A and B values.     

First-principles theory for helium and xenon diffusion in uranium dioxide

The diffusion properties of He and Xe in UO₂ have been investigated, using density-functional calculations employing the projector-augmented-wave (PAW) method and the generalized gradient approximation (GGA). The migration energies corresponding to both interstitial and vacancy-assisted mechanisms have been calculated and the results for the two noble gas atoms are compared with each other. We suggest that He likely diffuses by hopping through a single vacancy with computed low migration energies smaller than 0.79 eV and its diffusivity is much higher than that of Xe. Xe has a quite large migration energy compared to He; the strain energy plays a key role in Xe diffusion in UO₂.     

A non-equilibrium molecular dynamics study of the thermal conductivity of uranium dioxide

The thermal conductivity of uranium dioxide in the temperature range of 300–2400 K was estimated by non-equilibrium molecular dynamics calculation using Fourier law.The Kawamura function was adopted as the interatomic potential function.The calculated thermal conductivities are found to be strongly dependent on the temperature of the simulation cube.The thermal conductivity simulation results are compared with the experiment results and agreed well with the experimental results when the temperature is above 600 K.The thermal conductivities scale effects are found to be existed in uranium dioxide nanometer thin film.The approximate mean free paths of phonons in different temperatures can be examined.     

Thickness and MeV Si ions bombardment effects on the thermoelectric properties of Ce3Sb10 thin films

The three single layer Ce₃Sb₁₀ thin films were grown on silicon dioxide and quartz (suprasil) substrates with thicknesses of 297, 269 and 70 nm using ion beam assisted deposition (IBAD) technique. The high-energy cross plane Si ion bombardments with constant energy of 5 MeV have been performed with varying fluence from 1 × 10¹², 1 × 10¹³, 1 × 10¹⁴, 1 × 10¹⁵ ions/cm². The Si ions bombardment modified the thermoelectric properties of films as expected. The fluence and temperature dependence of cross plane thermoelectric parameters that are Seebeck coefficient, electrical and thermal conductivities were determined to evaluate the dimensionless figure of merit, ZT. Rutherford backscattering spectrometry (RBS) enabled us to determine the elemental composition of the deposited materials and layer thickness of each film.     

Thermal Expansion and Thermal Conductivity of Cesium Uranates

Two kinds of cesium uranates, which are often predicted by thermochemical calculations to be formed in irradiated oxide fuels with high oxygen potentials, were prepared from U₃O₈ and Cs₂CO₃ to determine the thermal expansions and the thermal conductivities. The lattice parameters of tetragonal Cs₂UO₄ and monoclinic Cs₂U₂O₇ were measured by the high-temperature X-ray diffraction method as a function of temperature. The linear thermal expansions of Cs₂UO₄ and Cs₂U₂O₇ obtained from the temperature dependencies of the lattice parameters were 1.2% and 1.1% from room temperature to 973 and 1,073K, respectively. The thermal diffusivities of Cs₂UO₄ and Cs₂U₂O₇ were measured on the disk-shaped samples by the laser flash method as a function of temperature. The thermal conductivities were evaluated from the measured thermal diffusivities and the bulk densities, and the specific heat capacity available in literature. The thermal conductivity of Cs₂UO₄ corrected for 100%TD was 1.2W/m·K at 980K and that of Cs₂U₂O₇ was 0.94W/m·K at 1,093K, which are about 30% and 27% of that of UO₂, respectively.     

Thermal conductivity and electrical resistivity of liquid Ag–In alloy

To understand and predict the progression of core meltdown accidents in nuclear power plants, it is important to understand the behavior of molten core materials. We focused on the melting behavior of Ag–In–Cd alloys used in the control rods of pressurized water reactors that are known to melt first when a severe accident occurs. To obtain fundamental knowledge about these alloys, we studied the thermal conductivity of Ag–In binary alloys in this study. We evaluated thermal conductivity using two approaches: evaluating from thermal diffusivity up to 873 K measured by the laser-flash method, and calculating based on the Wiedemann–Franz law using the electrical resistivity up to 1273 K measured by the four-probe method. The values of thermal conductivity of liquid Ag–In alloys obtained by these two methods agreed well except for pure indium. Although Ag is known as a material that has one of the highest thermal conductivities, the thermal conductivity of liquid Ag–In alloys is much lower than that of pure liquid Ag (177 W/mK at 1273 K), but almost the same or less than that of liquid In (59.2 W/mK at 1273 K) in all Ag_1?xIn_x (x = 0.2–0.8) alloys at all temperatures in this measurement.