Calculations on fission gas behaviour in the high burnup structure

The behaviour of fission gas in high burnup fuel during steady-state and transient conditions is of special interest for safety reasons. Despite this, mechanistic models that reflect the fission gas transport processes and reliably predict the evolution of the remaining fission gas in the high burnup structure (HBS) are largely missing today. We start to address this problem by developing a one-dimensional, mass balance model and apply it to LWR UO₂ fuel at the moderate temperatures found in the rim region. We examine the quantity of gas remaining in the HBS fuel matrix at steady state and compare it with experimental values. We find that the current model reproduces the 0.2 wt% observed xenon concentration under certain conditions, viz. fast grain boundary diffusion and an effective volume diffusion coefficient. A sensitivity analysis is also conducted for the model parameters, the relative importance for which is not well established a priori.     

Simulations of heat and oxygen diffusion in UO2 nuclear fuel rods

We present finite-element simulations of coupled heat and oxygen atom diffusion for UO₂ fuel pellets. The expressions for thermal conductivity, specific heat and oxygen diffusivity for the fuel element are obtained directly from previously published correlations, or from analysis of previously published data. We examine the temperature and non-stoichiometry distributions for a varying range of conditions. Simulations are performed for steady-state and transient regime in one-dimensional (purely radial) configurations. For steady-state conditions we perform parametric studies that determine the maximum temperature in the fuel rod as a function of non-stoichiometry and heat generation rate intensity. For transient simulations, we examine the time lag in the response of the temperature and non-stoichiometry distributions with respect to sudden changes in heat generation rate intensity and oxygen removal rate. All simulations are performed with the commercial code COMSOL Multiphysics™.     

Spent fuel radionuclide source-term model for assessing spent fuel performance in geological disposal. Part I: Assessment of the instant release fraction

A source-term model for the short-term release of radionuclides from spent nuclear fuel (SNF) has been developed. It provides quantitative estimates of the fraction of various radionuclides that are expected to be released rapidly (the instant release fraction, or IRF) when water contacts the UO₂ or MOX fuel after container breaching in a geological repository. The estimates are based on correlation of leaching data for radionuclides with fuel burnup and fission gas release. Extrapolation of the data to higher fuel burnup values is based on examination of data on fuel restructuring, such as rim development, and on fission gas release data, which permits bounding IRF values to be estimated assuming that radionuclide releases will be less than fission gas release. The consideration of long-term solid-state changes influencing the IRF prior to canister breaching is addressed by evaluating alpha self-irradiation enhanced diffusion, which may gradually increase the accumulation of fission products at grain boundaries.     

Fission product release in high-burn-up UO2 oxidized to U3O8

Results of oxidation experiments on high-burn-up UO₂ are presented where fission-product vaporisation and release rates have been measured by on-line mass spectrometry as a function of time/temperature during thermal annealing treatments in a Knudsen cell under controlled oxygen atmosphere. Fractional release curves of fission gas and other less volatile fission products in the temperature range 800-2000 K were obtained from BWR fuel samples of 65 GWd t⁻¹ burn-up and oxidized to U₃O₈ at low temperature. The diffusion enthalpy of gaseous fission products and helium in different structures of U₃O₈ was determined.     

Ab initio energetics of some fission products (Kr, I, Cs, Sr and He) in uranium dioxide

A computational study of some fission products (FP) energetics in uranium dioxide is presented. Krypton, iodine, caesium, strontium and helium are considered. Calculations are made within the density functional theory in the local density approximation with the plane wave pseudopotential method. Three insertion sites are considered: the octahedral interstitial position and the oxygen and uranium substitution sites. The importance of atomic relaxations is estimated on the He and Kr cases. They prove quantitatively important but can be neglected to draw qualitative trends. For each fission product incorporation and solution energies are calculated. The obtained values of the solutions energies of the various FP are in good agreement with their experimental behaviour: Kr, Cs and I atoms are insoluble in uranium dioxide, Sr solubility depends on the stoichiometry of urania. He atoms are found to have little interaction with their environment in uranium doxide.     

Enhanced diffusion under alpha self-irradiation in spent nuclear fuel: Theoretical approaches

Various theoretical approaches have been developed in order to estimate the enhanced diffusion coefficient of fission products under alpha self-irradiation in spent nuclear fuel. These simplified models calculate the effects of alpha particles and recoil atoms on mobility of uranium atoms in UO₂. They lead to a diffusion coefficient which is proportional to the volume alpha activity with a proportionality factor of about 10⁻⁴⁴ (m⁵). However, the same models applied for fission lead to a radiation-enhanced diffusion coefficient which is approximately two orders of magnitude lower than values reported in literature for U and Pu. Other models are based on an extrapolation of radiation-enhanced diffusion measured either in reactors or under heavy ion bombardment. These models lead to a proportionality factor between the alpha self-irradiation enhanced diffusion coefficient and the volume alpha activity of 2 × 10⁻⁴¹ (m⁵).     

Characterization of zirconia-thoria-urania ceramics by X-ray and electron interactions

X-ray and electron interactions with matter were used as probes to characterize the structure and chemistry of zirconia-thoria-urania ceramics. The ceramics were prepared by coprecipitation of Zr, Th and U salts. In this study, transmission electron microscopy (TEM) techniques such as energy dispersive X-ray (EDX) analysis and electron energy loss spectroscopy (EELS) complement X-ray diffraction, extended X-ray absorption fine structure (EXAFS) and X-ray absorption near edge spectroscopy (XANES), techniques to reveal the phase structure and chemistry. The results from XRD and EDX show that these ceramics separate into a Zr-based phase and an actinide-based phase with low mutual affinity of Th and Zr, as well as partial solubility of U in Zr. The comparison of EELS spectra collected for the ceramics with spectra collected for UO₂ and U₃O₈ reference materials also allow us to assess U oxidation state independently in the two separate phases.     

On stability of spatial distributions of crystal structure defects in irradiated high burnup UO2 fuel

Conditions of Kinoshita instability development of point defects and dislocation spatial distributions in the crystal structure of UO₂ fuel are studied. As a result of the instability development, spatially non-uniform regions with increased dislocation density are formed. Closed-form expressions of instability increment and spatial scale are derived. Parameters of the instability for irradiation conditions of high burnup UO₂ fuel are obtained by means of numerical simulation. Instability development time is shown to be inversely proportional to fission rate and it increases as dislocation density decreases. Calculated values of instability spatial scale and increment are in accordance with the size of fine grains and their formation rate in the peripheral zones of high burnup LWR fuel pellets.     

Statistical approach and benchmarking for modeling of multi-dimensional behavior in TRISO-coated fuel particles

The fundamental design for a gas-cooled reactor relies on the behavior of the coated particle fuel. The coating layers, termed the TRISO coating, act as a mini-pressure vessel that retains fission products. Results of US irradiation experiments show that many more fuel particles have failed than can be attributed to one-dimensional pressure vessel failures alone. Post-irradiation examinations indicate that multi-dimensional effects, such as the presence of irradiation-induced shrinkage cracks in the inner pyrolytic carbon layer, contribute to these failures. To address these effects, the methods of prior one-dimensional models are expanded to capture the stress intensification associated with multi-dimensional behavior. An approximation of the stress levels enables the treatment of statistical variations in numerous design parameters and Monte Carlo sampling over a large number of particles. The approach is shown to make reasonable predictions when used to calculate failure probabilities for irradiation experiments of the New Production - Modular High Temperature Gas Cooled Reactor Program.     

Correlation of yield stress and microhardness in 08Cr16Ni11Mo3 stainless steel irradiated to high dose in the BN-350 fast reactor

The relationship between the microhardness and the engineering yield stress in 08Cr16Ni11Mo3 steel after irradiation in the BN-350 reactor has been experimentally derived and agrees with a previously published correlation developed by Toloczko for unirradiated 316 in a variety of cold-work conditions. Even more importantly, when the correlation is derived in the K_Δ format where the correlation involves changes in the two properties, excellent agreement is found with a universal K_Δ correlation developed by Busby and coworkers. Additionally, this report points out that microhardness measurements must take into account that sodium exposure at high temperature and neutron fluence alters the metal surface to produce ferrite, and therefore the altered layers should be removed prior to testing.     

Burnup simulations and spent fuel characteristics of ZrO2 based inert matrix fuels

Reducing the inventory of long lived isotopes that are contained in spent nuclear fuel is essential for maximizing repository capacity and extending the lifetime of related storage. Because of their non-fertile matrices, inert matrix fuels (IMF’s) could be an ideal vehicle for using light-water reactors to help decrease the inventory of plutonium and other transuranics (neptunium, americium, curium) that are contained within spent uranium oxide fuel (UOX). Quantifying the characteristics of spent IMF is therefore of fundamental importance to determining its effect on repository design and capacity. We consider six ZrO₂ based IMF formulations with different transuranic loadings in a 1-8 IMF to UOX pin-cell arrangement. Burnup calculations are performed using a collision probability model where transport of neutrons through space is modeled using fuel to moderator transport and escape probabilities. The lethargy dependent neutron flux is treated with a high resolution multigroup thermalization method. The results of the reactor physics model are compared to a benchmark case performed with Montebruns and indicate that the approach yields reliable results applicable to high-level analyses of spent fuel isotopics. The data generated show that a fourfold reduction in the radiological and integrated thermal output is achievable in single recycle using IMF, as compared to direct disposal of an energy equivalent spent UOX.     

Constituent redistribution in U-Pu-Zr fuel during irradiation

The thermo-migration fluxes of U, Pu and Zr in U-Pu-Zr metallic alloy fuel during irradiation in the Experimental Breeder Reactor II (EBR-II) were calculated using the constituent redistribution profiles measured in postirradiation examinations. Based on these fluxes, the diffusion coefficients, and the sums of heat of transport and enthalpy of solution for the γ, γ+ζ and δ+ζ phases in U-Pu-Zr were obtained. Using these data, the predicted concentration redistribution profiles are consistent with the measurements. The effect of minor actinide (Am and Np) addition was also examined. Am migration generally followed that of Zr with local precipitation, while Np behaved similarly to Pu.     

Assessment of the constitutive properties from small ball punch test: experiment and modeling

An assessment of the true stress-true strain relationship has been done by means of tensile and small ball punch tests on austenitic and tempered martensitic steel at room temperature. A finite element model was developed and validated to calculate the force-deflection curve obtained from the ball punch experiment. The effects of the specimen thickness and material properties on the overall shape of the ball punch test curve are discussed. The constitutive behavior assigned to the specimen for the calculations was determined from the tensile test but we showed that assumptions have to be done to extend it to large strains as those arising during the punch tests. Using an inverse methodology, it was possible to show that a linear strain-hardening stage takes place at large strains. The potential for evaluating the evolution of the strain-hardening capacity after irradiation is outlined.     

Nanoindentation characterization of ErT2 thin films

The properties of ErT₂ films change as the tritium decays into ³He, which has important implications for long-term film stability in applications such as neutron generators. Ultra-low load nanoindentation, analyzed using finite-element modeling to separate the nanomechanical properties of 500 nm ErT₂ layers from those of the underlying substrates, has been used to examine the films as they age. The ³He bubbles which form as the film ages act as barriers to dislocation movement, hardening the material, but not dramatically affecting the elastic properties. By modeling the layer as an isotropic, elastic-plastic solid with the Mises yield criterion, the nanoindentation data is shown to correspond to an increase of nearly 2× in strength after aging for over a year.     

Transmission electron microscopy examination of oxide layers formed on Zr alloys

A transmission electron microscopy investigation was performed on oxides formed on three zirconium alloys (Zircaloy-4, ZIRLO and Zr-2.5Nb) in pure water and lithiated water environments. This research is part of a systematic study of oxide microstructures using various techniques to explain differences in corrosion rates of different zirconium alloys. In this work, cross-sectional transmission electron microscopy was used to determine the morphology of the oxide layers (grain size and shape, oxide phases, texture, cracks, and incorporation of precipitates). These characteristics were found to vary with the alloy chemistry, the corrosion environment, and the distance from the oxide/metal interface. These are discussed and used in conjunction with observations from other techniques to derive a mechanism of oxide growth in zirconium alloys.     

Irradiation damage in 304 and 316 stainless steels: experimental investigation and modeling. Part II: Irradiation induced hardening

The consequences of irradiation damage in austenitic stainless steels on their mechanical properties, namely the yield stress, are investigated both experimentally and theoretically. The observed hardening is correlated with the quantitative characteristics of irradiation defects population. A simple model allowing for the defaulting of Frank loops under stress predicts the hardening and its saturation at large doses.     

Investigation of physico-mechanical properties of ceramic oxide kernels for nuclear applications

In the present work, two different classes of oxide kernels were investigated: unirradiated thoria, urania and (Th,U)O₂ fuel kernels and low-density Al₂O₃ kernels for the incorporation of minor actinides. The physical mechanism of oxide kernel failure under uniaxial compression was investigated. A new method for determining the physico-mechanical properties of kernels has been developed and the parameters P_S and δ, characterising the level of stress required for destruction of the material structure and the brittleness of the investigated materials, respectively, were evaluated and discussed. It was shown that the value of P_S is analogous to traditional characteristics of material such as microhardness Hv. The `quantisation' effect was revealed in the kernel crushing strength and deformation distributions. The physico-mechanical properties of ceramic kernels (average particle size, microstructure, phase state, density, P_S and δ) were investigated and comparative analysis of different kernel types was performed. Additionally, the impact of annealing time on the properties of low-density Al₂O₃ kernels was examined.     

Characterization of the reaction layer in U-7wt%Mo/Al diffusion couples

The reaction layer in chemical diffusion couples U-7wt%Mo/Al was investigated using optical and scanning electron microscopy, electron probe microanalysis and X-ray diffraction (XRD) techniques. When the U-7wt%Mo alloy was previously homogenized and the γ(U, Mo) phase was retained, the formation of (U, Mo)Al₃ and (U, Mo)Al₄ was observed at 580 °C. Also a very thin band was detected close to the Al side, the structure of the ternary compound Al₂₀UMo₂ might be assigned to it. When the decomposition of the γ(U, Mo) took place, a drastic change in the diffusion behavior was observed. In this case, XRD indicated the presence of phases with the structures of (U, Mo)Al₃, Al₄₃U₆Mo₄, γ(U, Mo) and α(U) in the reaction layer.     

On the radiation damage characterization of candidate first wall materials in a fusion reactor using various molten salts

Evaluating radiation damage characteristics of structural materials considered to be used in fusion reactors is very crucial. In fusion reactors, the highest material damage occurs in the first wall because it will be exposed to the highest neutron, gamma ray and charged particle currents produced in the fusion chamber. This damage reduces the lifetime of the first wall material and leads to frequent replacement of this material during the reactor operation period. In order to decrease operational cost of a fusion reactor, lifetime of the first wall material should be extended to reactor’s lifetime. Using a protective flowing liquid wall between the plasma and first wall can decrease the radiation damage on first wall and extend its lifetime to the reactor’s lifetime. In this study, radiation damage characterization of various low activation materials used as first wall material in a magnetic fusion reactor blanket using a liquid wall was made. Various coolants (Flibe, Flibe + 4% mol ThF₄, Flibe + 8% mol ThF₄, Li₂₀Sn₈₀) were used to investigate their effect on the radiation damage of first wall materials. Calculations were carried out by using the code Scale4.3 to solve Boltzmann neutron transport equation. Numerical results brought out that the ferritic steel with Flibe based coolants showed the best performance with respect to radiation damage.     

Corrosion of steels with surface treatment and Al-alloying by GESA exposed in lead–bismuth

Corrosion tests were performed for T91, E911 and ODS (oxide dispersion strengthened) with surface treatment and Al-alloying by pulsed electron beam (GESA—GepulsteElektronenStrahlAnlage) in flowing lead bismuth eutectic (LBE) with an oxygen content of 10⁻⁶ wt% at 550 °C for 2000 h. The result was that the surface treatment by GESA led to a faster growing multiphase oxide layer which was very homogenous in thickness. After exposure of specimens to LBE, the average oxide layer at the surface was 14–15 μm thick for ODS, 19–20 μm for E911 and 8–22 μm for T91. No dissolution attack occurred. On the surface of the Al-alloyed specimens, thin protective alumina layers were observed at the places where FeAl was formed by the GESA process, otherwise multiphase oxide layers or corrosion attack were observed.