Simulation of Metal/Oxide Interface Mobility: Effects of Mechanical Stresses on Geometrical Singularities

During the last decade, an increasing importance has been given to the feedback of mechanical stresses on the chemical diffusion and, further, on corrosion. Many works point the active role of stresses on the material ageing especially on their negative consequences leading to the damaging of structures. Based on a theoretical study and using numerical tools and experimental results our previous works [1, on stress/diffusion coupling, highlight the strong influence of stress field on the diffusion process. The aim of the present paper is to describe the influence of some particular morphologies of the metal/oxide interface on both diffusion and oxidation process. The oxidation is assumed to be driven by a mass conservation law (Stefan's law) while the diffusion coefficient of oxygen in metal is locally influenced by the stress field. The stability of a waved-shape interface is studied in both cases: simple diffusion and coupled stress/diffusion process. In this purpose we have developed an original numerical model using a virtual metal/oxide interface of a mono-material with oxygen concentration-dependent parameters, which allows to operate easily with any shape of interface and to use simple finite element meshes. Furthermore, in order to underline in a more obvious way the consequences of mechanical stress on the diffusion process, a particular geometry is studied

Theoretical Study of Coupling Mechanisms between Oxygen Diffusion, Chemical Reaction, Mechanical Stresses in a Solid-Gas Reactive System

This paper offers a study of oxygen dissolution into a solid, and its consequences on the mechanical behaviour of the material. In fact, mechanical strains strongly influence the oxidation processes and may be, in some materials, responsible for cracking. To realize this study, mechanical considerations are introduced into the classical diffusion laws. Simulations were made for the particular case of uranium dioxide, which undergoes the chemical fragmentation. According to our simulations, the hypothesis of a compression stress field into the oxidised UO2 compound near the internal interface is consistent with some oxidation mechanisms of oxidation experimentally observed. More generally, this work will be extended to the simulation to an oxide layer growth on a metallic substrate

Specific Aspects of Internal Corrosion of Nuclear Clad Made of Zircaloy

In PWR, the Zircaloy based clad is the first safety barrier of the fuel rod, it must prevent the dispersion of the radioactive elements, which are formed by fission inside the UO2 pellets filling the clad. We focus here on internal corrosion that occurs when the clad is in tight contact with the UO2 pellet. In this situation, with temperature of 400^{\circ}C on the internal surface of the clad, a layer of oxidised Zircaloy is formed with a thickness ranging from 5 to 15 $\mu$m. In this paper, we will underline the specific behaviour of this internal corrosion layer compared to wet corrosion of Zircaloy. Simulations will underline the differences of stress field and their influences on corresponding dissolved oxygen profiles. The reasons for these differences will be discussed as function of the mechanical state at inner surface of the clad which is highly compressed. Differences between mechanical conditions generated by an inner or outer corrosion of the clad are studied and their influences on the diffusion phenomena are highlighted

A thermodynamic approach of the mechano-chemical coupling during the oxidation of uranium dioxide

International audienceThe aim of the present work is to introduce a thermodynamic model to describe the growth of an oxide layer on a metallic substrate. More precisely, this paper offers a study of oxygen dissolution into a solid, and its consequences on the apparition of mechanical stresses. They strongly influence the oxidation processes and may be, in some materials, responsible for cracking. To realize this study, mechanical considerations are introduced into the classical diffusion laws. Simulations were made for the particular case of uranium dioxide, which undergoes the chemical fragmentation. According to our simulations, the hypothesis of a compression stress field into the oxidised UO2 compound near the internal interface is consistent with the interpretation of the mechanisms of oxidation observed experimentally

Contribution à l'étude des interactions entre contraintes résiduelles et dissolution d'oxygène dans un solide déformable réactif

Cette thèse a pour objet la mise en évidence des interactions entre un champ de contraintes mécaniques et un champ de composition dans un processus de diffusion de matière au sein d un solide déformable réactif. Notre travail a évolué chronologiquement de l étude paramétrique numérique, vers la mise en ouvre expérimentale d une démarche destinée a révéler le rôle moteur des contraintes dans la diffusion de matière.Différentes sources de contraintes mécaniques ont tout d'abord été analysées numériquement a travers leurs impacts sur le processus de diffusion d'oxygène dans un métal (Zr) ou une céramique (UO2) soumis à un environnement oxydant. Cette approche a permis entre autres : de dégager un procédé de traitement de surface (grenaillage) susceptible d'engendrer un champs de contraintes résiduelles particulier comme préalable à la mise en ouvre d'une étude expérimentale destinées à valider les conclusions numériques ; de mettre en évidence le caractère stabilisateur de la contrainte sur la morphologie ondulée d'une interface oxyde/métal (cas du Zr).Dans l'approche expérimentale, différents outils ont été exploités pour caractériser le matériau (SDL, MEB, ATG, MTI, microdureté). Ils ont permis la mise en évidence d'une influence forte de la durée de grenaillage sur le ralentissement de l'oxydation. L analyse comparative des résultats expérimentaux et de simulations est révélatrice d intéractions fortes entre les champs de contraintes et de composition induits par les différents traitements (grenaillage et/ou pré-oxydation)The aim of this PhD work is to highlight the interactions between the mechanical stress and the chemical composition within diffusion of matter process for a reactive solid. The chronological evolution of our work goes from a parametric numerical study to an experimental study and reveals the role of mechanical stresses on the oxygen diffusion process.Different origins of mechanical stress were first numerically analysed from the point of view of their impacts on the process of oxygen diffusion into a metal (Zr) or a ceramic (UO2) subjected to an oxidizing environment. This approach allowed us: to identify a surface treatment (shot-peening) able to generate a residual specific stress field, as a starting point for an experimental study implementation in order to validate the numerical study conclusions; to highlight the ability of the stress field on the stabilisation of the morphology of an undulated metal/oxide interface (case of Zr).In the experimental approach, different technics were used to characterize the material (GDOS, SEM, TGA, hole-drilling method, micro-hardness tests). They permitted the detection of a strong influence of shot-peening on the oxidation rate. The comparison of experimental and numerical simulation results reveals strong interactions between stress and compositions fields induced by the different treatments (shot-peening and/or pre-oxidation)DIJON-BU Doc.électronique (212319901) / SudocSudocFranceF

Internal Interface Strains Effects on UO2/U3O7 Oxidation Behaviour

The growth of a U3O7 oxide layer during the anionic oxidation of UO2 pellets induced very important mechanical stresses due to the crystallographic lattice parameters differences between UO2 and its oxide. These stresses, combined with the chemical processes of oxidation, can lead to the cracking of the system, called chemical fragmentation. We study the crystallographic orientation of the oxide lattice growing at the surface of UO2, pointing the fact that epitaxy relations at interface govern the coexistence of UO2 and U3O7. In this work, several results are given: - Determination of the epitaxy relations between the substrate and its oxide thanks to the Bollmann's method; epitaxy strains are deduced. - Study of the coexistence of different domains in the U3O7 (crystallographic compatibility conditions at the interface between two phases: Hadamard conditions). - FEM simulations of a multi-domain U3O7 connected to a UO2 substrate explain the existence of a critical thickness of U3O7 layer

Modélisation numérique avec apport de matière du soudo-brasage des assemblages hétérogènes acier / aluminium

Dans cette étude nous abordons la modélisation numérique thermomécanique du soudo-brasage de tôles d'acier et d'aluminium par la technique CMT dans une configuration à clin. Ces métaux ont des coefficients de dilatation thermique différents, ce qui provoque des déformations et des contraintes résiduelles élevées. Cette simulation prend en compte l'apport de matière durant le processus. Une validation de la modélisation est faite sur le cas simple du dépôt d'un cordon de matériau d'apport sur une plaque d'aluminium. Pour l'assemblage hétérogène des comparaisons sont faites entre les résultats numériques et expérimentaux en termes de déplacements hors-plan

Influence of the U3O7 domain structure on cracking during the oxidation of UO2

International audienceCracking is observed when a UO2 single crystal is oxidised in air. Previous studies led to the hypothesis that cracking occurs once a critical depth of U3O7 oxidised layer is reached. We present some μ-Laue X-ray diffraction results, which evidence that the U3O7 layer, grown by topotaxy on UO2, is made of domains with different crystalline orientations. This observation was used to perform a modelling of oxidation coupling chemical and mechanical parameters, which showed that the domain patterning induces stress localisation. This result is discussed in comparison with stress localisation observed in thin layer deposited on a substrate and used to propose an interpretation of UO2 oxidation and cracking