Papers by Author: Sébastien Garruchet

Abstract: We investigated the oxidation of nanocrystalline aluminum surfaces by using variable charge molecular dynamics at 600 K under three oxygen pressures: 1, 10 and 20 atm. The interaction potential was described by the electrostatic plus (Es+) model that allows dynamical charge transfer among atoms. We mainly focused on the effect of the oxygen pressure on the oxidation kinetic, the chemical composition and the microstructure of the oxide films formed. The results show that oxidation kinetics as well as chemical composition and microstructure depend on the applied oxygen pressure. The oxide film thickness tends to a limiting value equal to ~3 nm. Finally, we obtained a partially crystalline oxide films for all oxygen pressures and we observed that the degree of crystallinity increases with time.

Abstract: 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 to 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.

Abstract: Variable charge molecular dynamic simulations have been performed to study the diffusion mechanisms of oxygen atoms (O) in nickel (Ni) in the temperature range 950-1600 K and the very first steps of oxidation of monocrystalline nickel surfaces at 300 K and 950 K. The oxygen diffusivity can be well described by an Arrhenius law over the temperature range considered. The oxygen diffusion coefficient has been analysed and values of Ea = 1.99 eV for the activation energy and D0 = 39 cm2.s-1 for the pre-exponential factor were obtained. The first steps growth of the oxide layer show that after the dissociative chemisorption of the oxygen molecules on nickel surface, the oxidation leads to an island growth mode as observed experimentally.

Abstract: The 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.

Abstract: In this paper we give a brief presentation of the approaches we have recently developed on the oxidation of metals. Firstly, we present an analytical model based on non-equilibrium thermodynamics to describe the reaction kinetics present during the oxidation of a metal. Secondly, we present the molecular dynamics results obtained with a code specially tailored to study the oxidation and growth of an oxide film of aluminium. Our simulations present an excellent agreement with experimental results.