Study of corrosion processes and irradiation effect on aluminium alloys used for research reactors material structure
Description
Materials Testing Reactors (MTR) are experimental nuclear reactors used to irradiate materials. Aluminium alloys, in particular the 6061-T6, are used in MTR of the core components and for the fuel cladding. In the aqueous media of the core, these alloys are corroded and an aluminium hydroxide film covers their surface. Because of a low thermal conductivity, this film degrades the thermal exchange between the core components and the aqueous media; this can lead to an overheating of the reactor. As a result, it is important to determinate the hydroxide thicknesses on the surface of the aluminium alloys. In the literature, empirical models have been developed to predict these thicknesses depending on the operational conditions of the reactors. Tests in corrosion loop have been performed at a temperature superior to 100 C. The data resulting of these tests is used to extrapolated the empirical models. However, in the French reactors, the maximal temperature of the core components is between 70 and 100 C. Thus, in order to use the empirical models in the French reactors, their application range should be extended to a temperature inferior to 100 C. With this goal, parametric studies are performed with different temperatures (70-100 C), pressures (0.5-12 bar) and pH (5-7.5). These studies indicate that the temperature and the pH have an important impact on the aluminium corrosion and on the hydroxide growth. The hydroxide thicknesses are more important at 70 C than at 100 C. This observation is due to a change in the crystalline phase of aluminium hydroxide: the hydroxide formed at 70 C is less protective for the aluminium oxidation than the one at 100 C. The pH influences the hydroxide solubility and thus the hydroxide thicknesses, a pH of 5 allows to reduce these thicknesses compared to 7.5. However, the data collected during these parametric studies does not allow to adapt the empirical models to a temperature inferior to 100 C, this is due to variations of pH during corrosion tests and to a too low evolution of the hydroxide thicknesses. As a result, more tests with corrosion loop are needed. In addition, in the reactor, the 6061-T6 alloy is exposed to neutron irradiation. According to the literature, this irradiation increases the aluminium corrosion. Ion irradiations have been performed in order to evaluate if it is possible to use ion irradiations to approach the conditions found in nuclear core. The first irradiation with Al ions is performed on the non-corroded metal with at most 14 dpa; this causes an amorphization of the dispersoids and increases the dislocation density. These types of damage seem to increase the hydroxide growth and the aluminium corrosion. The second irradiation with Al ions is performed on aluminium hydroxide with at most 4.5 dpa. This causes a change in the microstructure of the hydroxide crystals (from parallelepiped, they become globular), the formation of cavity and the dehydration of the hydroxide resulting in the formation of nanocrystallites of oxide η-Al2O3. These types of damage seem to increase the hydroxide growth. The effects of the ionic irradiations are compared to the results of a neutron irradiation performed in the reactor Osiris at the CEA of Saclay. The both types of irradiation are similar effects on the aluminium corrosion. As a result, tests in a corrosion loop coupled with ion irradiations would be used to enrich the database used to extrapolate the empirical models to temperature inferior to 100 C. (author)
Abstract (French)
Les Materials Testing Reactors (MTR) sont des reacteurs experimentaux nucleaires utilises dans le but d'irradier des materiaux. Les alliages d'aluminium en particulier l'alliage 6061-T6 sont utilises dans les MTR pour les gaines de combustibles ou les elements de structures du coeur nucleaire. Dans le milieu aqueux du coeur, ces alliages se corrodent et un film d'hydroxyde d'aluminium recouvre leur surface. Ayant une mauvaise conductivite thermique, ce film degrade les echanges thermiques entre les elements du coeur et le milieu aqueux, ce qui peut mener a une surchauffe. Il est donc important d'etudier la corrosion des alliages d'aluminium et de determiner les epaisseurs d'hydroxyde a leur surface. Pour cela, il existe dans la litterature des modeles empiriques qui permettent d'estimer les epaisseurs d'hydroxyde selon les conditions de fonctionnement des reacteurs. Ces modeles ont ete extrapoles a partir de donnees obtenues a la suite d'essais realises en boucle de corrosion a une temperature superieure a 100 C. Dans les reacteurs experimentaux francais, la temperature maximale des elements de structures du coeur est comprise entre 70 et 100 C. Ainsi, pour pouvoir utiliser ces modeles empiriques dans les reacteurs francais, il est necessaire d'elargir leur domaine d'application aux temperatures inferieures a 100 C. Pour cela, des etudes parametriques ont ete menees avec differentes valeurs de temperature (70-100 C), de pression (0,5-12 bar) et de pH (5-7,5). Il est montre que la temperature possede un important impact: l'alliage 6061-T6 se corrode plus et les epaisseurs d'hydroxydes sont plus importantes a 70 C qu'a 100 C. Ces observations sont associees a un changement de phase cristalline d'hydroxyde d'aluminium: l'hydroxyde forme a 70 C est moins protecteur que celui a 100 C. Le pH possede lui aussi un fort impact sur la croissance de l'hydroxyde. Notamment, un pH de 5 permet de diminuer les epaisseurs d'hydroxyde compare a un pH de 7,5. Cependant, ces etudes parametriques ne permettent pas d'adapter les modeles empiriques a une temperature inferieure a 100 C a cause de variations de pH en cours d'essai et d'une trop faible evolution des epaisseurs d'hydroxyde. D'avantages essais en boucle de corrosion sont necessaires.Aussi, en reacteur, l'alliage 6061-T6 se corrodent sous flux neutronique. Selon la litterature, cette irradiation accelere la corrosion des alliages d'aluminium. Dans le but de savoir s'il est possible de se rapprocher des conditions trouvees en reacteur avec des irradiations ioniques, des irradiations aux ions ont ete realisees sur le metal non corrode et sur l'hydroxyde. Une premiere irradiation aux ions Al realisee sur la matrice d'aluminium a 14 dpa au maximum provoque une amorphisation des dispersoides et une augmentation du nombre de dislocations. Ces deux types de dommages semblent causer une augmentation des epaisseurs d'hydroxyde et de l'oxydation de l'aluminium. Ensuite, une deuxieme irradiation aux ions Al a ete realisee sur l'hydroxyde pour un niveau de dommage de 4,5 dpa au maximum. L'irradiation provoque un changement de microstructure des cristaux d'hydroxyde (de parallelepipediques, ils deviennent globulaires), la formation de cavite et une deshydratation de l'hydroxyde se traduisant par la formation de nanocristallites d'oxyde η-Al2O3. Ces dommages d'irradiation semblent provoquer une augmentation de la croissance de l'hydroxyde. Ces effets des irradiations ioniques ont ete compares a ceux d'une irradiation aux neutrons realisee dans le reacteur Osiris au CEA Saclay. Il est montre que les deux types d'irradiations ont des effets similaires. Ainsi, pour la suite, il sera possible d'utiliser une boucle de corrosion couplee a des irradiations ioniques dans le but d'enrichir la base de donnees utilisee pour extrapoler les modeles empiriques de la litterature aux temperatures inferieures a 100 C
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Additional details
Additional titles
- Original title (French)
- Etude des mecanismes de corrosion et des effets d'irradiation sur la corrosion d'un alliage d'aluminium utilise dans les reacteurs nucleaires experimentaux
Publishing Information
- Imprint Pagination
- 173 p.
- Report number
- FRCEA-TH--13633
INIS
- Country of Publication
- France
- Country of Input or Organization
- France
- INIS RN
- 53017514
- Subject category
- S36: MATERIALS SCIENCE;
- Resource subtype / Literary indicator
- Thesis
- Descriptors DEI
- ALUMINIUM ALLOYS; ALUMINIUM HYDROXIDES; CORROSION; EXTRAPOLATION; MICROSTRUCTURE; OSIRIS REACTOR; OXIDATION; PH VALUE; SOLUBILITY; SURFACES; TEMPERATURE DEPENDENCE; THICKNESS
- Descriptors DEC
- ALLOYS; ALUMINIUM COMPOUNDS; CHEMICAL REACTIONS; DIMENSIONS; ENRICHED URANIUM REACTORS; HYDROGEN COMPOUNDS; HYDROXIDES; IRRADIATION REACTORS; MATERIALS TESTING REACTORS; MATHEMATICAL SOLUTIONS; NUMERICAL SOLUTION; OXYGEN COMPOUNDS; REACTORS; RESEARCH AND TEST REACTORS; RESEARCH REACTORS; TANK TYPE REACTORS; THERMAL REACTORS; WATER COOLED REACTORS; WATER MODERATED REACTORS
Optional Information
- Notes
- 172 refs.; Available from the INIS Liaison Officer for France, see the INIS website for current contact and E-mail addresses