Elaboration of self-healing coatings for the development of robust materials in nuclear conditions
Description
This study aims to improve oxidation resistance of nuclear fuel claddings in accident conditions. In this context, Cr-Al-C and Cr2AlC coatings deposition and their behavior were studied. Firstly, we investigated the influence of HiPIMS process parameters on the properties of the plasma and the deposited films. Despite more intense ionic fluxes due to the HiPIMS process, coatings do not crystallize without an additional energy supply. Partially crystallized Cr2AlC thin films were obtained by a 500 C annealing of as-deposited Cr-Al-C coatings. This two-step process is a viable solution to protect nuclear claddings with Cr2AlC coating while maintaining the metallurgical properties of the zirconium based substrates. Secondly, the assessment of the oxidation resistance of as-deposited and annealed coatings revealed significant protective effect against rapid oxidation under dry and wet air at high temperatures (up to 1200 C) owing to the formation of a continuous oxide layer. During the first stages of oxidation, this layer is made of α-Al2O3 and Cr2O3 for as-deposited coating while only α-Al2O3 is present for the annealed one. Because of Al depletion, coatings later deteriorate and form a residual and porous intermediate chromium carbide (Cr7C3) layer which further fully oxidizes. It was shown that the inward diffusion of Al with Zr also accelerates the coating deterioration. To improve the oxidation resistance of these coatings, multilayered architectures were developed. Adding a molybdenum interlayer as diffusion barrier globally decreased the oxidation resistance of the coating. In contrast, topping Cr-Al-C and Cr2AlC with a Cr layer improved oxidation behavior over single-layer coatings. (author)
Abstract (French)
Dans le cadre des recherches menees sur l'amelioration de la resistance a l'oxydation des gaines de combustible en conditions accidentelles, des revetements Cr-Al-C et Cr2AlC ont ete developpes dans ce travail. Dans la premiere partie, nous avons etudie le procede HiPIMS afin de comprendre l'effet de differents parametres de depot sur le plasma et les proprietes des films obtenus. Il en ressort que malgre un bombardement ionique plus intense, un apport supplementaire d'energie est requis pour obtenir un revetement cristallin. Des recuits a partir de 500 C sous argon de systemes Cr-Al-C tels que deposes permettent ainsi une cristallisation partielle des revetements en Cr2AlC a une temperature suffisamment basse pour etre compatible avec la metallurgie des alliages de zirconium. Dans un second temps, l'evaluation du comportement a haute temperature de ces deux types de revetements, recuits ou non, a revele un effet protecteur contre l'oxydation rapide du zirconium jusqu'a 1200 C en atmosphere oxydante grace a la formation d'une couche d'oxyde continue. Cette couche est constituee d'un melange d'alumine α et de chromine pour le revetement de Cr-Al-C tandis que seule l'alumine α est presente pour le revetement Cr2AlC dans les premiers instants de l'oxydation. Ensuite, en raison de l'appauvrissement en Al, les revetements se degradent en formant une couche intermediaire residuelle de carbure Cr7C3 servant de reservoir de Cr jusqu'a complete oxydation. Ces resultats ont egalement montre la perte d'une partie du reservoir d'Al par diffusion dans les alliages Zr. Une architecture multicouche a ete developpee pour limiter cette diffusion et ainsi prolonger la duree de vie du revetement. L'ajout d'un intercalaire en Mo pour bloquer la diffusion d'Al dans le substrat s'est avere peu concluant, le molybdene s'evaporant a haute temperature. Les systemes base Cr-Al-C revetus chrome, presentent quant a eux, un comportement ameliore par rapport aux revetements monocouches
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Additional details
Additional titles
- Original title (French)
- Etude de l'elaboration de revetements autocicatrisants pour le developpement de materiaux robustes en condition nucleaire
Publishing Information
- Imprint Pagination
- 251 p.
- Report number
- CEA-R--6545
INIS
- Country of Publication
- France
- Country of Input or Organization
- France
- INIS RN
- 51097761
- Subject category
- S36: MATERIALS SCIENCE;
- Resource subtype / Literary indicator
- Thesis
- Descriptors DEI
- ACCIDENTS; ANNEALING; CRACKS; CRYSTALLIZATION; DIFFUSION; FUEL CANS; KINETICS; OXIDATION; THICKNESS; THIN FILMS
- Descriptors DEC
- CHEMICAL REACTIONS; DIMENSIONS; FILMS; HEAT TREATMENTS; PHASE TRANSFORMATIONS
Optional Information
- Notes
- 420 refs.; Available from the INIS Liaison Officer for France, see the INIS website for current contact and E-mail addresses
- Secondary number(s)
- FRCEA-TH--11802