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AbstractAbstract
[en] During their aqueous alteration, AVM French nuclear glasses exhibit a large range of behaviour, in spite of a small range of composition. AVM glasses alteration rates are controlled by two phenomena: (i) precipitation of secondary phases, mostly aluminous hectorites, and (ii) diffusion of water across a more or less protective gel. The magnesium contained in these glasses increases the precipitation of these secondary phases, leading to a partial or total dissolution of the gel layer. This dissolution increases the glass alteration rates. On the other hand, Mg also incorporates in the gel, increasing his passivation properties. The predominance of one of these two phenomena depends on the initial composition of the glass, the pH of the solution, and the alteration conditions. In presence of Bure geological disposal site water (Mg and Ca rich), AVM glasses undergo less alteration than in initially pure water, in spite of larger amounts of secondary phase precipitates. This results from incorporation of calcium in the gel instead of sodium and magnesium, improving its passivating properties. We have adapted the geochemical GRAAL model for AVM glasses. In spite of its limitations, this model allows us to describe the differences of behaviour between these glasses, in function of their composition. Moreover, GRAAL can be proposed as a basis of a future operational model for predicting the alteration of AVM glasses. (author)
[fr]
En milieu aqueux, les verres nucleaires AVM presentent de grandes differences de comportement a l'alteration, malgre de faibles variations de composition. La vitesse residuelle d'alteration de ces verres est controlee par deux phenomenes, qui sont la precipitation de phases secondaires de type hectorites alumineuses, qui en alterant le gel protecteur, augmentent la vitesse residuelle d'alteration du verre, et, la diffusion de l'eau a travers un gel plus ou moins protecteur. Le magnesium, contenu dans ces verres, facilite la precipitation de ces phases secondaires, mais s'incorpore egalement dans le gel, augmentant son pouvoir de passivation. La predominance de l'un ou l'autre de ces phenomenes depend de la composition initiale du verre, du pH de la solution, des conditions d'alteration. Alteres en eau souterraine de stockage (riche en Mg et Ca), les verres AVM s'alterent moins qu'en eau pure, et ce malgre la precipitation de phases secondaires. Le calcium s'incorpore dans le gel, a la place du sodium et du magnesium, augmentant son pouvoir de passivation. Nous avons adapte le modele geochimique d'alteration des verres GRAAL, aux verres AVM. Malgre ses limites, ce modele nous permet de rendre compte des differences de comportement entre les verres AVM, selon leur composition, ainsi que de servir de base a un futur modele operationnel de l'alteration des verres AVMOriginal Title
Developpement des bases theoriques necessaires a la modelisation de la vitesse residuelle d'alteration en milieu aqueux des verres nucleaires AVM
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3 Dec 2010; 412 p; CEA-R--6299; [140 refs.]; Available from the INIS Liaison Officer for France, see the 'INIS contacts' section of the INIS-NKM website for current contact and E-mail addresses: http://www.iaea.org/INIS/contacts/; Chimie des Materiaux
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