Abstract
One of the French options for the final disposal of high-level radioactive waste is a deep geological repository. The Callovo-Oxfordian formation in the Meuse and Haute-Marne (France) was proposed, by the French agency for the management of radioactive wastes (ANDRA), to be the site of a research laboratory in order to evaluate in situ the interaction between the host formation and the engineered barriers. In the previous experimental part, secondary minerals such as zeolites, tobermorite and katoite have been observed after the alteration of the Callovo-Oxfordian clay under alkaline conditions. Three different reactions of phyllosilicates alteration have been proposed as a function of both pH and chemical composition of the reacting solutions. The aim of this work was to simulate the reaction between the Callovo-Oxfordian clay and high-pH solutions in order to validate the proposed alteration reactions from experimental data. The thermodynamic modelling of stability relationships among minerals in the Callovo-Oxfordian clay was performed using the solution speciation solubility modelling code KINDIS at 120 °C for different chemical media (NaOH, KOH and Ca(OH) 2). Input data were the mineralogical composition of the <2 μm fraction of Callovo-Oxfordian clay at nearly the same burial depth of the underground laboratory construction as well as the neoformed minerals observed after the experimental alteration of this clay (zeolites and cement phases). In the NaOH and KOH runs, anacime, phillipsite and chabazite, respectively were the first stable minerals which appeared at the beginning of modelling. In the Ca(OH) 2 runs, oversaturated with respect to portlandite, katoite and then tobermorite were the first minerals occurring at the beginning of the alteration. Smectites and illites were undersaturated whatever the chemical composition. Both minerals and the interstratified illite-smectite were less stable in Ca(OH) 2 than in NaOH and KOH solutions. Concerning the secondary minerals, a discussion is developed in order to improve modelling and to predict the long term reactions between clays and alkaline solutions.
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