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• W3210347991 abstract "Document available in extended abstract form only. In the context of the geological disposal of high-level radioactive waste, it is of prime importance to understand the interaction mechanisms between the geological matrix, Callovo-Oxfordian clay rock (COx) and metallic iron, from the package overpack. In order to evidence the individual role of each clay component entering in the mineralogy of the COx, interactions between metallic iron and pure clays (smectites, illite and kaolinite) were first conducted. To investigate the role of the other minerals, the reactivity of COx, COx clay fraction (COxCF) and mixtures between COxCF and quartz, calcite or pyrite, was studied. Clays and additional minerals were put in contact with powder metallic iron with a weight ratio iron:clay fixed at 1:3 and a clay:solution ratio of 1:20. Proportions of non-clay minerals were deduced from the average COx composition: 50% clays, 24.5% quartz, 24.5% calcite and 1% pyrite. Batch experiments were carried out in anoxic conditions at 90 deg. C in the presence of background electrolyte (NaCl 0.02 M.L{sup -1}, CaCl{sub 2} 0.04 M.L{sup -1}) in Parr reactors for durations of one, three or nine months. After reaction, solid and liquid phases were separated by centrifugation and characterized by classical techniques combining chemical analyses (liquid analyses, transmission electron microscopy combined with Energy Dispersive of X-rays spectroscopy TEM-EDS), mineralogical (X-ray diffraction), spectroscopic ({sup 57}Fe Moessbauer) and morphometric techniques (TEM, scanning electron microscopy and N{sub 2} adsorption). For COx, COxCF and all the pure clay phases, major evolutions were observed during the first month, which shows that the oxidation of metallic iron is rapid in our experimental conditions. Release of iron cations in solution, pH increase (8-10) and Eh decrease (reductive conditions) are responsible for the partial dissolution of initial clay phases. Released iron is involved in the crystallization of Fe-serpentines, berthierine or odinite mainly or precipitates under the form of magnetite in low amount. Even if COx-iron and COxCF-iron interactions appear somehow similar, significant differences can be noticed in both the liquid and solid compartments of the reaction products. As far as solutions are concerned, pH is lower and Eh higher for COx compared with COxCF. In the solid phase, after 9 months of reaction, metallic iron is totally consumed in COx whereas it is still present for COxCF. In parallel, the formation of magnetite is negligible for COx. Upon reaction, the Al:Si ratio decreases in COx clay particles whereas it remains stable for COxCF. Finally, the evolution of specific surface areas (SSA) with reaction time is significantly different as an increase in SSA is observed for COx in contrast with a decrease for COxCF. The addition of either calcite or pyrite to COxCF does not significantly influence its interaction with iron. In contrast, the addition of quartz to COxCF leads to a pH decrease and an Eh increase. It also results in the quasi-complete absence of magnetite, a decrease of Al:Si ratio in clay particles and an increase in SSA. Upon quartz addition COxCF almost behaves as COx with regard to interactions with iron. Such a trend can be assigned to the partial dissolution of quartz, that provides additional silica for the precipitation of Fe-serpentines. As a conclusion, the main differences between COx-iron and COxCF-iron interactions can thus be explained by the presence and reactivity of quartz which modify the reaction pathway and products. (authors)" @default.
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• W3210347991 date "2012-10-15" @default.
• W3210347991 modified "2023-09-27" @default.
• W3210347991 title "Influence of non-clay minerals on the interaction between metallic iron and Callovo-Oxfordian clay fraction" @default.
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