Effects of temperature, pH, and iron/clay and liquid/clay ratios on experimental conversion of dioctahedral smectite to berthierine, chlorite, vermiculite, or saponite
Mosser-Ruck, Regine (Nancy-Université)
Cathelineau, Michel (Nancy-Université)
Guillaume, Damien (Observatoire Midi-Pyrénées)
Charpentier, Delphine (Université de Franche-Comté)
Rousset, Davy (G2R, Nancy-Université)
Barres, Odile (Laboratoire Environnement et Minéralurgie)
Michau, Nicolas (ANDRA. Direction Scientifique/Service Matériaux. Parc de la Croix Blanche)

Data:	2010
Resum:	In deep geological repositories for high-level nuclear wastes, interactions between steel canisters and clay-rich materials may lead to mineralogical transformations with a loss of the confining properties of the clays. Experiments simulating the conversion of smectite to Fe-rich clay phases in contact with Fe metal have been carried out to evaluate such a possibility by taking into account the effects of a series of critical parameters, including temperature, pH, and Fe/clay (Fe/C) and liquid/clay (L/C) ratios. The mineralogical and chemical transformations observed in these experiments have been compared with data from the literature, and subsequently used to propose a conceptual model for the main mineralogical transformations which can be expected in clay formations surrounding high-level nuclear waste repositories. In the presence of Fe metal and under low oxygen fugacity (<10) the main mineralogical sequences are as follows: (1) up to 150° C, under neutral pH, and L/C > 5: dioctahedral smectite (di-sm) → 7 A° Fe-rich phase (berthierine, odinite-cronstedtite) for large Fe/C ratios (>0. 5), or di-sm → Fe-rich di-sm + Fe-rich trioctahedral smectite (tri-sm) for small Fe/C ratios (0. 1); (2) up to 150C, under alkaline pH (10-12), and L/C > 5: di-sm → Fe di-sm (±palygorskite) for a small Fe/C ratio (0. 1); (3) at 300°C, Fe/C = 0. 1, and L/C > 5: di-sm → Fe-rich saponite → trioctahedral chlorite + feldspar + zeolite (near-neutral pH); di-sm → Fe-rich vermiculite + mordenite (pH 10-12). Low temperatures (<150°C) and large L/C and Fe/C ratios seem to favor the crystallization of the serpentine group minerals instead of Fe-rich trioctahedral smectites or chlorites, the latter being favored by higher temperatures. The role of L/C and Fe/C ratios and the competition between them at different temperatures is a crucial point in understanding the transformation of smectite in contact with Fe metal.
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Llengua:	Anglès
Document:	Article ; recerca ; Versió publicada
Matèria:	Berthierine ; Chlorite ; Fe Metal ; Nuclear Waste ; Saponite ; Smectite ; Vermiculite
Publicat a:	Clays and Clay Minerals, Vol. 58, Núm. 2 (2010) , p. 280-291, ISSN 1552-8367

DOI: 10.1346/CCMN.2010.0580212

12 p, 775.5 KB  Accés restringit a la UAB

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