Effect of natural and synthetic iron corrosion products on silicate glass alteration processes

Delphine D. Neff (1) , S. Gin (2) , Lucile Gentaz (1) , Diane Rebiscoul (3) , Philippe Dillmann (1, 4)

1 LAPA - UMR 3685 - Laboratoire Archéomatériaux et Prévision de l'Altération
2 SECM - Service d'Etudes du Comportement des Matériaux de Conditionnement
3 ICSM - UMR 5257 - Institut de Chimie Séparative de Marcoule
4 IRAMAT - LMC - IRAMAT - Laboratoire Métallurgies et Cultures

Glass long term alteration in the context of high-level radioactive waste (HLW) storage is influenced by near-field materials and environmental context. As previous studies have shown, the extent of glass alteration is strongly related to the presence of iron in the system, mainly provided by the steel overpack around surrounding the HLW glass package. A key to understanding what will happen to the glass-borne elements in the geological disposal lies in the relationship between the iron-bearing phases and the glass alteration products formed. In this study, we focus on the influence of the formation conditions (synthetized or in-situ) and the age of different iron corrosion products on SON68 glass alteration. Corrosion products obtained from archaeological iron artifacts are considered here to be true analogues of the corrosion products in a waste disposal system due to the similarities in formation conditions and physical properties. These representative corrosion products (RCP) are used in the experiment along with synthetized iron anoxic corrosion products and pristine metallic iron. The model-cracks of SON68 glass were altered in cell reactors, with one of the different iron-sources inserted in the crack each time. The study was successful in reproducing most of the processes observed in the long term archaeological system. Between the different systems, alteration variations were noted both in nature and intensity, confirming the influence of the iron-source on glass alteration. Results seem to point to a lesser effect of long term iron corrosion products (RCP) on the glass alteration than that of the more recent products (SCP), both in terms of general glass alteration and of iron transport.

Domaines: Matériaux

Delphine D. Neff, S. Gin, Lucile Gentaz, Diane Rebiscoul, Philippe Dillmann. Effect of natural and synthetic iron corrosion products on silicate glass alteration processes. Geochimica et Cosmochimica Acta, 2015, 172, pp.287-305. ⟨10.1016/j.gca.2015.09.033⟩. ⟨hal-01228556⟩