Evaluation of rare earth on layered silicates under subcritical conditions: Effect of the framework and interlayer space composition

Clay-based minerals are considered to be an important component in backfill barriers due to both their ability to seal and adsorb radioactive waste and to interact chemically with it under subcritical conditions. Herein, we describe a systematic study of the properties of layered silicates that coul...

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Bibliographic Details
Authors: Chain Villar, Pablo; Cota Reguero, Agustín; Pavón González, Esperanza; Pazos Zarama, Mery Carolina; Alba Carranza, María Dolores
Format: Article
Status:Submitted version
Publication date:2013
Country:España
Institution:Universidad de Sevilla (US)
Repository:idUS. Depósito de Investigación de la Universidad de Sevilla
OAI Identifier:oai:idus.us.es:11441/70496
Online Access:https://hdl.handle.net/11441/70496
https://doi.org/10.1016/j.chemgeo.2013.03.006
Access Level:Open access
Keyword:Subcritical conditions
Hydrothermal 35 treatment
Rare-earth
Radioactive waste
Engineered barrier
X-ray diffraction
MAS-NMR
Disilicates
Bentonite
Smectite
Description
Summary:Clay-based minerals are considered to be an important component in backfill barriers due to both their ability to seal and adsorb radioactive waste and to interact chemically with it under subcritical conditions. Herein, we describe a systematic study of the properties of layered silicates that could affect their hydrothermal reactivity, namely type of layers, octahedral occupancy, origin and total amount of the layer charge, and nature of the interlayer cation. The silicates studied were selected on the basis of their different characteristics associated with these properties and were treated hydrothermally at 300 °C for 48 h in a 7.3 · 10− 2 M Lu(NO3)3 · 3.6H2O solution. The final products were analyzed by X-ray diffraction and solid-state NMR spectroscopy. All the layered silicates studied were found to be able to generate a Lu2Si2O7 phase after hydrothermal treatment under subcritical conditions, thereby confirming the participation of a chemical mechanism of the clay barrier generating phases being stables with temperature and pH conditions. However, the extent of this reaction depends to a large extent on the physicochemical properties of the framework and the interlayer space composition, such as the presence or absence of an octahedral sheet, the degree of occupancy of this sheet, and the origin and total layer charge. Therefore, this study allows tuning the clay mineral framework characteristic that favors the rare earth cations (as trivalent actinide simulator) immobilization.