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The immobilization of U(VI) by C-S-H phases under conditions relevant for the cementitious near field of a repository for radioactive waste has been investigated. C-S-H phases have been synthesized using two different procedures: the "direct reaction" method and the "solution reaction" method.The stabilities of alkaline solutions of U(VI) (presence of precipitates or colloidal material) were studied prior to sorption and co-precipitation tests in order to determine the experimental U(VI) solubility limits. These U(VI) solubility limits were compared with the U(VI) solubilities obtained from thermodynamic speciation calculations assuming the presence of combinations of different solid U(VI) phases. The solid phase controlling U(VI) solubility in the present experiments was found to be CaUO 4 (s).The U(VI) uptake kinetics and sorption isotherms on C-S-H phases with different C:S ratios were determined under various chemical conditions; e.g., sorption and co-precipitation experiments and different pH's. U(VI) was found to sorb fast and very strongly on C-S-H phases with distribution ratios (R d values) ranging in value between 10 3 L kg -1 and 10 6 L kg -1 . Both sorption and co-precipitation experiments resulted in R d values which were very similar, thus indicating that no additional sorption sites for U(VI) were generated in the co-precipitation process. Furthermore, C-S-H synthesis procedures did not have a significant influence on U(VI) uptake. The U(VI) sorption isotherms were found to be non-linear, and further, increasing Ca concentrations resulted in increasing U(VI) uptake. The latter observation suggests that U(VI) uptake is controlled by a solubility-limiting process, while the former observation further indicates that pure Ca-uranate is not the solubility-limiting phase. It is proposed that a solid solution containing Ca and 2 2 UO + could control U(VI) uptake by C-S-H phases.

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The sorption behavior of europium onto two iron-oxides, goethite and magnetite, focused on the effect of carbonate species concentration was investigated in 0.01 M NaClO4 solution by the batch method over a pH range of 4 to 11. It was found that sorption of europium was enhanced in the higher concentration solution of carbonate species for both materials. The zeta-potential of goethite in the solutions including sodium bicarbonate was also measured to estimate the effect of sorbed carbonate species. Our experimental results and model calculation suggest that the production of surface carboxylic group FeOCOO by the sorption of carbonate species lowered the zeta-potential and enhanced europium sorption.