Calcium silicate hydrate (C-S-H) gel solubility data and a discrete solid phase model at 25 °C based on two binary non-ideal solid solutions

The interaction of EDTA with calcium silicate hydrate (C-S-H) and its impact on the sorption of U(VI) by C-S-H in the presence of EDTA at varying concentrations has been investigated under N2 and ambient atmosphere. The solid phase characterization was performed by FTIR, XRD and TGA measurements and the uranium concentration in solution has been determined by alpha-spectroscopy. At increased EDTA concentrations ([EDTA] > 0.1 M) calcium is complexed and extensively extracted from the solid resulting in a quantitative dissolution of the Ca(OH)2 phase and deterioration of C-S-H. At lower EDTA concentrations ([EDTA] ≤ 0.01 M), EDTA is sorbed into the solid phase and the associated adsorption capacity (qmax = 0.67 mol/kg) has been evaluated by fitting the corresponding data with the Langmuir isotherm model. The incorporation of EDTA in the C-S-H matrix was corroborated by FTIR, XRD and TGA measurements. Regarding the effect of EDTA on the U(VI) sorption by C-S-H, evaluation of the experimental data reveal a significant decrease of the Kd values in the presence of EDTA most probably due to the stabilization of U(VI) in the form of U(VI)-EDTA complexes in solution. Under ambient conditions a further decrease of the Kd values is observed because of the formation of U(VI)-carbonato complexes related to CO2 dissolution and hydrolysis.

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Evaluation of Sorption Behavior of Iodide Ions on Calcium Silicate Hydrate and Hydrotalcite

MRS Proceedings ◽

10.1557/opl.2015.336 ◽

2015 ◽

Vol 1744 ◽

pp. 29-34

Author(s):

Taiji Chida ◽

Jun Furuya ◽

Yuichi Niibori ◽

Hitoshi Mimura

Keyword(s):

Calcium Silicate ◽

Calcium Silicate Hydrate ◽

Solid Phase ◽

Pure Water ◽

Weight Ratio ◽

Cementitious Materials ◽

Sorption Behavior ◽

Nacl Solution ◽

Iodide Ions ◽

Engineered Barriers

ABSTRACTThe migration retardation of anionic radionuclides, notably I-129, in radioactive waste repositories is one of the most critical factors for improving the performance of engineered barriers. To gain more fundamental knowledge required to make such improvements, this study examined the sorption behavior of iodide ions on calcium silicate hydrate (CSH) and hydrotalcite (HT), which act as anion exchangers. CSH was synthesized using CaO and fumed silica, with Ca/Si molar ratios ranging from 0.4 to 1.6. The weight ratio of CSH to HT was 1.0. These solid samples were immersed for 14 days in a 30 mL sample of pure water or 0.6 M NaCl solution, each of which contained 0.5 mM iodide ions with a given liquid/solid weight ratio (10, 15, or 20). Raman spectroscopy studies indicated that the structures of CSH and HT were maintained during the hydration of the solid phase and the sorption of iodide ions. The distribution coefficients for the sorption of iodide ions on CSH and HT ranged from 6 to 13 L/kg for pure water and from 1 to 2 L/kg for NaCl solution. These retardation effects for iodide ions would contribute toward improving the performance of the repository system as most conventional safety assessments assume that iodide ions hardly sorb on engineered barriers such as cementitious materials.

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