期刊
GEOCHIMICA ET COSMOCHIMICA ACTA
卷 73, 期 4, 页码 990-1003出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.gca.2008.11.017
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资金
- National Cooperative for the Disposal or Radioactive Waste (Nagra), Wettingen, Switzerland
In this study the physico-chemical, titration and sorption characteristics of Na-illite du Puy (Na-illite) have been measured and modelled. Samples of illite, collected in the region of le Puy-en-Velay, France, were purified and conditioned to the Na-form and physico-chemically characterised. Potentiometric titrations on suspensions of the Na-illite were carried out using a batch backtitration technique in 0.01, 0.1 and 0.5 M NaClO4 background electrolytes from pH similar to 3 to similar to 11.5 in an inert atmosphere glove box. The supernatant solutions from each titration experiment in each series were analysed for K, Mg, Ca, Sr, Si, Al, Fe and Mn. The titration data were modelled in terms of the protolysis of two amphoteric edge sites (equivalent to(SOH)-O-w1 and equivalent to(SOH)-O-W2) without an electrostatic term. Sorption edges (solid/liquid distribution ratios versus pH at trace sorbate concentrations and constant ionic strength) were determined for the transitions metals Ni(II) and Co(II), the lanthanide Eu(III), and the heavy metal Sn(IV) on Na-illite with NaClO4 as the background electrolyte under anoxic conditions (CO2 <= 2 ppm, O-2 <= 2 ppm). The study thus encompasses a broad range of metals with different thermodynamic characteristics and with valence states ranging from II to IV. The results from the modelling of the titration data, in combination with a non electrostatic surface complexation and cation exchange sorption model were applied to quantitatively describe the uptake characteristics of the metals listed above on Na-illite. Since sorption edges were measured at trace concentrations, metal uptake was modelled as occurring on strong type sites (equivalent to(SOH)-O-s) only. This sorption model, the two site protolysis non electrostatic surface complexation and cation exchange model (2SPNE SC/CE model) had been previously developed and used to describe metal uptake on montmorillonite. (C) 2008 Elsevier Ltd. All rights reserved.
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