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X-ray absorption and photoelectron spectroscopy investigation of selenite reduction by FeII-bearing minerals

Scheinost, Andreas C., Kirsch, Regina, Banerjee, Dipanjan, Fernandez-Martinez, Alejandro, Zaenker, Harald, Funke, Harald, Charlet, Laurent·2008·Journal of Contaminant Hydrology
DOI 10.1016/j.jconhyd.2008.09.018
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Abstract

The long-lived radionuclide 79Se is one of the elements of concern for the safe storage of high-level nuclear waste, since clay minerals in engineered barriers and natural aquifer sediments strongly adsorb cationic species, but to lesser extent anions like selenate (SeVIO4(2-)) and selenite (SeIVO3(2-)). Previous investigations have demonstrated, however, that SeIV and SeVI are reduced by surface-associated FeII, thereby forming insoluble Se0 and Fe selenides. Here we show that the mixed FeII/III (hydr)oxides green rust and magnetite, and the FeII sulfide mackinawite reduce selenite rapidly (< 1 day) to FeSe, while the slightly slower reduction by the FeII carbonate siderite produces elemental Se. In the case of mackinawite, both S(-II) and FeII surface atoms are oxidized at a ratio of one to four by producing a defective mackinawite surface. Comparison of these spectroscopic results with thermodynamic equilibrium modeling provides evidence that the nature of reduction end product in these FeII systems is controlled by the concentration of HSe(-); Se0 forms only at lower HSe(-) concentrations related to slower HSeO3(-) reduction kinetics. Even under thermodynamically unstable conditions, the initially formed Se solid phases may remain stable for longer periods since their low solubility prevents the dissolution required for a phase transformation into more stable solids. The reduction by Fe2+-montmorillonite is generally much slower and restricted to a pH range, where selenit…

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Authors
Scheinost, A. C., Kirsch, R., Banerjee, D., Fernandez-Martinez, A., Zaenker, H., Funke, H., & Charlet, L.
Venue
Journal of Contaminant Hydrology
Publisher
Elsevier BV
Published
2008-12
Volume
102
Issue
3-4
Pages
228-245
ISSN
0169-7722
DOI
10.1016/j.jconhyd.2008.09.018
Cited by
173
References
3
Language
en
Licence
www.elsevier.com/tdm/userlicense/1.0/ (tdm)

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