Immobilisation of Uraniumvi in Cementitious Materials: Evidence for Structural Incorporation in Calcium–Silicate–Hydrates and Solid Solution Formation View Full Text


Ontology type: schema:Chapter     


Chapter Info

DATE

2012

AUTHORS

J. Tits , X. Gaona , N. Macé , D. Kulik , T. Stumpf , C. Walther , G. Geipel , E. Wieland

ABSTRACT

Cementitious materials are an important component in the multi-barrier concepts developed in many countries for the safe storage of low and intermediate level (L/ILW) radioactive waste in deep geological repositories. Reliable thermodynamic models able to predict the interaction between radionuclides and cementitious materials in the long term are important for performance assessment. The development of such models requires a sufficiently detailed macroscopic and molecular-level understanding of the uptake processes involved. This study applied wet chemistry and luminescence spectroscopy to determine speciation of UVI in cementitious materials. Batch sorption experiments on hardened cement paste (HCP) and its main constituent calcium–silicate–hydrate (C–S–H) phases were used to quantify UVI uptake and investigate the effect of changes in solution chemistry and solid composition on the nature of the UVI sorbed species. Complementary to wet chemistry, laser-induced luminescence spectroscopy studies on UVI doped HCP and C–S–H pastes has provided information on local coordination of sorbed UVI species. Wet chemistry studies and luminescence investigations showed that in HCP samples, UVI was predominantly bound to C–S–H. UVI uptake by HCP and C–S–H phases was found to be fast and sorption distribution ratios (R d values) were very high, indicating strong retention by the solids. In addition, a strong dependence of pH and CaO:SiO2 ratio was observed. Luminescence spectra of UVI-doped C–S–H phases were similar to UVI in the natural uranyl silicate soddyite, indicating comparable coordination of bound UVI, thus suggesting that sorbed UVI is incorporated in the interlayer of the C–S–H structure. Decay profile analysis combined with factor analysis of series of spectra of UVI – C–S–H suspensions, recorded with increasing delay times, revealed the presence of two luminescent sorbed UVI species in agreement with the wet chemistry data. At least the stronger sorbing species is incorporated in the C–S–H structure whereas the weaker sorbing species might be either an incorporated species or a surface complex. The high recrystallization rates found for C–S–H phases together with the information obtained from the wet chemistry and luminescence spectroscopy studies suggest that UVI uptake by C–S–H phases may be described by a solid solution model. A sub-lattice ideal solid solution model with three C–S–H end-members and three UVI-bearing end-members has been developed. More... »

PAGES

699-706

References to SciGraph publications

  • 1992. Electronic structure and bonding in actinyl ions in COMPLEXES, CLUSTERS AND CRYSTAL CHEMISTRY
  • Book

    TITLE

    Proceedings of the 10th International Congress for Applied Mineralogy (ICAM)

    ISBN

    978-3-642-27681-1
    978-3-642-27682-8

    Identifiers

    URI

    http://scigraph.springernature.com/pub.10.1007/978-3-642-27682-8_84

    DOI

    http://dx.doi.org/10.1007/978-3-642-27682-8_84

    DIMENSIONS

    https://app.dimensions.ai/details/publication/pub.1017535790


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