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Issue 13, 2012
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Discriminating factors affecting incorporation: comparison of the fate of Eu3+–Cm3+ in the Sr carbonate–sulfate system

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Abstract

The aim of this work is to assess the effect of ligand strength, symmetry, and coordination number on solid solution formation of trivalent actinides and lanthanides in carbonate and sulfate minerals. This is of particular importance in radionuclide migration where trivalent actinides such as Pu, Am, and Cm are responsible for the majority of radiotoxicity after 1000 years. Time-resolved laser fluorescence spectroscopy was used to study trace concentrations of the dopant ion after interaction with the mineral phase. This study expands on previous work with aragonite and gypsum where it was found that aragonite incorporates Eu3+ and Cm3+ while only surface sorption is observed in gypsum. This study uses isostructural minerals strontianite (SrCO3) and celestite (SrSO4) to decouple the effect of structure from that due to the anion. It is demonstrated that while distribution coefficients can predict the amount of dopant ion associated with the mineral phase, they do not have any correlation with solid solution formation. This substitution mechanism is most likely dictated by the symmetry of the site being substituted and the electronic structure of the dopant atom.

Graphical abstract: Discriminating factors affecting incorporation: comparison of the fate of Eu3+–Cm3+ in the Sr carbonate–sulfate system

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Publication details

The article was received on 14 Dec 2011, accepted on 18 Jan 2012 and first published on 26 Jan 2012


Article type: Paper
DOI: 10.1039/C2DT12425D
Citation: Dalton Trans., 2012,41, 3642-3647
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    Discriminating factors affecting incorporation: comparison of the fate of Eu3+–Cm3+ in the Sr carbonate–sulfate system

    K. Holliday, A. Chagneau, M. Schmidt, F. Claret, T. Schäfer and T. Stumpf, Dalton Trans., 2012, 41, 3642
    DOI: 10.1039/C2DT12425D

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