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Stability of Th(IV) polymers measured by electrospray mass spectrometry and laser-induced breakdown detection

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Abstract

The formation of polynuclear thorium hydroxide complexes in acidic aqueous solutions is observed by electrospray mass spectrometry. Size, number of hydroxide ligands and charge of all complexes in solution are identified independently. By repeated measurements over a time span of up to 418 days the stability of the polymers is observed. At concentrations above [Th(IV)]tot = 10 mM pentamers and dimers are the dominant stable species. In contrast, the fractions of pentamers initially present at [Th(IV)]tot = 0.2 mM decrease within less than 4 weeks, correlated with the formation of nm-sized colloids observed by LIBD indicating an Ostwald-ripening like process.

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Acknowledgments

We thank Marcus Altmaier (INE) for preparation of the stock solution and, together with Volker Neck, for many fruitful discussions. We also thank Oliver Schwindt for LIBD and the INE analytics group for ICP MS measurements. Finally, we acknowledge financial support by the “Programm Nuklear” and by the “Helmholtz Russia Joint Research Group” of the Helmholtz Gemeinschaft Deutscher Forschungszentren (HGF).

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Authors and Affiliations

  1. Institute for Nuclear Waste Disposal, Forschungszentrum Karlsruhe, P.O. Box 3640, 76021, Karlsruhe, Germany

    Clemens Walther, Markus Fuss, Sebastian Büchner & Horst Geckeis

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  1. Clemens Walther
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  2. Markus Fuss
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  3. Sebastian Büchner
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  4. Horst Geckeis
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Correspondence to Clemens Walther.

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Walther, C., Fuss, M., Büchner, S. et al. Stability of Th(IV) polymers measured by electrospray mass spectrometry and laser-induced breakdown detection. J Radioanal Nucl Chem 282, 1003–1008 (2009). https://doi.org/10.1007/s10967-009-0158-8

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  • DOI: https://doi.org/10.1007/s10967-009-0158-8

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