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Radiochimica Acta

International Journal for chemical aspects of nuclear science and technology

Ed. by Qaim, Syed M.

12 Issues per year


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Formation of Cm humate complexes in aqueous solution at pHc 3 to 5.5: The role of fast interchange

Markus Freyer
  • 1 Forschungszentrum Karlsruhe, Institut für Nukleare Entsorgung, Karlsruhe, Deutschland
/ Clemens Walther / Thorsten Stumpf
  • 2 Forschungszentrum Rossendorf, Institut für Radiochemie, Dresden, Deutschland
/ Gunnar Buckau
  • 3 Forschungszentrum Karlsruhe, Institut für Nukleare Entsorgung, Karlsruhe, Deutschland
/ Thomas Fanghänel
  • 4 Europäische Komission, Institute for Transuranium Elements, Karlsruhe, Deutschland
Published Online: 2009-12-04 | DOI: https://doi.org/10.1524/ract.2009.1628

Abstract

Safety assessment of nuclear waste disposal includes determination of the possible impact of natural dissolved organic matter on the transport of actinide ions via groundwater into the biosphere. Thereby, much attention is paid to americium as it dominates the radiotoxicity of the nuclear waste after about 300 y and up to about 1000 y (spent fuel) or 100000 y (vitrified reprocessing waste). A trustworthy description of the influence benefits from a sound chemical process understanding of the americium humate complexation and transport processes. A problem in this respect is that studies by TRLFS lead to inconclusive results with respect to the nature of the complexes involved. In the present study the outcome of TRLFS measurements in H2O and D2O, and at room temperature and in liquid nitrogen are compared. It is shown that the Cm3+ ion interchanges between aquo ion (Cm3aq) and humate complex (CmHA) on a time scale of milliseconds in a pH range between 3 and 5.5. Taking this interchange into account, the process can be described in the absence of ternary complexes by the 1:1 stoichiometry formation of one curium humate complex, or a sufficiently narrow distribution of complexes to be represented by one average complex.

Keywords: Curium; Humic substances; Time resolved laser fluorescence; TRLFS

* Correspondence address: Forschungszentrum Karlsruhe, Institut für Nukleare Entsorgung, Postfach 3640, 76021 Karlsruhe, Deutschland,


Published Online: 2009-12-04

Published in Print: 2009-10-01


Citation Information: Radiochimica Acta International journal for chemical aspects of nuclear science and technology. Volume 97, Issue 10, Pages 547–558, ISSN (Print) 0033-8230, DOI: https://doi.org/10.1524/ract.2009.1628, December 2009

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