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Titre du document / Document title

Speciation of the oxidation states of plutonium in aqueous solutions by UV/Vis spectroscopy, CE-ICP-MS and CE-RIMS

Auteur(s) / Author(s)

BÜRGER S. ; BANIK N. L. ; BUDA R. A. ; KRATZ J. V. ; KUCZEWSKI B. ; TRAUTMANN N. ;

Résumé / Abstract

For the speciation of the plutonium oxidation states in aqueous solutions, the online coupling of capillary electrophoresis (CE) with inductively coupled plasma mass spectrometry (ICP-MS) has been developed. Depending on the radius/electrical charge ratio, the oxidation states III, IV, V, and VI of plutonium are separated by CE, based on the different migration times through the capillary and are detected by ICP-MS. The detection limit is 20ppb, i.e. 109-1010 atoms (10-12-10-13 g) for one oxidation state with an uncertainty of the reproducibility of the migration times of < 1% and < 5% for the peak area. The redox kinetics of the different plutonium oxidation states in the presence of humic substances (humic and fulvic acid) have been studied. A relatively rapid reduction of Pu(VI) (10 to 1000 h) in contact with Gorleben fulvic or Aldrich humic acid could be observed, depending on the pH of the solution. Furthermore, at pH = 1, a reduction to Pu(III) and Pu(IV) in a mixture of all four oxidation states in contact with Gorleben fulvic acid after one month has been observed. In order to improve the sensitivity of the CE method, the offline coupling of CE to resonance ionization mass spectrometry (RIMS) has been explored. First applications of this new speciation method are presented.

Revue / Journal Title

Radiochimica acta    ISSN  0033-8230   CODEN RAACAP 

Source / Source

2007, vol. 95, no8, pp. 433-438 [6 page(s) (article)]

Langue / Language

Anglais

Editeur / Publisher

Oldenbourg, München, ALLEMAGNE  (1962) (Revue)

Mots-clés d'auteur / Author Keywords

Plutonium speciation

;

Oxidation state /Humic acid

;

Fulvic acid

;

Capillary electrophoresis

;

UV/Vis spectroscopy /ICP-MS/RIMS

;

Localisation / Location

INIST-CNRS, Cote INIST : 10156, 35400016146764.0010

Nº notice refdoc (ud4) : 18955175



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