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Radiochimica Acta

International Journal for chemical aspects of nuclear science and technology

Ed. by Qaim, Syed M.


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2193-3405
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New insights in the formation processes of Pu(IV) colloids

Clemens Walther* / Jörg Rothe1 / Boris Brendebach2 / Markus Fuss3 / Marcus Altmaier4 / Christian M. Marquardt5 / Sebastian Büchner6 / Hye-Ryun Cho7 / J.-I. Yun8 / Alice Seibert9

1 Forschungszentrum Karlsruhe, Institut für Nukleare Entsorgung, Karlsruhe, Deutschland

2 Forschungszentrum Karlsruhe, Institut für Nukleare Entsorgung, Karlsruhe

3 Institut für Nukleare Entsorgung, Forschungszentrum Karlsruhe, Karlsruhe

4 Forschungszentrum Karlsruhe, Institut für Nukleare Entsorgung, Karlsruhe, Deutschland

5 Forschungszentrum Karlsruhe, Institut für Nukleare Entsorgung, Karlsruhe, Deutschland

6 Forschungszentrum Karlsruhe, Institut für Nukleare Entsorgung, Karlsruhe

7 Nuclear Chemistry Research Division, Korea Atomic Energy Research Institute, Republik Korea

8 Dept. of Nuclear and Quantum Engineering, Republik Korea

9 European Commission, JRC, Inst. For Transuranium Elements, Karlsruhe, Deutschland

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

Citation Information: Radiochimica Acta. Volume 97, Issue 4-5, Pages 199–207, ISSN (Online) 2193-3405, ISSN (Print) 0033-8230, DOI: 10.1524/ract.2009.1595, September 2009

Publication History

Published Online:
2009-09-25

Abstract

The high tendency of tetravalent plutonium to form polymeric complexes and colloids is well known but the exact processes underlying their formation are still controversially discussed. In the present work, the nucleation of small polynuclear hydroxide complexes, i.e. , ionic species containing more than one Pu ion, their aggregation and formation of larger colloids (polymers exceeding some 5 nm in size) and finally ripening processes of freshly formed amorphous Pu(IV) colloids towards more crystalline particles are investigated by use of a combination of various spectroscopic techniques. By electrospray mass-spectrometry small polymers such as dimers, trimers and tetramers containing mixed oxidation states of Pu were observed. These polymers might be responsible for the equilibration between the Pu(III)/Pu(IV) and the plutonyl species Pu(V)/Pu(VI) even in dilute solutions in the absence of colloids or precipitates.

Keywords: Plutonium; Hydrolysis; Polymerization; Colloids; EXAFS

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