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Radiochimica Acta

International Journal for chemical aspects of nuclear science and technology

Editor-in-Chief: Qaim, Syed M.


IMPACT FACTOR 2018: 1.339

CiteScore 2018: 1.20

SCImago Journal Rank (SJR) 2018: 0.333
Source Normalized Impact per Paper (SNIP) 2018: 0.720

Online
ISSN
2193-3405
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Volume 97, Issue 4-5

Issues

Solubility of plutonium in MgCl2 and CaCl2 solutions in contact with metallic iron

Marcus Altmaier / Volker Neck / J. Lützenkirchen / Thomas Fanghänel
Published Online: 2009-09-25 | DOI: https://doi.org/10.1524/ract.2009.1593

Abstract

The solubility of Pu(IV) hydrous oxide is studied at 22±2 °C under Ar atmosphere in 0.25 and 3.5 M MgCl2 (pHc≈9) and 3.5 M CaCl2 (pHc=11–12) solutions in contact with iron powder. In alkaline 3.5–4.0 M CaCl2 ternary Ca-Pu-OH complexes are formed and the solubility of PuO2·xH2O(s) increases from about 10-10 M at pHc=11 to 10-8–10-7 M at pHc=12, both in the presence and absence of Fe powder. In the presence of iron the aqueous speciation is dominated by Pu(III) at pHc<10 and by Pu(IV) complexes at pHc>10. In the absence of reducing agents the aqueous speciation is dominated by Pu(V), with significant contributions of Pu(IV) complexes at pHc>10. The effect of ternary Ca-Pu(III,IV,V)-OH complexes in alkaline CaCl2 solutions can be described by assuming complex stoichiometries and experimental data from the oxidation state analogs Cm(III)/Nd(III), Th(IV) and Np(V). The ion interaction Pitzer approach is used for model calculations.

Keywords: Plutonium; Solubility; Redox control; Iron; Ternary Ca-Pu-OH complexes

About the article

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


Published Online: 2009-09-25

Published in Print: 2009-05-01


Citation Information: Radiochimica Acta, Volume 97, Issue 4-5, Pages 187–192, ISSN (Online) 2193-3405, ISSN (Print) 0033-8230, DOI: https://doi.org/10.1524/ract.2009.1593.

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Chemical Reviews, 2013, Volume 113, Number 2, Page 1016
[2]
Marcus Altmaier, Xavier Gaona, and Thomas Fanghänel
Chemical Reviews, 2013, Volume 113, Number 2, Page 901
[3]
Volker Metz, Horst Geckeis, Ernesto Gonzáles-Robles, Andreas Loida, Christiane Bube, and Bernhard Kienzler
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Johannes Lützenkirchen
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