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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

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2193-3405
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Volume 96, Issue 9-11

Issues

Solubility of Zr(IV), Th(IV) and Pu(IV) hydrous oxides in CaCl2 solutions and the formation of ternary Ca-M(IV)-OH complexes

Marcus Altmaier / Volker Neck / Thomas Fanghänel
Published Online: 2009-09-25 | DOI: https://doi.org/10.1524/ract.2008.1535

Abstract

The solubility of Zr(IV), Th(IV) and Pu(IV) hydrous oxides is investigated at 22±2 °C in alkaline 0.1−4.5 M CaCl2 solutions. Further studies are performed with Zr(IV) over the entire pH range in NaCl and CaCl2 media, and with Zr(IV) and Th(IV) in alkaline Ca(ClO4)2 solutions. The comparison of Zr(IV) data in different ionic media (NaCl, NaClO4, CaCl2 and Ca(ClO4)2) of similar ionic strength shows that the solubility in the acidic and neutral pH range is not affected by strong interactions between the aqueous M(IV) species and the medium ions. However, in alkaline CaCl2 and Ca(ClO4)2 solutions the formation of ternary Ca-M(IV)-OH complexes causes unexpectedly high solubilities of Zr(IV) at pHc=10−12 and [Ca2+]>0.05 M and of Th(IV) at pHc=11−12 and [Ca2+]>0.5 M. The dependence of the Zr(IV) and Th(IV) solubilities on the H+ and CaCl2 concentrations shows that the complexes Zr(OH)62− and Th(OH)84− with an unusual large number of OH ligands are stabilized by the formation of associates or ion pairs with Ca2+ ions. The SIT is used to derive equilibrium constants at zero ionic strength for the complexes Zr(OH)62− (in calcium-free solutions), Ca2[Zr(OH)6]2+, Ca3[Zr(OH)6]4+ and Ca4[Th(OH)8]4+. In analogous studies with Pu(IV) hydrous oxide, the solubility increasing effect of ternary complex formation with Ca2+ ions is only observed at CaCl2 concentrations above 2 M.

Keywords: Zirconium; Thorium; Plutonium; Ternary Ca-M(IV)-OH complexes; Solubility

About the article

Published Online: 2009-09-25

Published in Print: 2008-11-01


Citation Information: Radiochimica Acta International journal for chemical aspects of nuclear science and technology, Volume 96, Issue 9-11, Pages 541–550, ISSN (Print) 0033-8230, DOI: https://doi.org/10.1524/ract.2008.1535.

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