Details
| Originalsprache | Englisch |
|---|---|
| Seiten (von - bis) | 89-95 |
| Seitenumfang | 7 |
| Fachzeitschrift | Radiochimica Acta |
| Jahrgang | 95 |
| Ausgabenummer | 2 |
| Publikationsstatus | Veröffentlicht - 11 Apr. 2007 |
| Extern publiziert | Ja |
Abstract
The hydrolysis of tetravalent plutonium in 0.5 M HCl/NaCl has been investigated by a combination of spectroscopy and redox potential measurements in the concentration range from 10-5 to 4 × 10-4 M and at pHc 0.3-2.1. Redox potentials were both measured and calculated from the plutonium oxidation state distributions using well-known equilibrium constants for the redox reactions of plutonium. The plutonium oxidation states in solution were quantified by spectroscopy. The pe values calculated from the plutonium redox couples Pu(V)/Pu(VI) and PuO 2(am,hyd)/Pu(V) were found to be consistent with the measured p e values whereas those calculated from the Pu(III)/Pu(IV) couple were found to deviate, suggesting that the formation constants selected in recent reviews for the mononuclear hydroxide complexes of Pu(IV) are overestimated. Combining the redox potentials and the spectroscopically determined Pu(III) and Pu(IV) concentrations, the formation constants of the first, second, and third mononuclear hydroxide complexes Pu(OH)n4-n at I = 0.5 M and 23 ± 2°C are calculated and corrected to zero ionic strength using the specific ion interaction theory (SIT): log β°11 = 14.0 ± 0.2, log β°12 = 26.8 ± 0.6, and log β°13= 38.9 ± 0.9.
ASJC Scopus Sachgebiete
- Chemie (insg.)
- Physikalische und Theoretische Chemie
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in: Radiochimica Acta, Jahrgang 95, Nr. 2, 11.04.2007, S. 89-95.
Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review
}
TY - JOUR
T1 - Investigation of the hydrolysis of plutonium(IV) by a combination of spectroscopy and redox potential measurements
AU - Yun, J. I.
AU - Cho, H. R.
AU - Neck, V.
AU - Altmaier, M.
AU - Seibert, Alice
AU - Marquardt, Christian M.
AU - Walther, Clemens
AU - Fanghänel, Thomas
PY - 2007/4/11
Y1 - 2007/4/11
N2 - The hydrolysis of tetravalent plutonium in 0.5 M HCl/NaCl has been investigated by a combination of spectroscopy and redox potential measurements in the concentration range from 10-5 to 4 × 10-4 M and at pHc 0.3-2.1. Redox potentials were both measured and calculated from the plutonium oxidation state distributions using well-known equilibrium constants for the redox reactions of plutonium. The plutonium oxidation states in solution were quantified by spectroscopy. The pe values calculated from the plutonium redox couples Pu(V)/Pu(VI) and PuO 2(am,hyd)/Pu(V) were found to be consistent with the measured p e values whereas those calculated from the Pu(III)/Pu(IV) couple were found to deviate, suggesting that the formation constants selected in recent reviews for the mononuclear hydroxide complexes of Pu(IV) are overestimated. Combining the redox potentials and the spectroscopically determined Pu(III) and Pu(IV) concentrations, the formation constants of the first, second, and third mononuclear hydroxide complexes Pu(OH)n4-n at I = 0.5 M and 23 ± 2°C are calculated and corrected to zero ionic strength using the specific ion interaction theory (SIT): log β°11 = 14.0 ± 0.2, log β°12 = 26.8 ± 0.6, and log β°13= 38.9 ± 0.9.
AB - The hydrolysis of tetravalent plutonium in 0.5 M HCl/NaCl has been investigated by a combination of spectroscopy and redox potential measurements in the concentration range from 10-5 to 4 × 10-4 M and at pHc 0.3-2.1. Redox potentials were both measured and calculated from the plutonium oxidation state distributions using well-known equilibrium constants for the redox reactions of plutonium. The plutonium oxidation states in solution were quantified by spectroscopy. The pe values calculated from the plutonium redox couples Pu(V)/Pu(VI) and PuO 2(am,hyd)/Pu(V) were found to be consistent with the measured p e values whereas those calculated from the Pu(III)/Pu(IV) couple were found to deviate, suggesting that the formation constants selected in recent reviews for the mononuclear hydroxide complexes of Pu(IV) are overestimated. Combining the redox potentials and the spectroscopically determined Pu(III) and Pu(IV) concentrations, the formation constants of the first, second, and third mononuclear hydroxide complexes Pu(OH)n4-n at I = 0.5 M and 23 ± 2°C are calculated and corrected to zero ionic strength using the specific ion interaction theory (SIT): log β°11 = 14.0 ± 0.2, log β°12 = 26.8 ± 0.6, and log β°13= 38.9 ± 0.9.
KW - Formation constants
KW - Hydrolysis
KW - Plutonium(IV)
KW - Redox potential
KW - Spectroscopy
UR - http://www.scopus.com/inward/record.url?scp=34047217047&partnerID=8YFLogxK
U2 - 10.1524/ract.2007.95.2.89
DO - 10.1524/ract.2007.95.2.89
M3 - Article
AN - SCOPUS:34047217047
VL - 95
SP - 89
EP - 95
JO - Radiochimica Acta
JF - Radiochimica Acta
SN - 0033-8230
IS - 2
ER -