Details
Original language | English |
---|---|
Pages (from-to) | 7-16 |
Number of pages | 10 |
Journal | Radiochimica Acta |
Volume | 95 |
Issue number | 1 |
Publication status | Published - 11 Apr 2007 |
Externally published | Yes |
Abstract
Tetravalent plutonium readily undergoes hydrolysis even in highly acidic aqueous solutions. In the past, many attempts were made to quantify hydrolysis species by means of optical absorption spectroscopy. In the present work solutions ranging from 10-5 M to 10-2 M (total Pu) concentration in 0.5 M HCl/NaCl (0.3 < pHc < 2.1) are carefully investigated by combining absorption-spectroscopy (UV-Vis, liquid core waveguide capillary) and laser-induced breakdown detection, with special emphasis on the limited solubility of Pu(IV). The results clearly indicate that all changes in the absorption spectra originate from the formation of Pu-polyspecies and colloids. The molar absorptivity of mononuclear Pu(IV) hydroxide complexes does not vary with increasing pHc and ongoing hydrolysis. The normalized absorption spectra of at least the first and the second hydroxide complex (Pu(OH)n4-n n = 1, 2) do not differ from those of the hydrated Pu4+ ion.
Keywords
- Capillary waveguide, Colloids, Disproportionation, Hydrolysis, LIBD, Plutonium, Polymer, Redox reaction, Tetravalent, UV-Vis
ASJC Scopus subject areas
- Chemistry(all)
- Physical and Theoretical Chemistry
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In: Radiochimica Acta, Vol. 95, No. 1, 11.04.2007, p. 7-16.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Hydrolysis of plutonium(IV) in acidic solutions
T2 - No effect of hydrolysis on absorption-spectra of mononuclear hydroxide complexes
AU - Walther, Clemens
AU - Cho, H. R.
AU - Marquardt, Christian M.
AU - Neck, V.
AU - Seibert, Alice
AU - Yun, J. I.
AU - Fanghänel, Thomas
PY - 2007/4/11
Y1 - 2007/4/11
N2 - Tetravalent plutonium readily undergoes hydrolysis even in highly acidic aqueous solutions. In the past, many attempts were made to quantify hydrolysis species by means of optical absorption spectroscopy. In the present work solutions ranging from 10-5 M to 10-2 M (total Pu) concentration in 0.5 M HCl/NaCl (0.3 < pHc < 2.1) are carefully investigated by combining absorption-spectroscopy (UV-Vis, liquid core waveguide capillary) and laser-induced breakdown detection, with special emphasis on the limited solubility of Pu(IV). The results clearly indicate that all changes in the absorption spectra originate from the formation of Pu-polyspecies and colloids. The molar absorptivity of mononuclear Pu(IV) hydroxide complexes does not vary with increasing pHc and ongoing hydrolysis. The normalized absorption spectra of at least the first and the second hydroxide complex (Pu(OH)n4-n n = 1, 2) do not differ from those of the hydrated Pu4+ ion.
AB - Tetravalent plutonium readily undergoes hydrolysis even in highly acidic aqueous solutions. In the past, many attempts were made to quantify hydrolysis species by means of optical absorption spectroscopy. In the present work solutions ranging from 10-5 M to 10-2 M (total Pu) concentration in 0.5 M HCl/NaCl (0.3 < pHc < 2.1) are carefully investigated by combining absorption-spectroscopy (UV-Vis, liquid core waveguide capillary) and laser-induced breakdown detection, with special emphasis on the limited solubility of Pu(IV). The results clearly indicate that all changes in the absorption spectra originate from the formation of Pu-polyspecies and colloids. The molar absorptivity of mononuclear Pu(IV) hydroxide complexes does not vary with increasing pHc and ongoing hydrolysis. The normalized absorption spectra of at least the first and the second hydroxide complex (Pu(OH)n4-n n = 1, 2) do not differ from those of the hydrated Pu4+ ion.
KW - Capillary waveguide
KW - Colloids
KW - Disproportionation
KW - Hydrolysis
KW - LIBD
KW - Plutonium
KW - Polymer
KW - Redox reaction
KW - Tetravalent
KW - UV-Vis
UR - http://www.scopus.com/inward/record.url?scp=34047198669&partnerID=8YFLogxK
U2 - 10.1524/ract.2007.95.1.7
DO - 10.1524/ract.2007.95.1.7
M3 - Article
AN - SCOPUS:34047198669
VL - 95
SP - 7
EP - 16
JO - Radiochimica Acta
JF - Radiochimica Acta
SN - 0033-8230
IS - 1
ER -