Hydrolysis of plutonium(IV) in acidic solutions: No effect of hydrolysis on absorption-spectra of mononuclear hydroxide complexes

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Autorschaft

  • Clemens Walther
  • H. R. Cho
  • Christian M. Marquardt
  • V. Neck
  • Alice Seibert
  • J. I. Yun
  • Thomas Fanghänel

Externe Organisationen

  • Karlsruher Institut für Technologie (KIT)
  • Gemeinsame Forschungsstelle (GFS)
  • Ruprecht-Karls-Universität Heidelberg
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Details

OriginalspracheEnglisch
Seiten (von - bis)7-16
Seitenumfang10
FachzeitschriftRadiochimica Acta
Jahrgang95
Ausgabenummer1
PublikationsstatusVeröffentlicht - 11 Apr. 2007
Extern publiziertJa

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.

ASJC Scopus Sachgebiete

Zitieren

Hydrolysis of plutonium(IV) in acidic solutions: No effect of hydrolysis on absorption-spectra of mononuclear hydroxide complexes. / Walther, Clemens; Cho, H. R.; Marquardt, Christian M. et al.
in: Radiochimica Acta, Jahrgang 95, Nr. 1, 11.04.2007, S. 7-16.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Walther C, Cho HR, Marquardt CM, Neck V, Seibert A, Yun JI et al. Hydrolysis of plutonium(IV) in acidic solutions: No effect of hydrolysis on absorption-spectra of mononuclear hydroxide complexes. Radiochimica Acta. 2007 Apr 11;95(1):7-16. doi: 10.1524/ract.2007.95.1.7
Walther, Clemens ; Cho, H. R. ; Marquardt, Christian M. et al. / Hydrolysis of plutonium(IV) in acidic solutions : No effect of hydrolysis on absorption-spectra of mononuclear hydroxide complexes. in: Radiochimica Acta. 2007 ; Jahrgang 95, Nr. 1. S. 7-16.
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title = "Hydrolysis of plutonium(IV) in acidic solutions: No effect of hydrolysis on absorption-spectra of mononuclear hydroxide complexes",
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",
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Download

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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

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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

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