Stability of Th(IV) polymers measured by electrospray mass spectrometry and laser-induced breakdown detection

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Autoren

  • Clemens Walther
  • Markus Fuss
  • Sebastian Büchner
  • Horst Geckeis

Externe Organisationen

  • Karlsruher Institut für Technologie (KIT)
Forschungs-netzwerk anzeigen

Details

OriginalspracheEnglisch
Seiten (von - bis)1003-1008
Seitenumfang6
FachzeitschriftJournal of Radioanalytical and Nuclear Chemistry
Jahrgang282
Ausgabenummer3
PublikationsstatusVeröffentlicht - 16 Juli 2009
Extern publiziertJa

Abstract

The formation of polynuclear thorium hydroxide complexes in acidic aqueous solutions is observed by electrospray mass spectrometry. Size, number of hydroxide ligands and charge of all complexes in solution are identified independently. By repeated measurements over a time span of up to 418 days the stability of the polymers is observed. At concentrations above [Th(IV)] tot = 10 mM pentamers and dimers are the dominant stable species. In contrast, the fractions of pentamers initially present at [Th(IV)]tot = 0.2 mM decrease within less than 4 weeks, correlated with the formation of nm-sized colloids observed by LIBD indicating an Ostwald-ripening like process.

ASJC Scopus Sachgebiete

Ziele für nachhaltige Entwicklung

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Stability of Th(IV) polymers measured by electrospray mass spectrometry and laser-induced breakdown detection. / Walther, Clemens; Fuss, Markus; Büchner, Sebastian et al.
in: Journal of Radioanalytical and Nuclear Chemistry, Jahrgang 282, Nr. 3, 16.07.2009, S. 1003-1008.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Walther C, Fuss M, Büchner S, Geckeis H. Stability of Th(IV) polymers measured by electrospray mass spectrometry and laser-induced breakdown detection. Journal of Radioanalytical and Nuclear Chemistry. 2009 Jul 16;282(3):1003-1008. doi: 10.1007/s10967-009-0158-8
Walther, Clemens ; Fuss, Markus ; Büchner, Sebastian et al. / Stability of Th(IV) polymers measured by electrospray mass spectrometry and laser-induced breakdown detection. in: Journal of Radioanalytical and Nuclear Chemistry. 2009 ; Jahrgang 282, Nr. 3. S. 1003-1008.
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abstract = "The formation of polynuclear thorium hydroxide complexes in acidic aqueous solutions is observed by electrospray mass spectrometry. Size, number of hydroxide ligands and charge of all complexes in solution are identified independently. By repeated measurements over a time span of up to 418 days the stability of the polymers is observed. At concentrations above [Th(IV)] tot = 10 mM pentamers and dimers are the dominant stable species. In contrast, the fractions of pentamers initially present at [Th(IV)]tot = 0.2 mM decrease within less than 4 weeks, correlated with the formation of nm-sized colloids observed by LIBD indicating an Ostwald-ripening like process.",
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Download

TY - JOUR

T1 - Stability of Th(IV) polymers measured by electrospray mass spectrometry and laser-induced breakdown detection

AU - Walther, Clemens

AU - Fuss, Markus

AU - Büchner, Sebastian

AU - Geckeis, Horst

N1 - Funding information: Acknowledgments We thank Marcus Altmaier (INE) for preparation of the stock solution and, together with Volker Neck, for many fruitful discussions. We also thank Oliver Schwindt for LIBD and the INE analytics group for ICP MS measurements. Finally, we acknowledge financial support by the ‘‘Programm Nuklear’’ and by the ‘‘Helmholtz Russia Joint Research Group’’ of the Helmholtz Gemeinschaft Deutscher Forschungszentren (HGF).

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N2 - The formation of polynuclear thorium hydroxide complexes in acidic aqueous solutions is observed by electrospray mass spectrometry. Size, number of hydroxide ligands and charge of all complexes in solution are identified independently. By repeated measurements over a time span of up to 418 days the stability of the polymers is observed. At concentrations above [Th(IV)] tot = 10 mM pentamers and dimers are the dominant stable species. In contrast, the fractions of pentamers initially present at [Th(IV)]tot = 0.2 mM decrease within less than 4 weeks, correlated with the formation of nm-sized colloids observed by LIBD indicating an Ostwald-ripening like process.

AB - The formation of polynuclear thorium hydroxide complexes in acidic aqueous solutions is observed by electrospray mass spectrometry. Size, number of hydroxide ligands and charge of all complexes in solution are identified independently. By repeated measurements over a time span of up to 418 days the stability of the polymers is observed. At concentrations above [Th(IV)] tot = 10 mM pentamers and dimers are the dominant stable species. In contrast, the fractions of pentamers initially present at [Th(IV)]tot = 0.2 mM decrease within less than 4 weeks, correlated with the formation of nm-sized colloids observed by LIBD indicating an Ostwald-ripening like process.

KW - Colloid

KW - Electrospray

KW - Laser-induced breakdown detection

KW - Polymerization

KW - Thorium

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