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Spectroscopic identification of ternary Cm - Carbonate surface complexes

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Autorschaft

  • M. Marques Fernandes
  • Thorsten Stumpf
  • B. Baeyens
  • Clemens Walther

Externe Organisationen

  • Paul Scherrer Institut (PSI)
  • Karlsruher Institut für Technologie (KIT)
  • Ruprecht-Karls-Universität Heidelberg

Details

OriginalspracheEnglisch
Seiten (von - bis)921-927
Seitenumfang7
FachzeitschriftEnvironmental Science and Technology
Jahrgang44
Ausgabenummer3
PublikationsstatusVeröffentlicht - 5 Jan. 2010
Extern publiziertJa

Abstract

The influence of dissolved CO2 on the sorption of trivalent curium (Cm) on alumina (γ-Al2O3) and kaolinite was investigated by time resolved laser fluorescence spectroscopy (TRLFS) using the optical properties of Cm as a local luminescent probe. Measurements were performed at T < 20 K on Cm loaded γ-Al2O3 and kaolinite wet pastes prepared in the absence and presence of carbonate in order to pictorially illustrate any changes through a direct comparison of spectra from both systems. The red-shift of excitation and emission spectra, as well as the increase of fluorescence lifetimes observed in the samples with carbonate, clearly showed the influence of carbonate and was fully consistent with the formation of Cm(III) surface species involving carbonate complexes. In addition, the biexponential decay behavior of the fluorescence lifetime indicated that at least two different Cm(III) - carbonate species exist at the mineral - water interface. These results provide the first spectroscopic evidence for the formation of ternary Cm(III) - carbonate surface complexes.

ASJC Scopus Sachgebiete

Zitieren

Spectroscopic identification of ternary Cm - Carbonate surface complexes. / Marques Fernandes, M.; Stumpf, Thorsten; Baeyens, B. et al.
in: Environmental Science and Technology, Jahrgang 44, Nr. 3, 05.01.2010, S. 921-927.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Marques Fernandes, M, Stumpf, T, Baeyens, B, Walther, C & Bradbury, MH 2010, 'Spectroscopic identification of ternary Cm - Carbonate surface complexes', Environmental Science and Technology, Jg. 44, Nr. 3, S. 921-927. https://doi.org/10.1021/es902175w
Marques Fernandes, M., Stumpf, T., Baeyens, B., Walther, C., & Bradbury, M. H. (2010). Spectroscopic identification of ternary Cm - Carbonate surface complexes. Environmental Science and Technology, 44(3), 921-927. https://doi.org/10.1021/es902175w
Marques Fernandes M, Stumpf T, Baeyens B, Walther C, Bradbury MH. Spectroscopic identification of ternary Cm - Carbonate surface complexes. Environmental Science and Technology. 2010 Jan 5;44(3):921-927. doi: 10.1021/es902175w
Marques Fernandes, M. ; Stumpf, Thorsten ; Baeyens, B. et al. / Spectroscopic identification of ternary Cm - Carbonate surface complexes. in: Environmental Science and Technology. 2010 ; Jahrgang 44, Nr. 3. S. 921-927.
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abstract = "The influence of dissolved CO2 on the sorption of trivalent curium (Cm) on alumina (γ-Al2O3) and kaolinite was investigated by time resolved laser fluorescence spectroscopy (TRLFS) using the optical properties of Cm as a local luminescent probe. Measurements were performed at T < 20 K on Cm loaded γ-Al2O3 and kaolinite wet pastes prepared in the absence and presence of carbonate in order to pictorially illustrate any changes through a direct comparison of spectra from both systems. The red-shift of excitation and emission spectra, as well as the increase of fluorescence lifetimes observed in the samples with carbonate, clearly showed the influence of carbonate and was fully consistent with the formation of Cm(III) surface species involving carbonate complexes. In addition, the biexponential decay behavior of the fluorescence lifetime indicated that at least two different Cm(III) - carbonate species exist at the mineral - water interface. These results provide the first spectroscopic evidence for the formation of ternary Cm(III) - carbonate surface complexes.",
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TY - JOUR

T1 - Spectroscopic identification of ternary Cm - Carbonate surface complexes

AU - Marques Fernandes, M.

AU - Stumpf, Thorsten

AU - Baeyens, B.

AU - Walther, Clemens

AU - Bradbury, M. H.

PY - 2010/1/5

Y1 - 2010/1/5

N2 - The influence of dissolved CO2 on the sorption of trivalent curium (Cm) on alumina (γ-Al2O3) and kaolinite was investigated by time resolved laser fluorescence spectroscopy (TRLFS) using the optical properties of Cm as a local luminescent probe. Measurements were performed at T < 20 K on Cm loaded γ-Al2O3 and kaolinite wet pastes prepared in the absence and presence of carbonate in order to pictorially illustrate any changes through a direct comparison of spectra from both systems. The red-shift of excitation and emission spectra, as well as the increase of fluorescence lifetimes observed in the samples with carbonate, clearly showed the influence of carbonate and was fully consistent with the formation of Cm(III) surface species involving carbonate complexes. In addition, the biexponential decay behavior of the fluorescence lifetime indicated that at least two different Cm(III) - carbonate species exist at the mineral - water interface. These results provide the first spectroscopic evidence for the formation of ternary Cm(III) - carbonate surface complexes.

AB - The influence of dissolved CO2 on the sorption of trivalent curium (Cm) on alumina (γ-Al2O3) and kaolinite was investigated by time resolved laser fluorescence spectroscopy (TRLFS) using the optical properties of Cm as a local luminescent probe. Measurements were performed at T < 20 K on Cm loaded γ-Al2O3 and kaolinite wet pastes prepared in the absence and presence of carbonate in order to pictorially illustrate any changes through a direct comparison of spectra from both systems. The red-shift of excitation and emission spectra, as well as the increase of fluorescence lifetimes observed in the samples with carbonate, clearly showed the influence of carbonate and was fully consistent with the formation of Cm(III) surface species involving carbonate complexes. In addition, the biexponential decay behavior of the fluorescence lifetime indicated that at least two different Cm(III) - carbonate species exist at the mineral - water interface. These results provide the first spectroscopic evidence for the formation of ternary Cm(III) - carbonate surface complexes.

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