Uptake of trivalent actinides (curium(III)) by hardened cement paste: A time-resolved laser fluorescence spectroscopy study

Thorsten Stumpf; Jan Tits; Clemens Walther; Erich Wieland; Thomas Fanghänel

doi:10.1016/j.jcis.2004.03.014

Uptake of trivalent actinides (curium(III)) by hardened cement paste: A time-resolved laser fluorescence spectroscopy study

Thorsten Stumpf^*
, Jan Tits
, Clemens Walther
, Erich Wieland
, Thomas Fanghänel

^*Korrespondierende*r Autor*in für diese Arbeit

Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review

Abstract

The curium(III) interaction with cement was investigated using time-resolved laser fluorescence spectroscopy at trace concentrations. Four different Cm(III) species were identified: a nonfluorescing species which corresponds to curium hydroxide real colloids, which were characterized in detail by laser-induced breakdown detection (LIBD), a fluorescing Cm(III)/portlandite sorption species, and two fluorescing Cm(III)/calcium silicate hydrate (CSH) species. From the fluorescence emission lifetimes it is predicted that the two fluorescing Cm(III)/CSH species have one to two and no water molecules, respectively, left in their first coordination sphere, suggesting that these species are incorporated into the CSH structure.

Originalsprache	Englisch
Seiten (von - bis)	118-124
Seitenumfang	7
Fachzeitschrift	Journal of Colloid and Interface Science
Jahrgang	276
Ausgabenummer	1
DOIs	https://doi.org/10.1016/j.jcis.2004.03.014
Publikationsstatus	Veröffentlicht - 27 Apr. 2004
Extern publiziert	Ja

ASJC Scopus Sachgebiete

Elektronische, optische und magnetische Materialien
Biomaterialien
Oberflächen, Beschichtungen und Folien
Kolloid- und Oberflächenchemie

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10.1016/j.jcis.2004.03.014

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title = "Uptake of trivalent actinides (curium(III)) by hardened cement paste: A time-resolved laser fluorescence spectroscopy study",

abstract = "The curium(III) interaction with cement was investigated using time-resolved laser fluorescence spectroscopy at trace concentrations. Four different Cm(III) species were identified: a nonfluorescing species which corresponds to curium hydroxide real colloids, which were characterized in detail by laser-induced breakdown detection (LIBD), a fluorescing Cm(III)/portlandite sorption species, and two fluorescing Cm(III)/calcium silicate hydrate (CSH) species. From the fluorescence emission lifetimes it is predicted that the two fluorescing Cm(III)/CSH species have one to two and no water molecules, respectively, left in their first coordination sphere, suggesting that these species are incorporated into the CSH structure.",

keywords = "Cement, CSH, Curium, Incorporation, LIBD, Sorption, Surface complexation, TRLFS",

author = "Thorsten Stumpf and Jan Tits and Clemens Walther and Erich Wieland and Thomas Fangh{\"a}nel",

note = "Funding information: We thank Andr{\'e} Rossberg for providing the factor analysis program code designed for the analysis of EXAFS, UV–vis, and TRLFS spectra and J.I. Yun and H.R. Cho for performing the LIBD measurements. We thank the Institut f{\"u}r Radiochemie at the Forschungszentrum Rossendorf for their support and the supply of the laser equipment. Partial financial support was provided by the Swiss National Cooperative for the Disposal of Radioactive Waste (Nagra).",

year = "2004",

month = apr,

day = "27",

doi = "10.1016/j.jcis.2004.03.014",

language = "English",

volume = "276",

pages = "118--124",

journal = "Journal of Colloid and Interface Science",

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TY - JOUR

T1 - Uptake of trivalent actinides (curium(III)) by hardened cement paste

T2 - A time-resolved laser fluorescence spectroscopy study

AU - Stumpf, Thorsten

AU - Tits, Jan

AU - Walther, Clemens

AU - Wieland, Erich

AU - Fanghänel, Thomas

N1 - Funding information: We thank André Rossberg for providing the factor analysis program code designed for the analysis of EXAFS, UV–vis, and TRLFS spectra and J.I. Yun and H.R. Cho for performing the LIBD measurements. We thank the Institut für Radiochemie at the Forschungszentrum Rossendorf for their support and the supply of the laser equipment. Partial financial support was provided by the Swiss National Cooperative for the Disposal of Radioactive Waste (Nagra).

PY - 2004/4/27

Y1 - 2004/4/27

N2 - The curium(III) interaction with cement was investigated using time-resolved laser fluorescence spectroscopy at trace concentrations. Four different Cm(III) species were identified: a nonfluorescing species which corresponds to curium hydroxide real colloids, which were characterized in detail by laser-induced breakdown detection (LIBD), a fluorescing Cm(III)/portlandite sorption species, and two fluorescing Cm(III)/calcium silicate hydrate (CSH) species. From the fluorescence emission lifetimes it is predicted that the two fluorescing Cm(III)/CSH species have one to two and no water molecules, respectively, left in their first coordination sphere, suggesting that these species are incorporated into the CSH structure.

AB - The curium(III) interaction with cement was investigated using time-resolved laser fluorescence spectroscopy at trace concentrations. Four different Cm(III) species were identified: a nonfluorescing species which corresponds to curium hydroxide real colloids, which were characterized in detail by laser-induced breakdown detection (LIBD), a fluorescing Cm(III)/portlandite sorption species, and two fluorescing Cm(III)/calcium silicate hydrate (CSH) species. From the fluorescence emission lifetimes it is predicted that the two fluorescing Cm(III)/CSH species have one to two and no water molecules, respectively, left in their first coordination sphere, suggesting that these species are incorporated into the CSH structure.

KW - Cement

KW - CSH

KW - Curium

KW - Incorporation

KW - LIBD

KW - Sorption

KW - Surface complexation

KW - TRLFS

UR - https://www.scopus.com/pages/publications/3042528511

U2 - 10.1016/j.jcis.2004.03.014

DO - 10.1016/j.jcis.2004.03.014

M3 - Article

AN - SCOPUS:3042528511

SN - 0021-9797

VL - 276

SP - 118

EP - 124

JO - Journal of Colloid and Interface Science

JF - Journal of Colloid and Interface Science

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ER -