Trivalent actinide coprecipitation with powellite (CaMoO4): Secondary solid solution formation during HLW borosilicate-glass dissolution
| LEADER | caa a22 4500 | ||
|---|---|---|---|
| 001 | 378927221 | ||
| 003 | CHVBK | ||
| 005 | 20180305123620.0 | ||
| 007 | cr unu---uuuuu | ||
| 008 | 161128e20041101xx s 000 0 eng | ||
| 024 | 7 | 0 | |a 10.1524/ract.92.9.639.54976 |2 doi |
| 035 | |a (NATIONALLICENCE)gruyter-10.1524/ract.92.9.639.54976 | ||
| 245 | 0 | 0 | |a Trivalent actinide coprecipitation with powellite (CaMoO4): Secondary solid solution formation during HLW borosilicate-glass dissolution |h [Elektronische Daten] |c [Dirk Bosbach, Thomas Rabung, Felix Brandt, Thomas Fanghänel] |
| 520 | 3 | |a Powellite (CaMoO4) is one of the various crystalline secondary alteration phases which form during the corrosion of high level waste (HLW) glasses. Due to their structural variability, powellite can accommodate considerable chemical substitutions including trivalent actinides. Batch adsorption and coprecipitation experiments in mixed flow reactors have been used to study quantitatively the uptake of Cm(III) and Eu(III) (as a nonradioactive chemical homologue for trivalent actinides) from aqueous solution under repository relevant conditions. A metal ion concentration-independent Kd of 1200ml/g has been determined for adsorption above pH 4 up to 3μmol/L Eu(III). The partition coefficient for coprecipitation varies between 10 and 800 depending on the precipitation rate. Time-resolved laser fluorescence spectroscopy has been used to study the aqueous complexation of Cm(III)/Eu(III) and MoO42- as well as their incorporation into the powellite crystal lattice during coprecipitation. A red shift of the Cm(III) fluorescence emission of the transition indicates the formation of aqueous CmMoO4+ (598nm) and Cm(MoO4)22- (601nm) complexes. The incorporation of Cm(III) is indicated by a significant red shift. The corresponding lifetime of 165μs indicates quench effects. A similar behaviour has been observed for Eu(III). The life time of the 5D0-7F2 transition is 350μs for an incorporated Eu(III) species, suggesting also intrinsic quench effects, due to the local crystal field or impurities. | |
| 540 | |a © 2004 Oldenbourg Wissenschaftsverlag GmbH | ||
| 690 | 7 | |a Laboratory techniques, experiments |2 nationallicence | |
| 690 | 7 | |a Analytical chemistry |2 nationallicence | |
| 690 | 7 | |a Inorganic chemistry |2 nationallicence | |
| 700 | 1 | |a Bosbach |D Dirk |4 aut | |
| 700 | 1 | |a Rabung |D Thomas |4 aut | |
| 700 | 1 | |a Brandt |D Felix |4 aut | |
| 700 | 1 | |a Fanghänel |D Thomas |4 aut | |
| 773 | 0 | |t Radiochimica Acta/International journal for chemical aspects of nuclear science and technology |d Oldenbourg Wissenschaftsverlag GmbH |g 92/9-11/2004(2004-11-01), 639-643 |x 0033-8230 |q 92:9-11/2004<639 |1 2004 |2 92 |o ract | |
| 856 | 4 | 0 | |u https://doi.org/10.1524/ract.92.9.639.54976 |q text/html |z Onlinezugriff via DOI |
| 908 | |D 1 |a research article |2 jats | ||
| 950 | |B NATIONALLICENCE |P 856 |E 40 |u https://doi.org/10.1524/ract.92.9.639.54976 |q text/html |z Onlinezugriff via DOI | ||
| 950 | |B NATIONALLICENCE |P 700 |E 1- |a Bosbach |D Dirk |4 aut | ||
| 950 | |B NATIONALLICENCE |P 700 |E 1- |a Rabung |D Thomas |4 aut | ||
| 950 | |B NATIONALLICENCE |P 700 |E 1- |a Brandt |D Felix |4 aut | ||
| 950 | |B NATIONALLICENCE |P 700 |E 1- |a Fanghänel |D Thomas |4 aut | ||
| 950 | |B NATIONALLICENCE |P 773 |E 0- |t Radiochimica Acta/International journal for chemical aspects of nuclear science and technology |d Oldenbourg Wissenschaftsverlag GmbH |g 92/9-11/2004(2004-11-01), 639-643 |x 0033-8230 |q 92:9-11/2004<639 |1 2004 |2 92 |o ract | ||
| 900 | 7 | |b CC0 |u http://creativecommons.org/publicdomain/zero/1.0 |2 nationallicence | |
| 898 | |a BK010053 |b XK010053 |c XK010000 | ||
| 949 | |B NATIONALLICENCE |F NATIONALLICENCE |b NL-gruyter | ||