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| Hauptseite > Publikationsdatenbank > Solid solution formation and uptake of Radium in the presence of barite > print |
| Hauptseite > Publikationsdatenbank > Solid solution formation and uptake of Radium in the presence of barite > print |
| 001 | 138578 | ||
| 005 | 20240708133855.0 | ||
| 037 | _ | _ | |a FZJ-2013-04677 |
| 100 | 1 | _ | |a Brandt, Felix |0 P:(DE-Juel1)144040 |b 0 |u fzj |e Corresponding author |
| 111 | 2 | _ | |a Goldschmidt Conference 2013 |c Firenze |d 2013-08-25 - 2013-08-30 |w Italy |
| 245 | _ | _ | |a Solid solution formation and uptake of Radium in the presence of barite |
| 260 | _ | _ | |c 2013 |
| 336 | 7 | _ | |a Conference Presentation |b conf |m conf |0 PUB:(DE-HGF)6 |s 1382439850_8542 |2 PUB:(DE-HGF) |x Other |
| 336 | 7 | _ | |a Conference Paper |0 33 |2 EndNote |
| 336 | 7 | _ | |a Other |2 DataCite |
| 336 | 7 | _ | |a LECTURE_SPEECH |2 ORCID |
| 336 | 7 | _ | |a conferenceObject |2 DRIVER |
| 336 | 7 | _ | |a INPROCEEDINGS |2 BibTeX |
| 520 | _ | _ | |a The phase relations in the BaSO4-RaSO4-H2O system may determine the solubility of radium in natural waters due to the formation of a solid solution. In the near-field of nuclear waste repositories for spent fuel, radium may enter a system in which barite is in equilibrium with the aqueous solution. Thermodynamically, a RaxBa1-xSO4 solid solution is expected to form as solubility controlling phase rather than RaSO4. However, due to a lack of reliable data, the solid solution system RaSO4-BaSO4-H2O is currently not considered in long term safety assessments for nuclear waste repositories. The solubility product of the pure RaSO4 endmember is poorly constrained between pKRaSO4 = 10.26 to 10.41 by only very few experimental data [1,2]. Published interaction parameters WBaRa of the RaSO4-BaSO4-H2O system varies varies in different studies [3, 4] between 0.9 and 3.9 - 6.5 kJ/mol.
In this study we have combined experimental data, atomistic calculations and thermodynamic modeling to study in detail how a radium containing solution will equilibrate with solid BaSO4 under repository relevant conditions. Batch sorption experiments at close to equilibrium conditions indicate the formation of a RaxBa1-xSO4 solid. Our first principles calculations based on the single defect method [5] indicate a value of WBaRa = 2.5 ± 1.0 kJ/mol, implying a non-ideal solid solution. Thermodynamic assessment calculations indicate that the final experimental Ra(aq) concentration at room temperature and 90 °C can be matched with
WBaRa ≈ 1.5 kJ/mol and pKRaSO4 ≈ 10.41.
[1] Lind, S. C., et al (1918). J Am Chem Soc 40, 465-472. [2] Paige, C. R. et al.(1998). Geochim. Cosmochim. Acta 62, 15-23. [3] Zhu, C., 2004. Geochim. Cosmochim. Acta 68, 3327-3337. [4] Curti, E., et al. (2010). Geochim. Cosmochim. Acta 74, 3553-3570. [5] Sluiter & Kawazoe (2002) Europhys Lett. 57, 526-532. |
| 536 | _ | _ | |a 142 - Safety Research for Nuclear Waste Disposal (POF2-142) |0 G:(DE-HGF)POF2-142 |c POF2-142 |x 0 |f POF II |
| 536 | _ | _ | |a SKIN - Slow processes in close-to-equilibrium conditions for radionuclides in water/solid systems of relevance to nuclear waste management (269688) |0 G:(EU-Grant)269688 |c 269688 |x 1 |f FP7-Fission-2010 |
| 700 | 1 | _ | |a Klinkenberg, Martina |0 P:(DE-Juel1)130364 |b 1 |u fzj |
| 700 | 1 | _ | |a Vinograd, Victor |0 P:(DE-Juel1)144348 |b 2 |u fzj |
| 700 | 1 | _ | |a Rozov, Konstantin |0 P:(DE-Juel1)144076 |b 3 |u fzj |
| 700 | 1 | _ | |a Bosbach, Dirk |0 P:(DE-Juel1)130324 |b 4 |u fzj |
| 909 | C | O | |o oai:juser.fz-juelich.de:138578 |p openaire |p VDB |p ec_fundedresources |
| 910 | 1 | _ | |a Forschungszentrum Jülich GmbH |0 I:(DE-588b)5008462-8 |k FZJ |b 0 |6 P:(DE-Juel1)144040 |
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| 914 | 1 | _ | |y 2013 |
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