Abstract
The suitability of perrhenate (Re(VII)) to act as an analog for pertechnetate (Tc(VII)) was tested using solvent extraction and the carrier/tracer systems 99Tc(VII)/99mTc(VII) and 185/187Re/186/188Re(VII). Perrhenate is often used as a non-radioactive analogue of pertechnetate, but scarce data is available for the comparison of these metals for liquid-liquid extraction applications. Results show that neither Tc(VII) nor Re(VII) extraction is influenced by pH in the 2–8 range. The anion extractant also separates electrolyte anions, with increasing extraction following the order Cl− < NO3− ≪ ClO4−, resulting in a decreased Tc(VII) and Re(VII) extraction in presence of salt. In particular, the extraction of Re and Tc is suppressed in presence of NaCl at concentrations higher than 1 mM. While Tc extraction is larger than that of Re in absence of electrolyte, they are statistically identical in presence of enough electrolyte. Furthermore, tetraphenylphosphonium chloride (Ph4PCl) is a stronger extractant than iodonitrotetrazolium chloride (INT).
Funding source: U.S. National Nuclear Security Administration
Award Identifier / Grant number: DE-NA0002916
Funding statement: This work was funded by the U.S. National Nuclear Security Administration, Funder Id: http://dx.doi.org/10.13039/100006168 under the SSAA Grant DE-NA0002916.
References
1. Serne, R. J., Rapko, B. M., Pegg, I. L.(Eds.): Technetium Inventory, Distribution, and Speciation in Hanford Tanks. Technical Report PNNL-23319 Rev.1, PNNL, Richland (2014).Search in Google Scholar
2. Lavrukhina, A. K. (Ed.): Analytical Chemistry of Technetium, Promethium, Astatine and Francium. Ann Arbor-Humphrey Science Publishers, Ann Arbor (1970).Search in Google Scholar
3. Lieser, K. H.: Technetium in the nuclear fuel cycle, in medicine and in the environment. Radiochim. Acta 63, 5 (1993).10.1524/ract.1993.63.special-issue.5Search in Google Scholar
4. Lieser, K. H., Bauscher, C.: Technetium in the hydrosphere and in the geosphere. I. Radiochim. Acta 42, 205 (1987).10.1524/ract.1987.42.4.205Search in Google Scholar
5. Kim, E., Boulegue, J.: Chemistry of rhenium as an analogue of technetium: experimental studies of the dissolution of rhenium oxides in aqueous solutions. Radiochim. Acta 91, 211 (2003).10.1524/ract.91.4.211.19968Search in Google Scholar
6. Krebs, B., Hasse, K. D.: Refinements of the crystal structures of KTcO4, KReO4 and OsO4. The bond lengths in tetrahedral oxo-anions and oxides of d0 transition metals. Acta Crystallogr. Sect. B B32, 1334 (1976).10.1107/S056774087600530XSearch in Google Scholar
7. Whittaker, E. J. W., Muntus, R.: Ionic radii for use in geochemistry. Geochim. Cosmochim. Acta 34, 945 (1970).10.1016/0016-7037(70)90077-3Search in Google Scholar
8. Shannon, R. D.: Revised effective ionic radii and systematic studies of interatomie distances in halides and chaleogenides. Acta Crystallogr. Sect. A A32, 751 (1976).10.1107/S0567739476001551Search in Google Scholar
9. Holger, S., Gloe, K., Kraus, W., Spies, H., Johannsen, B., Wichmann, K., Reck, G., Chand, D. K., Bharadwaj, P. K., Mueller, U., Mueller, W. M., Voegtle, F.: Binding and Extraction of Pertechnetate and Perrhenate by Azacages, Fundamentals and Applications of Anion Separations, [Proceedings of the Symposium “Fundamentals and Applications of Anion Separations” held during the American Chemical Society National Meeting], Chicago (2004), p. 151.Search in Google Scholar
10. Rard, J. A., Rand, M. H., Anderegg, G., Wanner, H. (Eds.): Chemical Thermodynamics of Technetium. OECD Nuclear Energy Agency, Issy-les-Moulineaux (1999).Search in Google Scholar
11. Biersack, H.-J. (Ed.): Clinical Nuclear Medicine. Springer-Verlag, Berlin (2007).10.1007/978-3-540-28026-2Search in Google Scholar
12. Buechele, A. C., Lukens, W. W., Shuh, D. K., Mckeown, D. A., Muller, I. S., Pegg, I. L.: Comparison of the behavior of technetium and rhenium in low activity waste glass formulations subjected to the vapor hydration test. Microsc. Microanal. 16, 1628 (2010).10.1017/S143192761006232XSearch in Google Scholar
13. McKeown, D. A., Buechele, A. C., Lukens, W. W., Shuh, D. K., Pegg, I. L.: Tc and Re behavior in borosilicate waste glass vapor hydration tests. Environ. Sci. Technol. 41, 431 (2007).10.1021/es061306uSearch in Google Scholar PubMed
14. Kopunec, R., Abudeab, F. N., Skragkovfi, S.: Extraction of pertechnetate with tetraphenylphosphonium in the presence of various acids, salts and hydroxides. J. Radioanal. Nucl. Chem. 230, 51 (1998).10.1007/BF02387446Search in Google Scholar
15. Makaiova, R. K. N. A.: Extraction characteristics of pertechnetate with tetraphenylarsonium in the presence of chloride, nitrate and perchlorate anions. J. Radioanal. Nucl. Chem. 208, 207 (1996).10.1007/BF02039761Search in Google Scholar
16. Rohal, K., Can Seggen, D., Clark, J.: Solvent extraction of pertechnetate and perrhenate ions from nitrate-rich acidic and alkaline aqueous solutions. Solvent Extr. Ion Exc. 14, 401 (2007).10.1080/07366299608918347Search in Google Scholar
17. Xia, Y., Hess, N. J., Felmy, A. R.: Stability constants of technetium(IV) oxalate complexes as a function of ionic strength. Radiochim. Acta 94, 137 (2006).10.1524/ract.2006.94.3.137Search in Google Scholar
18. Hess, N. J., Qafoku, O., Xia, Y., Moore, D. A., Felmy, A. R.: Thermodynamic model for the solubility of TcO2 x H2O in aqueous oxalate systems. J. Solution Chem. 37, 1471 (2008).10.1007/s10953-008-9328-5Search in Google Scholar
19. Gu, B., Dong, W., Liang, L., Wall, N. A.: Dissolution of technetium(IV) oxide by natural and synthetic organic ligands under both reducing and oxidizing conditions. Environ. Sci. Technol. 45, 4771 (2011).10.1021/es200110ySearch in Google Scholar PubMed
20. Boggs, M. A., Gribat, L. C., Boele, C. A., Wall, N. A.: Rapid separation of VI/VII technetium oxidation states by solvent extraction with iodonitrotetrazolium chloride. J. Radioanal. Nucl. Chem. 293, 843 (2012).10.1007/s10967-012-1744-8Search in Google Scholar
21. Friend, M. T., Eiroa-Lledo, C., Lecrivain, L. M., Wall, D. E., Wall, N. A.: Thermodynamic parameters for the complexation of technetium(IV) with EDTA. Radiochim. Acta 106, 963 (2018).10.1515/ract-2018-2992Search in Google Scholar
22. Buckley, P. T., Dugan, D. L., Elliston, J. T.: Radioisotopes in medicine : preparing a technetium-99m generator and determining its efficiency. J. Chem. Educ. 83, 625 (2006).10.1021/ed083p625Search in Google Scholar
Supplementary Material
The online version of this article offers supplementary material (https://doi.org/10.1515/ract-2019-0006).
©2020 Walter de Gruyter GmbH, Berlin/Boston
