journal article·2014-06Open access

Redox-dependent solubility of technetium in low activity waste glass

Chuck Z. Soderquist, Michael J. Schweiger, Dong-Sang Kim, Wayne W. Lukens, John S. McCloy

Journal of Nuclear Materials· Volume 449· Issue 1-3

Abstract

Abstract The solubility of technetium was measured in a Hanford low activity waste (LAW) glass simulant, to investigate the extent that technetium solubility controls the incorporation of technetium into LAW glass. A series of LAW glass samples, spiked with 500–6000 ppm of Tc as potassium pertechnetate, were melted at 1000 °C in sealed fused quartz ampoules. Technetium solubility was determined in the quenched bulk glass to be 2000–2800 ppm, with slightly reducing conditions due to choice of milling media resulting in reductant contamination and higher solubility. The chemical form of technetium obtained by X-ray absorption near edge spectroscopy is mainly isolated, octahedrally-coordinated Tc(IV), with a minority of Tc(VII) in some glasses and TcO 2 in two glasses. The concentration and speciation of technetium depends on glass redox and amount of technetium added. Salts formed at the top of higher technetium loaded glasses during the melt. The results of this study show that technetium solubility should not be a factor in technetium retention during melting of Hanford LAW glass.
Source: openaire · Quality: candidate unverified · Source record ↗

Research context

OpenAlex topics: Nuclear materials and radiation effects · Radioactive element chemistry and processing · Glass properties and applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (35)

Show source-provided references
1. P.J. Certa, P. A. Empey, River Protection Project System Plan, Office of River Protection, US Department of Energy, Richland, WA, ORP-11242 Revision 6, 2011.
2. Toste · J. Radioanal. Nucl. Chem. · 1995 · 194 · 2510.1007/BF02037609 ↗
3. Golcar · Rev · 2000
4. D.S. Kim, L.M. Bagaasen, J.V. Crum, A. Fluegel, A. Gallegos, B. Martinez, J. Matyas, P.A. Meyer, D.R. Paulsen, B.J. Riley, M.J. Schweiger, C.W. Stewart, R.G. Swoboda, J.D. Yeager, Investigation of Tc Migration Mechanism During Bulk Vitrification Process Using Re Surrogate, Pacific Northwest National Laboratory, Richland, WA, PNNL-16267, 2006.10.2172/903263 ↗
5. Darab · Chem. Mater. · 1996 · 8 · 100410.1021/cm950418+ ↗
6. Bibler · Mater. Res. Soc. Symp. Proc. · 1988 · 112 · 58510.1557/PROC-112-585 ↗
7. Ebert · Mater. Res. Soc. Symp. Proc. · 1996 · 412 · 22110.1557/PROC-412-221 ↗
8. Lukens · Chem. Mater. · 2007 · 19 · 55910.1021/cm0622001 ↗
9. Lukens · Mater. Res. Soc. Symp. Proc. · 2004 · 802 · DD3.3.1
10. Antonini · J. Non-Cryst. Solids · 1985 · 71 · 21910.1016/0022-3093(85)90290-X ↗
11. Lanza · J. Trace Microprob. Technol. · 1992 · 10 · 257
12. D.L. Blanchard, G.N. Brown, S.D. Conradson, S.K. Fadeff, G.R. Golcar, N.J. Hess, G.S. Klinger, D.E. Kurath, Technetium in alkaline, high-salt, radioactive tank waste supernate, in: Preliminary Characterization and Removal, Pacific Northwest National Laboratory, Richland, WA, PNNL-11386, 1997.10.2172/475671 ↗
13. Lukens · Environ. Sci. Technol. · 2002 · 36 · 112410.1021/es015653+ ↗
14. Lukens · Environ. Sci. Technol. · 2004 · 38 · 22910.1021/es034318d ↗
15. Xia · Radiochim. Acta · 2006 · 94 · 13710.1524/ract.2006.94.3.137 ↗
16. Hess · ACS Symp. Ser. · 2006 · 943 · 28610.1021/bk-2006-0943.ch016 ↗
17. McKeown · Environ. Sci. Technol. · 2007 · 41 · 43110.1021/es061306u ↗
18. Buechele · Microsc. Microanal. · 2010 · 16 · 162810.1017/S143192761006232X ↗
19. Buechele · J. Nucl. Mater. · 2012 · 429 · 15910.1016/j.jnucmat.2012.05.032 ↗
20. Riley · J. Am. Ceram. Soc. · 2013 · 96 · 115010.1111/jace.12280 ↗
21. Jantzen · Mater. Res. Soc. Symp. Proc. · 2005 · 168 · 141
22. Muller · Hyperfine Interact. · 2009 · 191 · 347
23. K.S. Matlack, I.S. Muller, R.A. Callow, N. D’Angelo, T. Bardakci, I. Joseph, I. L. Pegg, Improved Technetium Retention in Hanford LAW glass – phase 2, Vitreous state laboratory, The Catholic University of America, Washington, DC, VSL-11R2260-1, 2011.
24. McCloy · Environ. Sci. Technol. · 2012 · 46 · 1261610.1021/es302734y ↗
25. Goel · Int. J. Appl. Glass Sci. · 2013 · 4 · 4210.1111/ijag.12003 ↗
26. Gibson · Radiochim. Acta · 1993 · 60 · 12110.1524/ract.1993.60.23.121 ↗
27. Baumann · Analyst · 1992 · 117 · 91310.1039/an9921700913 ↗
28. Webb · Phys. Scr. · 2005 · 2005 · 101110.1238/Physica.Topical.115a01011 ↗
29. Ravel · Phys. Scr. · 2005 · T115 · 100710.1238/Physica.Topical.115a01007 ↗
30. Newville · J. Synchr. Rad. · 2001 · 8 · 32210.1107/S0909049500016964 ↗
31. Rehr · Phys. Rev. Lett. · 1992 · 69 · 339710.1103/PhysRevLett.69.3397 ↗
32. Rodriguez · J. Am. Chem. Soc. · 2007 · 129 · 1024410.1021/ja0727363 ↗
33. Schreiber · J. Am. Ceram. Soc. · 1984 · 67 · C-10610.1111/j.1151-2916.1984.tb19710.x ↗
34. King · Earth. Planet. Sci. Lett. · 2000 · 178 · 9710.1016/S0012-821X(00)00071-6 ↗
35. Raman analysis of perrhenate and pertechnetate in alkali salts and borosilicate glasses10.1002/jrs.4427 ↗