Hostname: page-component-78c5997874-dh8gc Total loading time: 0 Render date: 2024-11-08T05:32:25.723Z Has data issue: false hasContentIssue false

Leachability of Nd, U, Th, and Sr from Cements in a CO2 Free Atmosphere

Published online by Cambridge University Press:  15 February 2011

R. J. Serne
Affiliation:
Pacific Northwest National Laboratory, P. O. Box 999, MS K6-8 1, Richland, Washington 99352, rj_serne@pnl.gov
D. Rai
Affiliation:
Pacific Northwest National Laboratory, P. O. Box 999, MS K6-8 1, Richland, Washington 99352, rj_serne@pnl.gov
P. F. Martin
Affiliation:
Pacific Northwest National Laboratory, P. O. Box 999, MS K6-8 1, Richland, Washington 99352, rj_serne@pnl.gov
A. R. Felmy
Affiliation:
Pacific Northwest National Laboratory, P. O. Box 999, MS K6-8 1, Richland, Washington 99352, rj_serne@pnl.gov
L. Rao
Affiliation:
Pacific Northwest National Laboratory, P. O. Box 999, MS K6-8 1, Richland, Washington 99352, rj_serne@pnl.gov
S. Ueta
Affiliation:
Mitsubishi Materials Corporation, Naka Nuclear Development Center, Naka-Gun, Ibaraki-Ken, 311-01, Japan
Get access

Abstract

To determine the leachability and concentration-controlling solids for nuclides contained in solidified low-level nuclear wastes, cement doped with neodymium, uranium, thorium and strontium was prepared and cured in a CO2-free atmosphere. Leaching tests were conducted by equilibrating aliquots of the crushed doped cement with CO2-free deionized water at pcH+ values ranging from 7.5 to 12.5 in an effort to determine if solubility constraints could be used to predict leachable concentrations of Nd (an analog of trivalent actinides), U, Th, and Sr. Steady state concentrations of Nd, U, Th and Sr were attained within a few days. The observed Nd concentrations continually decreased with the increase in pcH+ from about 7.5 to 9.0, and were at detection limit at pcH+ values > 9.0. The comparison of these results with thermodynamic data suggests that Nd(OH)3(am) is the controlling solid phase. The observed U concentrations decreased by two orders of magnitude with a unit increase in pcH+ in the range of 7.5 to 9.0 and were at the detection limit at pcH+ > 9.0. From the multitude of U(VI) solids that can form under the test conditions, the data suggest that CaUO4 is the likely controlling solid. The concentration of Th was at the detection limit over the entire pcH+ range covered. Based on previous work, ThO2(am) is likely to be the controlling solid. In the absence of CO2, no solubility-controlling solid was found for Sr.

Type
Research Article
Copyright
Copyright © Materials Research Society 1996

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

1. IAEA. 1993. Improved Cement Solidification of Low and Intermediate Level Radioactive Wastes, Technical Reports Series No. 350, International Atomic Energy Agency, Vienna, Austria.Google Scholar
2. Atkins, M., Bennett, D. G., Dawes, A. C., Glasser, F. P., Kindness, A., and Read, D., Cement and Concrete Res. 22:497502 (1992).Google Scholar
3. Reardon, E. J., Waste Management, 12:221239 (1992).Google Scholar
4. Alcorn, S. R., Coons, W. E., and Gardiner, M. A., In Scientific Basis for Nuclear Waste Management XIII, ed. by Oversby, V. M. and Brown, P. W. (Mater, Res. Soc. Proc. 176, Pittsburgh, PA 1990), p. 165173.Google Scholar
5. Haworth, A., Sharland, S. M., and Tweed, C. J., In Scientific Basis for Nuclear Waste Management XII, ed. by Lutze, W. and Ewing, R. C. (Mater. Res. Soc. Proc. 127, Pittsburgh, PA 1989), p. 447454.Google Scholar
6. Haworth, A., Sharland, S. M., and Tweed, C. J., In Scientific Basis for Nuclear Waste Management XIII, ed. by Oversby, V. M. and Brown, P. W. (Mater. Res. Soc. Proc. 176, Pittsburgh, PA 1990), p. 175181.Google Scholar
7. Rai, Dhanpat, Felny, A. R., Juracich, S. P., and Rao, L.. Estimating the Hydrogen Ion Concentration in Concentrated NaCI and Na2SO4 Electrolyte, PNL-9992, Pacific Northwest Laboratory, Richland, WA (1994).Google Scholar
8. Rai, Dhanpat, Serne, R. J. and Moore, D. A., Soil Sci. Soc. Am. J. 44:490495 (1980).Google Scholar
9. Rai, Dhanpat, Felmy, A. R., and Fulton, R. W., J. Solut. Chem. 24:879895 (1995).Google Scholar
10. Felmy, A. R., Rai, Dhanpat, and Mason, M. J., Radiochim. Acta. 55:177185 (1991).Google Scholar
11. Rai, Dhanpat, Radiochim. Acta. 35:97108 (1984).Google Scholar
12. Rao, L., Rai, D., Felmy, A. R.. Solubility of Nd(OH)3(c) in the Aqueous NaCI Solution at 25°C and 90°C, PNL-SA-26137, Pacific Northwest Laboratory, Richland, WA (1995).Google Scholar
13. Rai, Dhanpat, Serne, R. J., Felny, A. R., Rao, L., Martin, P. F. and Ueta, S., Leachability of Nd. U. Th. and Sr from Cements in a CO2 Free Atmosphere, PNWD-SA-4237, Battelle, Pacific Northwest Laboratories, Richland, WA (1995).Google Scholar
14. Silva, R. J., The Solubilities of Crystalline Neodymium and Americium Trihydroxides, LBL-15055, Lawrence Berkeley Laboratory, Berkeley, CA., 1987.Google Scholar
15. Grenthe, I., Fuger, J., Konings, R. J. M., Lemire, R. J., Muller, A. B., Nguyen-Trung, C., and Wanner, H., Chemical Thermodynamics of Uranium, ed. by Wanner, H. and Forest, I., (North-Holland Elsevier Science Publishers, New York, 1992).Google Scholar
16. Atkins, M., Cowie, J., Glasser, F. P., Jappy, T., Kindness, A., and Pointer, C., In Scientific Basis for Nuclear Waste Management XIII, ed. by Oversby, V. M. and Brown, P. W. (Mater. Res. Soc. Proc. 176, Pittsburgh, PA 1990), p. 117127.Google Scholar
17. Atkins, M., Glasser, F. P., and Moroni, L. P., In Scientific Basis for Nuclear Waste Management XIV, ed. by Abrajano, T. A. Jr. and Johnson, L. H. (Mater. Res. Soc. Proc. 212, Pittsburgh, PA 1991), p. 373386.Google Scholar
18. Ryan, J. L. and Rai, Dhanpat, Inorg. Chem. 26:41404142 (1987).Google Scholar
19. Rai, Dhanpat, Felmy, A. R., Moore, D. A., and Mason, M. J.. In Scientific Basis for Nuclear Waste Management XVIII, ed. by Murakami, T. and Ewing, R. C. (Mater. Res. Soc. Proc. 353 Part 2, Pittsburgh, PA 1995), p. 11431150.Google Scholar