Hostname: page-component-848d4c4894-x5gtn Total loading time: 0 Render date: 2024-05-14T04:49:46.362Z Has data issue: false hasContentIssue false

Solubility of Radionuclides in Fresh and Leached Cementitious Systems at 22°C and 50°C

Published online by Cambridge University Press:  10 February 2011

M. Ochs
Affiliation:
BMG Engineering Ltd, Ifangstrasse 11, CH-8952 Zürich-Schlieren, Switzerland
D. Hager
Affiliation:
BMG Engineering Ltd, Ifangstrasse 11, CH-8952 Zürich-Schlieren, Switzerland
S. Helfer
Affiliation:
BMG Engineering Ltd, Ifangstrasse 11, CH-8952 Zürich-Schlieren, Switzerland
B. Lothenbach
Affiliation:
BMG Engineering Ltd, Ifangstrasse 11, CH-8952 Zürich-Schlieren, Switzerland
Get access

Abstract

The solubility of Ni, Sn, Pb, Eu, and Sr was investigated at 22°C and 50°C in simulated cement porewaters corresponding to fresh cement (‘FPW’, pH 13.2) and cement leached of soluble alkalis, whose porewater chemistry is dominated by equilibrium with portlandite (‘APW’, pH 12.5). Solubility limits were approached from undersaturation, using Ni(OH)2(c), SnO2(c) (cassiterite), PbO(red), and Eu(OH)3(c) as solids. For Sr, no solubility experiments were carried out since the cement contains enough Sr to reach equilibrium with strontianite and celestite. Solubilities generally increase with increasing pH and temperature. The measured solubility of Pb ranges from about 4× 10−3 to 1×1O−2M and is within thermodynamically predicted values. The measured solubility of Ni is <O.5-1.3×10−7M in APW and about 3-4×10−7M in FPW, which is lower than predicted by most thermodynamic data. The measured solubility of Eu ranges from <6.6×10−10M in APW to 1.8-2.7×10−9M in FPW, which agrees well with thermodynamic calculations. The solubility of cassiterite is low, with dissolved Sn concentrations ranging from 3.5× 10−8M in APW to 3.3× 10−6M in FPW. Thermodynamic calculations predict much higher solubilities, presumably for less crystalline phases. However, oversaturation measurements in APW reproduced the solubility limits obtained by undersaturation within a factor of two. To our knowledge, no relevant thermodynamic data are available.

Type
Research Article
Copyright
Copyright © Materials Research Society 1998

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

REFERENCES

1 Berner, U., Nagra Technical Report NTB 90-12, Nagra, Wettingen, Switzerland, 1990.Google Scholar
2 Neall, F., Nagra Technical Report NTB 94-03, Nagra,Wettingen, Switzerland, 1994.Google Scholar
3 Rao, L., Rai, D. and Felmy, A.R., Radiochim. Acta 72, 151155 (1996).Google Scholar
4 Berner, U., Paul Scherrer Institute, Villigen, Switzerland, personal communication (1993)Google Scholar
5 OECD/NEA, NEA Data Bank, Gif-sur-Yvette, France (1986)Google Scholar
6 Pearson, F. J. Jr., and Berner, U., Nagra Technical Report NTB 91-17, Nagra, Wettingen, Switzerland, 1991.Google Scholar
7 Pearson, F. J. Jr., Berner, U. and Hummel, W., Nagra Technical Report NTB 91-18, Nagra, Wettingen, Switzerland, 1992.Google Scholar
8 Mattigod, S.V., Rai, D., Felmy, A.R. and Rao, L., J. Solution Chemistry, 26, 405417 (1997)Google Scholar
9 Pilkington, N.J. and Stone, N.S, NSS/R186, Harwell Laboratory, UKAEA, Harwell, 1990.Google Scholar
10 Baes, C. F. and Mesmer, R. E., The Hydrolysis of Cations, (Krieger Publishing, Malabar, USA, 1986).Google Scholar
11 Amaya, T., Chiba, T., Suzuki, K., Oda, C., Yoshikawa, H. and Yui, M., Mat. Res. Soc. Symp. Proc. 465, 751758 (1997)Google Scholar
12 Bayliss, S., Ewart, F.T., Howse, R.M., Lane, S.A., Pilkington, N.J., Smith-Briggs, J.L. and Williams, S.J., Mat. Res. Soc. Symp. Proc. 127, 879885 (1989)Google Scholar
13 Bayliss, S., Haworth, A., McCrohon, R., Moreton, A.D., Oliver, P., Pilkington, N.J., Smith, A.J. and Smith-Briggs, J.L., Mat. Res. Soc. Symp. Proc. 257, 641648 (1992)Google Scholar
14 Smith, R.E. and Martell, A.E., Critical Stability Constants. Vol. 4: Inorganic complexes, (Plenum Press, New York, 1976).Google Scholar
15 Bayliss, S., Ewart, F.T., Howse, R.M., Smith-Briggs, J.L., Thomason, H.P. and Willmott, H.A., Mat. Res. Soc. Symp. Proc. 112, 3342 (1988)Google Scholar
16 Ewart, F.T. and Tasker, P.W., Proc. Symp. Waste Management 87, 7178 (1987)Google Scholar
17 Bernkopf, M.F., Hydrolysereaktionen und Karbonatkomplexierung von dreiwertigen Americium im natuirlichen aquatischen System (Ph.D. thesis, Technical University of Munich, Munich, Germany, 1984).Google Scholar
18 Silva, R.J., Bidoglio, G., Rand, M.H., Robouch, P.B., Wanner, H. and Puigdomenech, I., Chemical Thermodynamics of Americium (North-Holland, Amsterdam, The Netherlands, 1995).Google Scholar