Hostname: page-component-586b7cd67f-rcrh6 Total loading time: 0 Render date: 2024-11-29T07:28:36.328Z Has data issue: false hasContentIssue false

Thermodynamic Modelling of the Effect of Hydroxycarboxylic Acids on the Solubility of Plutonium at High pH

Published online by Cambridge University Press:  01 January 1992

Anthony D Moreton*
Affiliation:
AEA Decommissioning & Radwaste, B.424.4, Harwell Laboratory, Oxfordshire, UK
Get access

Abstract

A number of the hydroxycarboxylic acids generated by the alkaline degradation of cellulosic wastes under reducing conditions in a cementitious repository can significantly increase the solubility of the actinides at high pH, especially plutonium. The solubility of plutonium at pH 12, in the presence of a range of hydroxycarboxylic acids containing a number of hydroxyl groups and between one and three carboxylate groups, has been modelled using the HARPHRQ code. All the plutonium-organic complexes assumed in the model are based on a stable unit in which a central plutonium ion is bound by four oxygen atoms. The oxygen atoms can be provided either by a deprotonated hydroxyl group on one of the ligands, or by hydroxide ions.

Type
Research Article
Copyright
Copyright © Materials Research Society 1993

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. Cross, J.E., Ewart, F.T. and Greenfield, B.F.,. Modelling the behaviour of organic degradation products. UK Nirex Ltd. Report NSS/R151 (1989).Google Scholar
2. Brown, P.L., Cross, J.E. and Hobley, J.. Modelling the effect of organic degradation products on actinide solubilities. UK Nirex Ltd. Report NSS/R211 (in publication, 1992).Google Scholar
3. Greenfield, B.F., Spindler, M.W. and Woodwark, D.R.,. Summary of the effects of organic degradation products on near-field radionuclide chemistry. UK Nirex Ltd. Report NSS/R298 (in publication).Google Scholar
4. Greenfield, B.F., Moreton, A.D., Spindler, M.W., Williams, S.J. and Woodwark, D.R.,. The effects of the degradation of organic materials in the near field of a radioactive waste repository. Paper presented at MRS'91, November 1991, Strasbourg. Sci. Basis Nucl. Waste Management XV, to be published.Google Scholar
5. Brown, P.L., Haworth, A., Sharland, S.M. and Tweed, C.J.,. HARPHRQ: A geochemical speciation program based on PHREEQE. UK Nirex Ltd. Report NSS/R188 (1991).Google Scholar
6. Cross, J.E. and Ewart, F.T.,. HATCHES - A thermodynamic database and management system. UK Nirex Ltd. Report NSS/R212 (1990).Google Scholar
7. Motekaitis, R.J. and Martell, A.E.,. Complexes of aluminium (III) with hydroxy carboxylic acids. Inorg. Chem. 1984, 23, 1823.Google Scholar
8. Gil, V.M.S.,. NMR comparative study of the complexation of oxoions of V(V), Mo(VI), W(VI) and U(VI) with 0a-hydroxycarboxylic acids. Pure & Appl. Chem., 1989, 61, 841848.Google Scholar
9. Martell, A.E. and Smith, R.M.,. Critical stability constants Volume 3, 'Other organic ligands' (Plenum Press, 1979).Google Scholar
10. Streitweiser, A. and Heathcock, C H. Introduction to organic chemistry (2nd Edn, Collier Macmillan, New York, 1981).Google Scholar
11. Cross, J.E., Moreton, A.D. and Tweed, C.J.,. Thermodynamic modelling of radioactive waste disposal: Assessment of near-field solubility. UK Nirex Ltd. Report NSS/R311 (in publication, 1992).Google Scholar
12. Moreton, A. D.. Data to be published as UK Nirex Ltd. Safety Studies Report (1992, in preparation).Google Scholar