Hostname: page-component-586b7cd67f-2brh9 Total loading time: 0 Render date: 2024-11-29T08:16:01.694Z Has data issue: false hasContentIssue false

On the Oxidation of Uraninite From Natural Reactor Cores

Published online by Cambridge University Press:  10 February 2011

Daqing Cui
Affiliation:
Department of Chemistry, Nuclear Chemistry, Royal Institute of Technology, S-100 44 Stockholm, Sweden
Trygve Eriksen
Affiliation:
Department of Chemistry, Nuclear Chemistry, Royal Institute of Technology, S-100 44 Stockholm, Sweden
Ulla-Britt Eklund
Affiliation:
Studvik Nuclear AB, S-611 82 Nykölping, Sweden
Get access

Abstract

Natural nuclear reactors provide unique evidence in helping to understand the processes that might occur over long timescales in radioactive waste disposal sites. In the presented work, the extent and kinetics of oxidation of core material from the Oklo-Bangombé natural reactors are investigated. The X-ray powder diffraction analysis shows that the uraninites core samples from the Bangombé Reactor and Oklo Reactor 2. and Oklo Reactor 13 have the same unit-cell parameters as synthetic UO2.25. A significant amount of fourmarierite, Pb(UO2)4O3(OH)4 4H2O, was identified in the core samples from two shallow reactors Bangombé and Oklo 2, but not in the deeper reactor Oklo 13. The results of U(IV)/U(IV) measurements indicate that the extent of oxidative weathering of shallow reactors (Bangombé and Oklo 2) is greater than for the deeper reactor Oklo 13. Evaporable organic compounds found in the uraninite inclusion containing “bitumen” at the edge of Okelobondo Reactor (400 °C) and in the black shale immediately above the Bangombé Reactor (260 °C) may work as a reducing buffer or/and a hydrophobic water shield to depress the oxidative dissolution of the uraninite cores.

Type
Research Article
Copyright
Copyright © Materials Research Society 1999

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. Gauthier-Lafaye, F., Holliger, P., Blanc, P.L., Natural fission reactors in the Franceville basin, A review of the conditions and results of a open-quotes critical evenclose quotes in a geologic system. Geochimica et Cosmochimica, 60, p.4861–4852 (1996)Google Scholar
2. Jensen, K.A. and Ewing, R. C., Petrography and chemistryV of the uraninite and uraninite alteration phase from the uranium ore-deposit at Bangombé, Oklo working group proceedings of the first EC-CEA work shop on Oklo – natural analogue phase II project, Sities Spain, 1997 EUR 18314 EN, p.139159 Google Scholar
3. Jensen, K.A., Ewing, R. C. and Gauthier-Lafaye, F., Uraninite A2GA Spent nuclear fuel from the natural fission reactor at Bagombe in Garbon, West Africa. Scientific Basis for Nuclear Waste Management XX Symposium, MRS, Pittsburgh, 1997, p12091218.Google Scholar
4. Zetterstrdm, L., Lead isotope studies of galenas and uraninite at Oklo, Oklo working group proceedings of the first EC-CEA work shop on Oklo – natural analogue phase II project, Sitjes Spain, 1997, EUR 18314 EN, p.171179.Google Scholar
5. Piret, P., The crystal structure offourmarierite Pb(U02)403(OH)4.4H20, Bulletin-de-Mineralogie-France, 108(5) p.659665, (1985).Google Scholar
6. Finch, R. J., Ewing, R.C., Alteration of natural UO2 under oxidising conditions from Shinkolobwe, Katanga Zaire: A natural analogue for the corrosion of spent fuel. Radochimica Acta, 52/53, p.395401, (1991).Google Scholar
7. Snelling, A. A., Uranium and its alteration products, Koongara uranium deposit, International uranium symposium on the Pine Creek Geosyncline, Sydney, 1979, p. 48.Google Scholar
8. Bromn, A., X-ray powder diffraction with Guinier-Hdigg Focusing Cameras, AE-409, Appendix II, (1970), Aktiebolaget Atomenergi, Studsvik, Sweden.Google Scholar
9. Brina, R., Miller, A. G., Determination of uranium and lanthanides in real-world samples by kinetic phosphorescence analysis, Spectroscopy, 8(3), p. 25, (1993)Google Scholar
10. Sunder, S., Sargent, F.P., Miller, N. H., X-ray photoelectron spectroscopic study of sample from a natural fission reactor at Oklo, in proc. 2nd CEC-CEA progress meeting, Brussels. 1992, EUR 14877 ENGoogle Scholar
11. Sunder, S.. Miller, N. H., and Duclos, A. M., Geochemistry of samples from naturalfissionreactors in Oklo uranium deposit: an XPS and XRD study, in Proc. 3rd Joint CEC-CEA Progress Meeting. Brussels, 1993, EUR 14877 EN.Google Scholar
12. Willis, B.T. M., Structure of UO2, UO2+x, and U4O9 by neutron diffraction. La diffraction et la diffusion des neutrons. Colloques Internationaux de Centre National de la Recherch. Scientifique, No. 126, Grenoble, 1963, p.7. 1964.Google Scholar
13. Puigdomench, I. and Bruno, J., Modeling uranium solubilities in aqueous solutions: validation of a thermodynamic data base for the EQ3/6 geochemical codes. Swedish Nuclear Fuel and Waste Management Co. (SKB) Technical Report, TR 88-21, Stockholm, 1988.Google Scholar