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Effect of cement water on UO2 solubility

Published online by Cambridge University Press:  03 July 2014

C. Cachoir
Affiliation:
SCK•CEN, Boeretang 200, B-2400 Mol, Belgium
Th. Mennecart
Affiliation:
SCK•CEN, Boeretang 200, B-2400 Mol, Belgium
K. Lemmens
Affiliation:
SCK•CEN, Boeretang 200, B-2400 Mol, Belgium
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Abstract

To assess the stability of spent fuel in the highly alkaline chemical environment of the Belgian Supercontainer design, static leach experiments were performed with depleted UO2 and 238Pu-doped UO2 at different SA/V ratios for 1.5 years in cement waters (11.7< pH < 13.5) at ambient temperature and under argon atmosphere. The influence of the calcium concentration on the uranium release was also investigated. While the ultrafiltered U(IV) concentration was 10-9-10-8 mol.L-1 and independent of the pH, the U(VI) release from the UO2 surface was enhanced by the OH- concentration, leading to soluble U concentrations up to 10-5 mol.L-1 at high SA/V and under the influence of radiolysis. Together with the high Ca concentration, this can lead to the formation of Ca-U(VI) colloids as precursor of Ca-U(VI) secondary phases, decreasing the soluble U concentration. The precipitation of Ca-U secondary phases was however not clearly evidenced by surface analyses.

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Articles
Copyright
Copyright © Materials Research Society 2014 

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