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Effect of Alpha Radiolysis on UO2 Dissolution under Reducing Conditions

Published online by Cambridge University Press:  01 February 2011

T. Mennecart ,
B. Grambow ,
M. Fattahi ,
G. Blondiaux  and
Z. Andriambololona
T. Mennecart
Affiliation:
SUBATECH - Ecole des Mines de Nantes, 4 rue Alfred Kastler, BP 20722 – 44307 Nantes cedex 3., France Agence Nationale pour la gestion des Déchets RAdioactifs, Parc de la Croix Blanche, 1/7 rue Jean Monnet, 92290 Châtenay-Malabry Cedex, France
B. Grambow
Affiliation:
SUBATECH - Ecole des Mines de Nantes, 4 rue Alfred Kastler, BP 20722 – 44307 Nantes cedex 3., France
M. Fattahi
Affiliation:
SUBATECH - Ecole des Mines de Nantes, 4 rue Alfred Kastler, BP 20722 – 44307 Nantes cedex 3., France
G. Blondiaux
Affiliation:
Centre d'Etude et de Recherche par Irradiation (CNRS), 3A, rue de la Férollerie, 45071, Orléans cedex 2, France
Z. Andriambololona
Affiliation:
Agence Nationale pour la gestion des Déchets RAdioactifs, Parc de la Croix Blanche, 1/7 rue Jean Monnet, 92290 Châtenay-Malabry Cedex, France
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Abstract

Effects of water radiolysis on the dissolution rate of UO2 were studied by irradiating UO2 colloids with an alpha particle beam of a cyclotron. The solution was kept under reducing conditions by applying a current of -10 or -50 nA and an ultrahigh purity argon bubbling. The solution pH was fixed at 6 during experiment. The particle flux was 1.1×1011 α.cm−2.s−1 entering in solution with an energy of 5 – 6 MeV. Despite initial reducing conditions water radiolysis increased the dissolution rate of uranium dioxide due to reaction with oxidizing radiolytic species such as H2O2, O2, OH•, HO2•, ClO3−. The monitoring of the redox potential showed that the solutions became rapidly oxidizing. The dissolution rate values were between 0.01 and 26 mg·m−2·d−1 depending on the ratio of the irradiated UO2 mass to the solution volume. This dependency is caused by hydrogen peroxide consumption at the UO2 surface. The rate of hydrogen peroxide consumption by reaction with colloids corresponds to an equivalent rate of UO2 oxidation/dissolution between 2 and 60 mg.m−2.d−1 indicating that only a small fraction of produced H2O2 is consumed by the dissolution reaction.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 807: Symposium Scientific Basis for Nuclear Waste Management XXVII , 2003 , 403
Copyright
Copyright © Materials Research Society 2004

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References

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