H. Christensen et al., OXIDATION OF NUCLEAR-FUEL (UO2) BY THE PRODUCTS OF WATER RADIOLYSIS -DEVELOPMENT OF A KINETIC-MODEL, Journal of alloys and compounds, 213, 1994, pp. 93-99
Radiolysis of groundwater will produce oxidants and reductants which c
an affect the oxidation and dissolution of used fuel (UO2) placed in a
geological disposal vault. A kinetic model to describe the oxidation
of UO2 by the products of radiolysis of water is described. This model
assumes that a monomolecular surface layer of UO2 reacts as if it wer
e dissolved in a thin layer of water of a thickness corresponding to t
he diffusion range of the radicals formed during radiolysis. In this m
anner we can use the rate constants for the reactions of radiolytic sp
ecies with dissolved uranium as an analog of the heterogeneous system
for which rate constants are unknown. The refinement of this model, ba
sed on a series of electrochemical and open-circuit corrosion experime
nts, is described. Model predictions are compared with dissolution rat
es measured in these experiments.