The Electrochemical Reactivity of 6.0 wt% Gd-Doped UO2 in Aqueous Carbonate/Bicarbonate Solutions
JOURNAL OF THE ELECTROCHEMICAL SOCIETY(2014)
Abstract
The effect of gadolinium doping on the anodic reactivity of UO2 in aqueous carbonate solutions has been investigated voltammetrically, potentiostatically, by Raman spectroscopy and X-ray photoelectron spectroscopy. The mechanism of oxidation/dissolution is the same as on undoped UO2 and lightly doped SIMFUEL (doped UO2) but the reactivity is significantly reduced. This is attributed to the formation of Gd-III-Oxygen vacancy (O-V) clusters which limits the availability of these vacancies required to accommodate excess O2- during matrix oxidation to (U1-2 lambda U2xO2+x)-U-IV-O-v. The subsequent reaction of this oxidized surface layer to (UO3 center dot yH2O)-O-VI/(UO2)-O-VI(CO3)(x)((2-2x)+) is also suppressed by Gd-doping. The overall oxidation/alteration (dissolution) reaction appears to be kinetically controlled by the creation of U-VI surface species prior to dissolution. (C) 2014 The Electrochemical Society.
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Key words
electrochemical reactivity,aqueous carbonate/bicarbonate,gd-doped
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