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 GdIII-Oxygen vacancy (OV) clusters which limits the availability of these vacancies required to accommodate excess O2− during matrix oxidation to UIV1−2xUV2xO2+x. The subsequent reaction of this oxidized surface layer to UVIO3.yH2O/UVIO2(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 UVI surface species prior to dissolution.
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