Abstract The corrosion of nuclear fuel under waste disposal conditions is likely to be influenced by the bicarbonate/carbonate content of the groundwater since it increases the solubility of the UVI corrosion product, [UO2]2+. As one of the half reactions involved in the corrosion process, the anodic dissolution of SIMFUEL (UO2) has been studied in bicarbonate/carbonate solutions (pH 9.8) using voltammetric and potentiostatic techniques and electrochemical impedance spectroscopy. The reaction proceeds by two consecutive one electron transfer reactions (UIV → UV → UVI). At low potentials (≤250 mV (vs. SCE) the rate of the first electron transfer reaction is rate determining irrespective of the total carbonate concentration. At potentials >250 mV (vs. SCE) the formation of a UVIO2CO3 surface layer begins to inhibit the dissolution rate and the current becomes independent of potential indicating rate control by the chemical dissolution of this layer.