Abstract
ABSTRACTInteractions during extended exposure of UO2 to 2:1 H2+O2 mixtures at room temperature and 0.13 bar pressure are investigated in an effort to describe chemical and kinetic behavior of spent fuel following contact with groundwater. Oxidation of UO2 to UO2+x by O2 occurs initially when oxide is directly exposed to the gas mixture or submerged in water, but immersion is accompanied by a 25-fold reduction in the rate. The initial rate is proportional to [O2]2 for gasphase oxidation and to [O2]1.5 for the submerged oxidation. Continued measurement during direct oxide-gas contact indicates sequential reactions in which the UO2+x product is further oxidized by H2O and ultimately reacts with H2 to form an oxide hydride.
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