Passivation Effect of Metallic Uranium by Superitical Fluid CO2

The present work is devoted to examine the passivation effect of metallic uraniu by supercritical fluid CO2, which is the most significant. The structure and thermodynamic properties of UC, C, UO2 and supercritical fluid CO2 have been calculated, based on which following simultaneous reactions have been examined using chemical equilibrium theory. The results indicate that the △G° for U(α)+CO2(g)UO2(s)+C(Graphite) reaction is -149.8～-632.0 kJ, △G° for 2U(α)+CO2(g)UO2(s)+UC(s) reaction is -725.1～-730.2 kJ, and both △G＜０ and equilibrium closely approach products. It is also well known that the supercritical fluid is quite active in kinetics, and therefore the product compounds UC, C and UO2 would be quite stable. After the calculated molar tatio of UC, C and UO2, the stoichiometric ratio of elements is UC0.65±0.01O1.30±0.01, which would be useful for XPS observation.