Y. Asano et al., KINETIC-STUDIES ON DISSOLUTION OF UO2 POWDERS IN ACID-SOLUTIONS BY USING CERIUM(IV) OR CHLORINE DIOXIDE AS OXIDANTS, Journal of Nuclear Science and Technology, 33(2), 1996, pp. 152-156
The UO2 powders of 100-150, 150-212, 212-250, and 250-300 mu m were di
ssolved in HNO3 or HCl solutions containing strong oxidants to examine
their effect on the dissolution rates. Cerium(IV) species and ClO2 we
re used as oxidants in HNO3 and HCl solutions, respectively The Ce(IV)
species were prepared by bubbling O-3 gas into HNO3 solutions contain
ing Ce(NO3)(3). All dissolution experiments were carried out under rap
id stirring conditions which make it possible to neglect the diffusion
effect. Dissolution reactions were analyzed on the assumptions that t
he UO2 powders are spherical particles and homogeneously dissolved fro
m their external surface. Dissolution rate constants (Phi) in mol . cm
(-2). min(-1) were measured at various concentrations of oxidants and
temperatures. Furthermore, the effect of acid concentrations on the di
ssolution rate was also examined. As a result, the dissolution rate co
nstants Phi were found to be expressed as Phi=k(N)[Ce(IV)][H+](0.6) fo
r HNO3 solution([HNO3]=1-5 M, Temp. less than or equal to 30 degrees C
) and Phi=k(H) [ClO2][H+](-0.3) for HCl solution([HCl]=1-5 M, Temp. le
ss than or equal to 30 degrees C), respectively. Activation energies(k
J . mol(-1)) for the apparent dissolution rate constants are 44.1+/-1.
9 for the HNO3 solution system and 33.5+/-2.8 far the HCl solution sys
tem. respectively.