Assessment of surface reactivity of thorium oxide in conditions close to chemical equilibrium by isotope exchange Th-229/Th-232 method

摘要

This work aims to assess the solubility and the surface reactivity of crystallized thorium at pH 3.0 in presence of three types of solids: synthesized powder at 1300 degrees C, crushed kernel, and intact kernel. In this study, the kernel is composed by the core solid from high temperature reactors (HTR) sphere particles. The originality of this work consisted in following in a sequential order the kinetic of dissolution, the surface reactivity in presence of isotope tracer Th-229, and its desorption process. Long time experiments (634 days) allowed to get deeper understanding on the behavior of the surface reactivity in contact with the solution. Solubility values are ranging from 0.3 x 10(-7) mol.L-1 to 3 x 10(-7) mol.L-1 with a dissolution rate of 10(-6)-10(-4) g.m(-2) day(-1). PHREEQC modeling showed that crystallized ThO2(cr, 20 nm) phase controls the equilibrium in solution. Isotope exchange between Th-229 and Th-232 indicated that well-crystallized phase exist as an inert surface regarding to the absence of exchange between surface solid and solution.