Discrepancies in thorium oxide solubility values: a new experimental approach to improve understanding of oxide surface at solid/solution interface

Abstract

AbstractThe solubility of ThO2(cr) was studied since many years but a large discrepancy in solubility values is noticed in the literature. The present work suggests that this discrepancy is related to differences in the surface properties of thorium oxide.To understand the role of surface properties on solubility values, we conducted experiments with ThO2(cr) spheres with reproducable surface properties. Batch dissolution experiments were conducted in 0.01 M NaCl solution at pH=3.0 and 4.0 for periods of time up to 270 days. The solutions were spiked with229Th to determine precipitation (sorption) rates of thorium, while dissolution rates were determined by measuring232Th released from ThO2(cr) spheres. We assume that229Th atoms are exchanged only with active sites involved in Th-dissolution. Using229Th as local sensor of attachement and detachment processes at the ThO2(cr) surface under close-to-equilibrium conditions, allows to assess surface reactivity of the solid during solubility experiments.