Effect of wet and dry cycles on dissolution of relatively insoluble particles containing Pu

Dissolution of gross alpha emitter radioactivity from particles composed of mixed uranium and plutonium oxides or of plutonium dioxide continually immersed in solvent typically display at least a two-phase dissolution pattern. Rapid dissolution of a small fraction of the total particulate mass is followed by much slower dissolution for the majority of the particulate mass. In this study, respirable particles of (U, Pu)O2 and PuO2 were subjected to dissolution using an alternate wetting and drying cycle. Particles were continuously immersed in solvent for 4 d and then dried in air for 3 d. This cycle was repeated weekly for 7 wk. Four solvents were used to represent a range of potential environmental conditions and a fifth solvent was used for comparison to other continuous immersion studies. In contrast to dissolution studies involving continuous immersion over periods of two or more weeks that exhibit a three-phase dissolution process, the alternate wet-dry cycling resulted in repetition of the first two phases of the dissolution pattern for each cycle. This led to significantly enhanced dissolution of both particulate materials. The enhancement in total dissolution ranged from two to ten times larger during each wet-dry cycle compared to studies involving continuous immersion. The results indicate a potential need to re-evaluate environmental models of actinide element bioavailability for particulate materials released to environments where wet-dry cycling may be routine, i.e. intermittent rainfall in an otherwise arid climate or in stream beds with intermittent flow.