Radiation damage effects in candidate titanates for Pu disposition: Zirconolite

Results from studies of radiation-induced damage from the alpha decay of 238Pu on the density and crystal structure of a nominally phase-pure zirconolite and two other zirconolite-bearing ceramics are discussed. Macro and micro swelling were found to be temperature independent, whereas the density determined with He gas pycnometry was temperature dependent. Approximately 2.6 × 1018 α/g were needed to render the specimens X-ray amorphous– more to saturate the swelling. Unlike pyrochlore-based ceramics, we did not observe any phase changes associated with storage temperature and damage ingrowth. The forward dissolution rate at a pH value of 2 for material containing essentially all zirconolite is 1.7(4) × 10−3 g/(m2 d) with very little pH dependence and no dependence on the amount of radiation-induced damage. Even after the radiation-induced swelling saturated, the specimens remained physically intact with no evidence for microcracking. Thus, the material remains physically a viable material for the disposition of surplus weapons-grade Pu.