Multicomponent pyrochlore solid solutions with uranium incorporation – A new perspective of materials design for nuclear applications

Abstract

Multicomponent pyrochlore solid solutions with and without uranium incorporation were fabricated and their thermal-mechanical properties were characterized. Multicomponent pyrochlore solid solutions without uranium exhibit comparable thermal conductivity and higher mechanical strength compared to baseline single component rare-earth titanate pyrochlore (A2Ti2O7). Uranium incorporation reduces hardness as compared with single component compositions. High entropy pyrochlore with uranium displays the highest thermal conductivity within multicomponent pyrochlore solid solutions with significantly better mechanical properties than UO2. The measured thermal conductivity correlates well with A-site cation mixing entropy and a modified size disorder parameter, and thus the size disorder and mixing entropy could be good indicators for predicting thermal conductivity of multicomponent pyrochlore solid solutions. This work opens up the possibility of designing multicomponent oxide solid solutions by controlling their chemical disorder/mixing entropy to achieve acceptable thermal-mechanical properties, desired radiation and corrosion performance for potential nuclear waste form and inert matrix fuel applications.