Surface thermodynamics of yttrium titanate pyrochlore nanomaterials†

Nanocrystalline pyrochlore materials have been investigated for their enhanced radiation tolerance as ceramic nuclear waste hosts. In this work, we study the thermodynamic driving force of nano-scale materials for radiation resistance. The size dependent thermodynamic properties of a series of Y₂Ti₂O₇ nanoparticles were investigated. Samples were synthesized by a sol–gel method and characterized by synchrotron X-ray diffraction, BET analysis, and thermogravimetric analysis. The surface and interface enthalpies of Y₂Ti₂O₇ were determined by high temperature oxide melt drop solution calorimetry to be 4.07 J m⁻² and 3.04 J m⁻², respectively. The experimentally obtained surface energy is in good agreement with computationally derived average surface energies for yttrium and other rare-earth titanate pyrochlores. Theoretical links between nanoparticle stability, surface energy, and radiation resistance of pyrochlore materials were then explored.