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In this study, oxygen exchange reactions performed on PuO₂ suggest the reaction is influenced by at least three mechanisms: an internal chemical reaction, surface mobility of active species/defects, and surface exchange of gaseous oxygen with lattice oxygen. Activation energies for the surface mobility and internal chemical reaction are presented. Determining which mechanism is dominant appears to be a complex function including at least specific surface area and temperature. Thermal exposure may also impact the oxygen exchange reaction by causing reductions in the specific surface area of PuO₂. Previous CeO₂ surrogate studies exhibit similar behavior, confirming that CeO₂ is a goodmore » qualitative surrogate for PuO₂, in regards to the oxygen exchange reaction. Comparison of results presented here with previous work on the PuO₂ oxygen exchange reaction allows complexities in the previous work to be explained. These explanations allowed new conclusions to be drawn, many of which confirm the conclusions presented here.« less