Interdiffusion coefficients of plutonium and uranium have been calcula
ted from electron microprobe analysis of diffusion couples UO2 (green
compact) / PuO2 (green compact) or UO2 (green compact) / UO2+PuO2 (gre
en compact). A series of these diffusion couples was sintered at 1773,
1873 and 2023 K during 0 to 50 hours and under controlled oxygen pote
ntial (-88, -95 and -125 kcal/mol). The results show that grain-bounda
ry diffusion predominates in the overall diffusion process, even durin
g sintering and that lattice diffusion is very slow. The sintering pro
cess enhances the interdiffusion coefficients which are greater by one
order of magnitude compared to those of polycrystalline diffusion cou
ples.