Abstract
When uranium or plutonium undergoes fission, the mean valency of the resulting fission product mixture may differ from that of the starting material. This paper describes the use of a computer programme to derive the composition of irradiated fuel, and how a combination of thermodynamic assessment and direct experiment is used to predict and confirm some of the consequences of the valency change in irradiated oxide fuels. The experiments consist of an X-ray study of the lattice dilation of uranium dioxide, a direct measurement of the oxygen/metal ratio in plutonium and mixed uranium-plutonium oxides, and electron probe microanalysis of inclusions formed in plutonium oxides. These demonstrate that the lanthanide fission products enter the oxide lattice so that irradiated uranium oxide does not become more oxidising with burn-up, but that plutonium oxide becomes significantly oxygen-rich during fission owing to the shift in the fission yield spectrum.
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