Determination of oxygen stoichiometry of oxide fuel during high temperature vapour pressure measurement

Abstract

This study presents an original approach of oxygen stoichiometry determination during high temperature (>2000K) measurements of vapour pressure using the Knudsen effusion mass spectrometry technique. The method has been developed taking into account the vapour pressure measurements of series of (U1-x,Pux)O2 samples with x(Pu)=0.25, 0.5, 0.75 together with pure UO2 and PuO2 end-members coupled with equilibrium calculations based on thermodynamic assessment of the U-Pu-O system. The presented method consists of two steps; in the first step the oxygen potential of the oxide phase is determined based on the measured partial vapour pressures of UO(g), UO2(g), PuO(g) and PuO2(g) gaseous species and during the second step the thus determined oxygen potential is attributed with matching oxygen stoichiometry of the sample. From the obtained results it has been demonstrated that it is possible to accurately estimate the oxygen stoichiometry of the mixed oxide fuel samples knowing the description of the oxygen potential of corresponding end-members only.