Spent UO$_{2}$ TRISO coated particles - instant release fraction and microstructure evolution

The impact of burn-up on the instant release fraction (IRF) from spent fuel was studied using very high burn-up UO2 fuel (∼ 100 GWd/t) from a prototype high temperature reactor (HTR). TRISO (TRi-structural-ISO-tropic) particles from the spherical fuel elements contain UO2 fuel kernels (500 μm diameter) which are coated by three tight layers ensuring the encapsulation of fission products during reactor operation. After cracking of the tight coatings 85Kr and 14C as 14CO2 were detected in the gas fraction. Xe was not detected in the gas fraction, although ESEM (Environmental Scanning Electron Micoscope) investigations revealed an accumulation in the buffer. UO2 fuel kernels were exposed to synthetic groundwater under oxic and anoxic/reducing conditions. U concentration in the leachate was below the detection limit, indicating an extremely low matrix dissolution. Within the leach period of 276 d 90Sr and 134/137Cs fractions located at grain boundaries were released and contribution to IRF up to max. 0.2% respectively 8%. Depending on the environmental conditions, different release functions were observed. Second relevant release steps occurred in air after ∼ 120 d, indicating the formation of new accessible leaching sites. ESEM investigations were performed to study the impact of leaching on the microstructure. In oxic environment, numerous intragranular open pores acting as new accessible leaching sites were formed and white spherical spots containing Mo and Zr were identified. Under anoxic/reducing conditions numerous metallic precipitates (Mo, Tc and Ru) filling the intragranular pores and white spherical spots containing Mo and Zr, were detected. In conclusion, leaching in different geochemical environments influenced the speciation of radionuclides and in consequence the stability of neoformed phases, which has an impact on IRF