Quantitative Assessment of the Instant Release Fraction (IRF) for Fission Gases and Volatile Elements as a Function of Burnup and Time under Geological Disposal Conditions

Abstract

ABSTRACTThe Instant Release Fraction at container failure time, IRF(t), is here considered as being the sum of (i) the initial labile fraction, corresponding to the sum of gap and grain boundary inventories of certain radionuclides on exit from the reactor, with a further possible contribution from segregation in the rim region and (ii) the time-dependent fraction of radionuclides accumulating at grain boundaries due to a self-irradiation enhanced diffusion through the grains. The initial labile fraction of radionuclides such as 14C, 36Cl, 79Se, 129I, and 135Cs has been estimated based on leaching experiments, post-irradiation fission gas release measurements and studies of solid-state chemistry of spent fuel, along with estimates of fission product segregation in the rim zone. The contribution of the a self-irradiation enhanced diffusion has also been estimated based on a diffusion coefficient decreasing with time proportionally with the volume α-activity of the spent fuel. Its contribution to the IRF is limited for UO2 fuels. The proposed bounding values of the IRF for fuel with a burnup of 55 GWd/tIHM for 14C, 36Cl, 79Se, 129I, and 135Cs are 11 % at t=0 and close to 15 % at a container failure time of 10,000 y.