Helium diffusion coefficient measurements in R7T7 nuclear glass by He(d,α)H nuclear reaction analysis

The immobilization of fission products and minor actinides by vitrification is the reference process for industrial management of high-level radioactive wastes generated by spent fuel reprocessing. Radiation damage and radiogenic helium accumulation must be specifically studied to evaluate the effects of minor actinide alpha decay on the glass long-term behavior under repository conditions.A specific experimental study was conducted for a comprehensive evaluation of the behavior of helium and its diffusion mechanisms in borosilicate nuclear waste glass. Helium production was simulated by external implantation with ³He ions at a concentration (≈1 at.%) 30 times higher than obtained after 10,000 years of storage. Helium diffusion coefficients as a function of temperature were extracted from the depth profiles after annealing. The ³He(d,α)¹H nuclear reaction analysis (NRA) technique was successfully adopted for low-temperature in situ measurements of depth profiles. Its high depth resolution revealed helium mobility at temperatures as low as 253 K and the presence of a trapped helium fraction. The diffusion coefficients of un-trapped helium atoms follow an Arrhenius law between 253 K and 323 K. An activation energy of 0.55 ± 0.03 eV was determined, which is consistent with a process controlled by diffusion in the glass free volume.