Radionuclide 137Cs is one of the major fission products that dominate heat
generation in spent fuels over the first 300 years. A durable waste
form for 137Cs that decays to 137Ba is needed
to minimize its environmental impact. Aluminosilicate pollucite CsAlSi2O6 is selected as a model waste form to study the
decay-induced structural effects. Whereas Ba-containing precipitates
are not present in charge-balanced Cs0.9Ba0.05AlSi2O6, they are found in Cs0.9Ba0.1AlSi2O6 and identified as monoclinic
Ba2Si3O8. Pollucite is susceptible
to electron-irradiation-induced amorphization. The threshold density
of electronic energy deposition for amorphization was determined to
be ∼235 keV/nm3. Pollucite can be readily amorphized
under F+ ion irradiation at 673 K. A significant amount
of Cs diffusion and release from the amorphized pollucite occurs during
the irradiation. However, cesium is immobile in the crystalline structure
under He+ ion irradiation at room temperature. The critical
temperature for amorphization is not higher than 873 K under F+ ion irradiation. If kept at or above 873 K all the time,
the pollucite structure is unlikely to be amorphized; Cs diffusion
and release are improbable. A general discussion regarding pollucite
as a potential waste form is provided in this report.