Characterization of radiation-induced aging in silica-reinforced polysiloxane composites

Changes in crosslink density and chemical structure of silica-reinforced silicone polymer composites due to aging in gamma radiation environments were examined in this study. Solvent swelling was utilized to determine the individual contributions of the matrix polymer and filler phase to the overall crosslink density of silica-reinforced silicone polymer composites. The results show how polymer–filler hydrogen bonding dominates the overall crosslink density of the material. Air-irradiated samples displayed decreased hydrogen bonding at the polymer–filler interface, while vacuum irradiation revealed the opposite effect. These results were supported by solid-state NMR experiments that correlated the motional dynamics of the polymer chains with crosslink density through T₂ relaxation time measurements. GC/MS analysis was used to identify degradation products formed as a result of irradiation and speculate upon likely degradation mechanisms.