Molecular Insights into Adhesion at a Buried Silica-Filled Silicone/Polyethylene Terephthalate Interface

Silicone adhesives are widely used in many important applications in aviation, automotive, construction, and electronics industries. The mixture of (3-glycidoxypropyl)trimethoxysilane (γ-GPS) and hydroxy-terminated dimethyl methylvinyl co-siloxanol (DMMVS) has been widely used as an adhesion promoter in silicone elastomers to enhance the adhesion between silicone and other materials including polymers. The interfacial molecular structures of silicone elastomers and the adhesion promotion mechanisms of a γ-GPS-DMMVS mixture in silicone without a filler or an adhesion catalyst (AC) have been extensively investigated using sum frequency generation (SFG) vibrational spectroscopy previously. In this research, SFG was applied to study interfacial structures of silicone elastomeric adhesives in the presence of a silica filler and/or a zirconium(IV) acetylacetonate adhesion catalyst at the silicone/polyethylene terephthalate (PET) interface in situ nondestructively to understand their individual and synergy effects. The interfacial structures obtained from the SFG study were correlated to the adhesion behavior to PET. The interfacial reactions of methoxy and epoxy groups of the adhesion promoter were found to play significant roles in enhancing the interfacial adhesion of the buried interface. This research provides an in-depth molecular-level understanding on the effects of a filler and an adhesion catalyst on the interfacial behavior of the adhesion promotion system for silicone elastomers as well as the related impact on adhesion.