Constructing Robust and Anti‐Aging Elastomer Composites via Natural Polyphenol‐Induced Dynamic Interfacial π‐π Stacking Interaction

ABSTRACT Robust and anti‐aging elastomer composites are witnessing growing demand in cutting‐edge fields such as intelligent equipment, yet their fabrication still faces significant challenges. In this work, by synergistically integrating the advantages of dynamic elastomer‐filler interfacial interactions and non‐migratory antioxidants, natural polyphenol resveratrol (Res) was covalently grafted onto nano‐silica (SiO 2 ) surfaces, yielding Res‐functionalized SiO 2 (SiO 2 ‐Res), which was subsequently incorporated into styrene‐butadiene rubber (SBR) as a functional filler to fabricate SBR composite. The grafted Res formed dynamic π‐π stacking interactions with SBR chains, which significantly suppressed the Payne effect of SiO 2 ‐Res and improved its dispersion in SBR. Consequently, SiO 2 ‐Res showed superior reinforcing efficiency for SBR compared to unmodified SiO 2 and silane modified SiO 2 . For instance, at the filler loading of 30 phr, the SBR/SiO 2 ‐Res composite exhibited a remarkable 87% improvement in tensile strength over SBR/SiO 2 while concurrently improving the elasticity. In addition, SiO 2 ‐Res significantly improved the thermo‐oxidative stability of SBR composites. This improvement is attributed to the efficient free radical scavenging by phenolic hydroxyl groups in the grafted Res with good migration resistance and thermal stability during thermal‐oxidative aging. This strategy may introduce a promising approach for the fabrication of elastomers with dual‐enhanced aging stability and mechanoelasticity.