Fully Recycled Polyolefin Elastomer‐Based Vitrimers with Ultra‐High, Universal, Stable, and Switchable Adhesion

Achieving both robust adhesion to arbitrary surfaces and thermal-switchable/recyclable properties has proven challenging, particularly for commodity polyolefins. Herein, a simple and effective route is reported to transform polyolefins elastomer (POE) into a fully recycled epoxy-functionalized POE vitrimers (E-POE vit) with ultra-high, universal, stable, and switchable adhesion via facile free radical grafting and dynamic cross-linking. The resultant E-POE vit exhibits increase in adhesion strength on glass exceeding three to ten times compared to those commonly used polymers, due to the synergy of dense hydrogen (H)-bonds and strong interfacial affinity. In addition, E-POE vit also displays strong adhesion on diverse surfaces ranging from inorganic to organic while maintaining good stability in various harsh environments. More importantly, temperature-sensitive H-bonds allow E-POE vit to switch between attachment-detachment at alternating temperatures, resulting in reversible adhesion without adhesion loss, even after 10 cycles. Moreover, E-POE vit is able to be fully recycled and reused more than ten times via thermo-activated transesterification reactions with negligible change in structure and performance. This work may unlock strategies to fabricate high-performance commercial polymer-based adhesives with adhesion and recyclable features for intelligent and sustainable applications.