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

Abstract

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.