Strong and ductile adhesives often undergo both interfacial and cohesive failure during the debonding process. Herein, we report a rare self-reinforcing polyurethane adhesive that shows the different phenomenon of only interfacial failure yet still exhibiting superior adhesive strength and toughness. It is synthesized by designing a hanging adhesive moiety, hierarchical H-bond moieties, and a crystallizable soft segment into one macromolecular polyurethane. The former hanging adhesive moiety allows the hot-melt adhesive to effectively associate with the target substrate, providing sufficient adhesion energy; the latter hierarchical H-bond moieties and a crystallizable soft segment cooperate to enable the adhesive to undergo large lap-shear deformations through sacrificing weak bonds and mechano-responsive strength through the fundamental mechanism of strain-induced crystallization. As a result, this polyurethane adhesive can keep itself intact during the debonding process while still withstanding a high lap-shear strength and dissipating tremendous stress energy. Its adhesive strength and work of debonding are as high as 11.37 MPa and 10.32 kN m−1, respectively, outperforming most reported tough adhesives. This self-reinforcing adhesive is regarded as a new member of the family of strong and ductile adhesives, which will provide innovative chemical and structural inspirations for future conveniently detachable yet high-performance adhesives.
Jinming Liu,Yiyu Cao,Haiming Chen,Haohao Lin,Dongsheng Mao
A robust and highly responsive pressure-sensitive adhesive (PSA) holds significant importance in interface interaction technology, requiring specific attributes such as a low modulus for surface adhesion, high strength to withstand stress, and responsiveness to external stimuli. However, achieving these requirements is often challenging due to structural limitations. In this study, a series of supramolecular ionogels with quadruple hydrogen bonding cross-linked networks and mobile ions were developed to decouple the modulus-strength relationship, thereby enhancing sensing performance. The quadruple hydrogen bonds cross-linked supramolecular networks exhibit good strength even with an increased ionic liquid content of up to 30 wt %. As a result, impressive lap-shear strengths of 2165.1 kPa on aluminum and tacking bond strengths of 1842.6 kPa on glass were attained, surpassing most of the literature-reported values. Additionally, the movement or orientation of ions under voltage application led to a 69.5% enhancement in the bonded strength. Moreover, the PSA demonstrated stress sensing capabilities, achieving a sensitivity of 32.2 MPa–1 in lap-shear applications and 9.5 MPa–1 in compression scenarios.
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