Instant Strong and Responsive Underwater Adhesion Manifested by Bioinspired Supramolecular Polymeric Adhesives

Abstract

Instant strong and responsive underwater adhesion is significant for many biomedical, industrial, and household applications. However, underwater adhesives simultaneously possessing these advantages are challenging to fabricate because strong and responsive adhesions are usually opposing properties. Herein, we have prepared bioinspired supramolecular polymeric adhesives containing complementary nucleobase moieties in nucleic acids and have demonstrated instantaneous underwater adhesion with an adhesion strength reaching as high as 1.5 MPa. Strong underwater adhesion is attributed to the high capability of the adhesives to substantially remove the interfacial water, which can be further modulated by temperature, light, and pH. Excellent underwater adhesion performances have been achieved on various substrates and under distinct aqueous conditions, showcasing the wide applications of the bioinspired nucleobase-containing adhesives developed here. This work opens up a new opportunity for fabricating underwater adhesives for diverse applications with the combined advantages of instant strong and responsive adhesion.

DNA Hydrogels in the Perspective of Mechanical Properties

“…[44] Therefore, the mechanical properties of the hydrogel are decisive to their applications. [45,46] Several strategies have been applied to strengthen gels in various dimensions. One of the main strategies to tune the mechanical properties of DNA hydrogel is changing the cross-linking modes, ranging from noncovalent interactions to covalent bonds, which further leads to various applications of DNA hydrogels.…”

Nucleobase-Interaction-Directed Biomimetic Supramolecular Self-Assembly

“… Schematic representation of the supramolecularly cross-linking hydrogel and the mechanism of adhesive performance induced by the nucleobase. Adapted from ref ( 58 ). Copyright 2022 American Chemical Society.…”

“…We have fabricated hydrophobic nucleobasecontaining adhesives by synthesizing a random copolymer using hydrophobic long aliphatic chain-containing monomers as well as both A-and T-containing monomers (Figure 9). 58 This elegantly designed supramolecularly assembled polymer network produced the strongest underwater adhesives reported to date, outperforming most previously reported underwater hydrogel-based adhesives.…”

“…Adhesion is another common property of living organisms, such as mussels clinging on rocks and geckos walking on vertical walls. As various non-covalent interactions are responsible for such adhesive properties, researchers have been interested in exploring adhesive materials based on nucleobase-pair interactions. − Long and co-workers prepared nucleobase-containing statistical copolymers by polymerizing A/T-functionalized acrylate monomers. Blending of A- and T-containing polymers led to supramolecularly cross-linked materials with tunable adhesive and cohesive strength depending on the A:T interaction.…”

“…Base-pair interactions have been explored to drive self-assembly to fabricate a wide variety of structures ranging from spherical micelles ,,, to vesicles, , one-dimensional fibers, ,, helices, and even more complex three-dimensional , structures, along with control of the functional design. These nucleobase-functionalized molecules and macromolecules have shown promising results in their prospective applications such as drug − and gene delivery, templated polymerization, − and superior adhesive − and self-healing , properties. The association constant of nucleobase interactions can be tuned from 10 2 to 10 6 M –1 as a function of several parameters such as the nature of the H-bonding unit, solvent polarity, temperature, , pH, , and number, sequence, and position of the nucleobases present in the system.…”