Elasticity‐Dependent Fast Underwater Adhesion Demonstrated by Macroscopic Supramolecular Assembly

Abstract

Macroscopic supramolecular assembly (MSA) is a recent development in supramolecular chemistry to associate visible building blocks through non-covalent interactions in a multivalent manner. Although various substrates (e.g. hydrogels, rigid materials) have been used, a general design rule of building blocks in MSA systems and interpretation of the assembly mechanism are lacking and are required. Herein we design three model systems with varied elastic modulus and correlated the MSA probability with the elasticity. Based on the effects of substrate deformability on multivalency, we have proposed an elastic-modulus-dependent rule that building blocks below a critical modulus of 2.5 MPa can achieve MSA for the used host/guest system. Moreover, this MSA rule applies well to the design of materials for fast underwater adhesion: Soft substrates (0.5 MPa) can achieve underwater adhesion within 10 s with one order of magnitude higher strength than that of rigid substrates (2.5 MPa).

Fabrication of alginate‐P(SBMA‐co‐AAm) hydrogels with ultrastretchability, strain sensitivity, self‐adhesiveness, biocompatibility, and self‐cleaning function for strain sensors

“…Because the density of polyzwitterion reduced, the modulus and toughness of hydrogels increased as the amount of alginate improved, resulting in the number and molecular mobility of superficial interactive moieties diminished. Only a limited portion of groups could reach the reactive distance for adhesion 35 . (This was the reason why double‐network had not been introduced into our hydrogels.)…”

Microphase separation of a quadruple hydrogen bonding supramolecular polymer: effect of the steric hindrance of the ureido-pyrimidone on their viscoelasticity

“…[1][2][3][4][5][6][7][8] As a novel polymeric material, the supramolecular polymer has been studied intensively in the last 20 years and many different kinds of supramolecular self-assembly structures have been synthesized by chemists. [9][10][11][12][13][14][15][16][17][18] The non-covalent interactions that can be reversibly broken and can be under thermodynamic equilibrium will bring additional features compared to normal polymers, potentially leading to new properties, such as improved processing, [19][20][21][22][23] selfhealing behavior [24][25][26][27][28] or stimuli responsiveness [29][30][31][32][33][34] and so on.…”

Parallel and Precise Macroscopic Supramolecular Assembly through Prolonged Marangoni Motion

“…Macroscopic supramolecular assembly (MSA), in which non‐covalently interactive motifs facilitate the assembly of building blocks of sizes exceeding 10 μm, presents a topical challenge in supramolecular chemistry and colloid science. MSA is meaningful for the scalable manufacture of structured materials through self‐assembly, the fabrication of tissue scaffolds, and the study and interpretation of adhesion phenomena . Unlike molecular assembly, in which recognition and binding is reversible and can often obtain kinetic energy from the thermal motion of the components, the realization of MSA faces two major challenges: 1) The large surfaces through which supramolecular motifs interact are usually very rough on the molecular scale, which is unfavorable for realizing efficient interfacial supramolecular interactions; and (2) a driving force is required to achieve collision between and assembly of the macroscopic building blocks, as they are too large to be propelled.…”

“…MSA is meaningful for the scalable manufacture of structured materials through self-assembly, [4][5][6] the fabrication of tissue scaffolds, [7,8] and the study and interpretation of adhesion phenomena. [9][10][11] Unlike molecular assembly,i nw hich recognition and binding is reversible and can often obtain kinetic energy from the thermal motion of the components,t he realization of MSA faces two major challenges:1 )The large surfaces through which supramolecular motifs interact are usually very rough on the molecular scale,w hich is unfavorable for realizing efficient interfacial supramolecular interactions;and (2) adriving force is required to achieve collision between and assembly of the macroscopic building blocks,as they are too large to be propelled. Until now,t he first issue has been addressed by introducing af lexible spacing coating to mediate the surface roughness, [12][13][14] while the second challenge is overcome with external agitation, such as rotation or shaking of the medium in which the macroscopic building blocks assemble,o rm agnetically assisted motion to cause directed diffusion and collision of the building blocks.…”