Precise macroscopic supramolecular assembly of photopatterned hydrogels

Xue, Yuan; Yu, Kai; Wang, Xuebin; Xiang, Yanxing; Pang, Shihao; Zhu, Linyong

doi:10.1039/d1cc03428f

Cited by 12 publications

(10 citation statements)

References 32 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…As the assembly scales up with many pathways and meta-stable structures, the challenge to selectively obtain designated structures is increasing together with the problem of low assembly precision 14 . Generally, two strategies have been proposed to confine the assembly results: (1) subtle designs of molecules or nanoparticles to exclude meta-stable assemblies 15 , 16 , which however requires tedious and difficult fabrication of microscale building blocks; (2) directly using μm-to-mm sized components to shorten the length gap from building blocks to final structures and to reduce the assembly possibilities, which is termed as macroscopic supramolecular assembly (MSA) 2 , 3 , 17 – 24 . Owing to the feasibility of fabrication at this length scale, it is facile to design MSA building blocks and to adjust assembly conditions 25 , 26 .…”

Section: Introductionmentioning

confidence: 99%

Self-sorting in macroscopic supramolecular self-assembly via additive effects of capillary and magnetic forces

et al. 2022

View full text Add to dashboard Cite

Supramolecular self-assembly of μm-to-mm sized components is essential to construct complex supramolecular systems. However, the selective assembly to form designated structures at this length scale is challenging because the short-ranged molecular recognition could hardly direct the assembly of macroscopic components. Here we demonstrate a self-sorting mechanism to automatically identify the surface chemistry of μm-to-mm components (A: polycations; B: polyanions) based on the A-B attraction and the A-A repulsion, which is realized by the additivity and the competence between long-ranged magnetic/capillary forces, respectively. Mechanistic studies of the correlation between the magnetic/capillary forces and the interactive distance have revealed the energy landscape of each assembly pattern to support the self-sorting results. By applying this mechanism, the assembly yield of ABA trimers has been increased from 30%~40% under conventional conditions to 100% with self-sorting. Moreover, we have demonstrated rapid and spontaneous self-assembly of advanced chain-like structures with alternate surface chemistry.

show abstract

Section: Introductionmentioning

confidence: 99%

Self-sorting in macroscopic supramolecular self-assembly via additive effects of capillary and magnetic forces

et al. 2022

View full text Add to dashboard Cite

show abstract

“…The macroscopic supramolecular assembly (MSA) refers to a self-assembly of micrometer-to-millimeter building blocks based on multivalent non-covalent interactions − and has developed rapidly toward the goal of “self-assembly at all scales” by bridging the molecular assembly behaviors to the macroscopic materials. Owing to the characteristics of interfacial interactions between micrometer-to-millimeter surfaces, studies of the MSA mechanism are used to understand diverse non-covalent interfacial phenomena such as bio-/wet adhesion, , self-healing. − Meanwhile, MSA has been developed as a facile modular fabrication strategy to prepare heterogeneous structures, bio-scaffolds, , actuators, and information storage materials. − To extend the applicable scenarios of MSA, much progress has been achieved on enriching supramolecular interactions (molecular recognition, , hydrogen bonding, electrostatic interactions, DNA hybridization, , and so on), extending building block materials (gels, ,,− , elastomers, ,, quartz, and metal) that could realize MSA, and revealing the assembly mechanism. ,,, These studies have demonstrated that MSA is not simply an amplification of the building block size from the molecular self-assembly but requires additional factors (e.g., external energy and fast interfacial adhesion) to facilitate the binding of two macroscopic surfaces.…”

Section: Introductionmentioning

confidence: 99%

Robust Electrostatically Interactive Hydrogel Coatings for Macroscopic Supramolecular Assembly via Rapid Wet Adhesion

Liu

Zhao

et al. 2023

ACS Appl. Mater. Interfaces

View full text Add to dashboard Cite

A macroscopic supramolecular assembly (MSA) refers to non-covalent interactions between building blocks over a micrometer scale, which provides insights into bio-/wet adhesion, self-healing, and so on and new fabrication strategies to heterogeneous structures and bio-scaffolds. The key to realize the MSA of rigid materials is pre-modifying a compliant coating known as a "flexible spacing coating" beneath the interactive moieties. However, available coatings are limited to polyelectrolyte multilayers with shortcomings of tedious fabrication, weak adhesion to substrates, susceptibility to external reagents, and so on. Here, we develop a facile method to induce a new "flexible spacing coating" of a poly(2-hydroxyethyl methacrylate) (PHEMA) hydrogel with electrostatic interactions to achieve MSA of diverse rigid materials (quartz, metal, rubber, and plastics). Selective self-assembly of positive−negative charged surfaces is observed by the naked eye under 3 min of shaking in water, providing strategies to rapid wet adhesion. The interfacial binding force between positive−negative interacted surfaces is 1018.1 ± 299.2 N/m 2 , which is over two magnitudes larger than that of control groups, that is, positive−positive (24.4 ± 10.0 N/m 2 ) and negative−negative (67.5 ± 16.7 N/m 2 ) interacted surfaces. In situ force measurements and control experiments of identically charged building blocks have strongly supported the improved binding strength and chemical selectivity between interactive building blocks. The coating is advantageous with a simple fabrication, strong adhesion to materials, robust solvent tolerance to assembly solutions, and feasibility of photo-patterning. We envision that the above strategy would broaden the material choices of flexible spacing coatings for efficient MSA and new methods for rapid interfacial adhesion.

show abstract

“…[10] In artificial self-assembly, loading appropriate energy into each building component to guide the assembly behaviors with good control remains challenging. [11][12][13][14] Especially, selfassembly of μm-to-mm building components, termed as macroscopic supramolecular assembly (MSA), [15][16][17][18][19][20][21][22][23][24][25][26][27] still lacks appropriate driving forces for the collision and interaction of components [28][29][30] because molecular thermal motions that drive molecular self-assembly are not sufficient at this length scale. To propel μm-to-mm components, external mechanical energy such as vigorous shaking or rotation, is used to trigger self-assembly, whose random feature inevitably induces mis-matched structures with low ordering.…”

Section: Introductionmentioning

confidence: 99%

A Hydrolyzable Supra‐amphiphile as a Marangoni Self‐Propulsion Fuel for Efficient Macroscopic Supramolecular Self‐Assembly

Zhu

Zhang

et al. 2023

Angewandte Chemie

View full text Add to dashboard Cite

Self‐assembly of μm‐to‐mm components is important for achieving all‐scale ordering with requirements of extra energy for motion and interaction of components. Marangoni flows caused by surfactants on water provide appropriate energy but have limited lifetimes because of the inevitable interfacial aggregation and difficult decomposition of aggregated covalent surfactants that inactivate Marangoni effects. Here we have synthesized a supra‐amphiphile Marangoni “fuel”—sodium‐4‐(benzylideneamino) benzenesulfonate (SBBS)—that can be hydrolyzed in a timely manner to a species without surface activity to extend the motion time by 10‐fold. The motion was optimized at pH=2 by a fine equilibrium between the releasing and removal of interfacial SBBS, leading to the self‐assembly of millimeter‐scaled ordered dimers. The underlying mechanism was interpreted by motion analyses and simulation. This strategy provides an active solution to self‐assembly at the μm‐to‐mm scale, as well as interactive ideas between miniaturized chemical robots.

show abstract

Precise macroscopic supramolecular assembly of photopatterned hydrogels

Abstract: Here we demonstrate that precise macroscopic supramolecular assembly (MSA) can be achieved by surface photopatterning strategy. The electrostatic interaction of the photopatterned polyelectrolytes drives hydrogel cuboids to form stable MSA...

Cited by 12 publications

References 32 publications

Self-sorting in macroscopic supramolecular self-assembly via additive effects of capillary and magnetic forces

Self-sorting in macroscopic supramolecular self-assembly via additive effects of capillary and magnetic forces

Robust Electrostatically Interactive Hydrogel Coatings for Macroscopic Supramolecular Assembly via Rapid Wet Adhesion

A Hydrolyzable Supra‐amphiphile as a Marangoni Self‐Propulsion Fuel for Efficient Macroscopic Supramolecular Self‐Assembly

Contact Info

Product

Resources

About