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.
Marangoni rotors are smart devices that are capable of self-propulsive motions based on the Marangoni effect, namely interfacial flows caused by a gradient of surface tension. Owing to the features of untethered motions and coupled complexity with fluid, these Marangoni devices are attractive for both theoretical study and applications in biomimicking, cargo delivery, energy conversion, etc. However, the controllability of Marangoni motions dependent on concentration gradients remains to be improved, including the motion lifetime, direction, and trajectories. The challenge lies in the flexible loading and adjustments of surfactant fuels. Herein, we design a multi-engine device in a six-arm shape with multiple fuel positions allowing for motion control and propose a strategy of diluting the surfactant fuel to prolong the motion lifetime. The resulting motion lifetime has been extended from 140 to 360 s by 143% compared with conventional surfactant fuels. The motion trajectories could be facilely adjusted by changing both the fuel number and positions, leading to diverse rotation patterns. By integrating with a coil and a magnet, we obtained a system of mini-generators based on the Marangoni rotor. Compared with the single-engine case, the output of the multi-engine rotor was increased by 2 magnitudes owing to increased kinetic energy. The design of the above Marangoni rotor has addressed the problems of concentration-gradient-driven Marangoni devices and enriched their applications in harvesting energy from the environment.
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