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Advanced synthetic materials are needed to produce nano‐ and mesoscale structures that function autonomously, catalyze reactions, and convert chemical energy into motion. This paper describes supracolloidal fiber‐like structures that are composed of self‐adhering, or “sticky,” oil‐in‐water emulsion droplets. Polymer zwitterion surfactants serve as the key interfacial components of these materials, enabling multiple functions simultaneously, including acting as droplet‐stabilizing surfactants, interdroplet adhesives, and building blocks of the fibers. This fiber motion, a surprising additional feature of these supracolloidal structures, is observed at the air–water interface and hinged on the chemistry of the polymer surfactant. The origin of this motion is hypothesized to involve transport of polymer from the oil–water interface to the air–water interface, which generates a Marangoni (interfacial) stress. Harnessing this fiber motion with functional polymer surfactants, and selection of the oil phase, produced worm‐like objects capable of rotation, oscillation, and/or response to external fields. Overall, these supracolloidal fibers fill a design gap between self‐propelled nano/microscale particles and macroscale motors, and have the potential to serve as new components of soft, responsive materials structures.

 

Oil‐in‐water droplets stabilized with polymer zwitterions (PZWs) exhibit salt‐responsive aggregation–disaggregation behavior. Here, a method to shape these droplets is described, starting from their aggregated state, into supracolloidal fibers by simply extruding them into aqueous media. The effect of salt concentration, in both the initial emulsion and the aqueous medium, on the ability of the emulsions to form fibers is examined. After fiber formation, a transition from well‐defined macroscopic structures to noninteracting droplet dispersions can be triggered, simply by increasing the salt concentration of the aqueous environment. The interdroplet energy of adhesion and emulsion rheology correlate qualitatively with salt concentration and thus impact the ability of the emulsions to be shaped by extrusion. The interdroplet adhesion is dependent on both salt concentration and polymer composition, which allows tailoring of conditions to trigger fiber disaggregation. Finally, fibers with variable compositions along their length are prepared by sequential loading and extrusion of emulsions containing oil phases of differing densities.

 

Two-dimensional responsive materials that change shape into complex three-dimensional structures are valuable for creating systems ranging from wearable electronics to soft robotics. Typically, the final 3D structure is unique and predetermined through the materials’ processing. Here, we use theory and simulation to devise a distinctive approach for driving shape changes of 2D elastic sheets in fluid-filled microchambers. The sheets are coated with catalyst to generate controllable fluid flows, which transform the sheets into complex 3D shapes. A given shape can be achieved by patterning the arrangement of the catalytic domains on the sheet and introducing the appropriate reactant to initiate a specific catalytic reaction. Moreover, a single sheet that encompasses multiple catalytic domains can be transformed into a variety of 3D shapes through the addition of one or more reactants. Materials systems that morph on-demand into a variety of distinct structures can simplify manufacturing processes and broaden the utility of soft materials. 

Marangoni flow is the motion induced by a surface tension gradient along a fluid–fluid interface. In this study, we report a Marangoni flow generated when a bath of surfactant contacts a pre-wetted film of deionized water on a vertical substrate. The thickness profile of the pre-wetted film is set by gravitational drainage and so varies with the drainage time. The surface tension is lower in the bath due to the surfactant, and thus a liquid film climbs upwards along the vertical substrate due to the surface tension difference. Particle tracking velocimetry is performed to measure the dynamics in the film, where the mean fluid velocity reverses direction as the draining film encounters the front of the climbing film. The effect of the surfactant concentration and the pre-wetted film thickness on the film climbing is then studied. High-speed interferometry is used to measure the front position of the climbing film and the film thickness profile. As a result, higher surfactant concentration induces a faster and thicker climbing film. Also, for high surfactant concentrations, where Marangoni driving dominates, increasing the film thickness increases the rise speed of the climbing front, since viscous resistance is less important. In contrast, for low surfactant concentrations, where Marangoni driving balances gravitational drainage, increasing the film thickness decreases the rise speed of the climbing front while enhancing gravitational drainage. We rationalize these observations by utilizing a dimensionless parameter that compares the magnitudes of the Marangoni stress and gravitational drainage. A model is established to analyse the climbing front, either in the Marangoni-driving-dominated region or in the Marangoni-balanced drainage region. Our work highlights the effects of the gravitational drainage on the Marangoni flow, both by setting the thickness of a pre-wetted film and by resisting the film climbing.