Enzyme Catalysis Causes Fluid Flow, Motility, and Directional Transport on Supported Lipid Bilayers.

The dynamic interplay between the composition of lipid membranes and the behavior of membrane-bound enzymes is critical to the understanding of cellular function and viability, and the design of membrane-based biosensing platforms. While there is a significant body of knowledge about how lipid composition and dynamics affect membrane-bound enzymes, little is known about how enzyme catalysis influences the motility and lateral transport on lipid membranes. Using enzyme-attached lipids in supported bilayers (SLBs), we provide direct evidence of catalysis-induced fluid flow that underlies the observed motility on SLBs. Additionally, by using active enzyme patches, we demonstrate the directional transport of tracer particles on SLBs. As expected, enhancing the membrane viscosity by incorporating cholesterol into the bilayer suppresses the overall movement. These are the first steps in understanding diffusion and transport on lipid membranes due to active, out-of-equilibrium processes that are the hallmark of living systems. In general, our study demonstrates how active enzymes can be used to control diffusion and transport in confined 2-D environments.

Self-Propelling Macroscale Sheets Powered by Enzyme Pumps.

Nanoscale enzymes anchored to surfaces act as chemical pumps by converting chemical energy released from enzymatic reactions into spontaneous fluid flow that propels entrained nano- and microparticles. Enzymatic pumps are biocompatible, highly selective, and display unique substrate specificity. Utilizing these pumps to trigger self-propelled motion on the macroscale has, however, constituted a significant challenge and thus prevented their adaptation in macroscopic fluidic devices and soft robotics. Using experiments and simulations, we herein show that enzymatic pumps can drive centimeter-scale polymer sheets along directed linear paths and rotational trajectories. In these studies, the sheets are confined to the air/water interface. With the addition of appropriate substrate, the asymmetric enzymatic coating on the sheets induces chemically driven, buoyancy flows that controllably propel the sheet's motion on the air/water interface. The directionality and speed of the motion can be tailored by changing the pattern of the enzymatic coating, type of enzyme, and nature and concentration of the substrate. This work highlights the utility of biocompatible enzymes for generating motion in macroscale fluidic devices and robotics and indicates their potential utility for in vivo applications.

Dynamic Oscillation and Motion of Oil-in-Water Emulsion Droplets.

The interplay of interfacial tensions on droplets results in a range of self-powered motions that mimic those of living systems and serve as a tunable model to understand their complex non-equilibrium behavior. Spontaneous shape deformations and oscillations are crucial features observed in nature but difficult to incorporate in synthetic artificial systems. Here, we report sessile oil-in-water emulsions that exhibit rapid oscillating behavior. The oscillations depend on the nature and concentration of the surfactant, the chemical composition of the oil, and the wettability of the solid substrate. The rapid changes in the contact angle per oscillation are observed using side-view optical microscopy. We propose that the changes in the interfacial tension of the oil droplets is due to the partitioning of the surfactant into the oil phase and the movement of self-emulsified oil out of the parent droplets giving rise to the rhythmic variation in droplet contact-line. The ability to control and understand droplet oscillation can help model similar oscillations in out-of-equilibrium systems in nature and reproduce biomimetic behavior in artificial systems for various applications, such as microfluidic lab-on-a-chip and adaptive materials.