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In the presence of appropriate substrates, surface-anchored enzymes can act as pumps and propel fluid through microchambers. Understanding the dynamic interplay between catalytic reactions and fluid flow is vital to enhancing the accuracy and utility of flow technology. Through a combination of experimental observations and numerical modelling, we show that coupled enzyme pumps can exhibit flow enhancement, flow suppression, and changes in the directionality (reversal) of the fluid motion. The pumps’ ability to regulate the flow path is due to the reaction selectivity of the enzymes; the resultant fluid motion is only triggered by the presence of certain reactants. Hence, the reactants and the sequence in which they are present in the solution, and the layout of the enzyme-attached patches form an “instruction set” that guides the flowing solution to specific sites in the system. Such systems can operate as sensors that indicate concentrations of reactants through measurement of the trajectory along which the flow demonstrates maximal speed. The performed simulations suggest that the solutal buoyancy mechanism causes fluid motion and is responsible for all the observed effects. More broadly, our studies provide a new route for forming self-organizing flow systems that can yield fundamental insight into non-equilibrium, dynamical systems. 

Enzymatic reactions in solution drive the convection of confined fluids throughout the enclosing chambers and thereby couple the processes of reaction and convection. In these systems, the energy released from the chemical reactions generates a force, which propels the fluids’ spontaneous motion. Here, we use theoretical and computational modeling to determine how reaction-convection can be harnessed to tailor and control the dynamic behavior of soft matter immersed in solution. Our model system encompasses an array of surface-anchored, flexible posts in a millimeter-sized, fluid-filled chamber. Selected posts are coated with enzymes, which react with dissolved chemicals to produce buoyancy-driven fluid flows. We show that these chemically generated flows exert a force on both the coated (active) and passive posts and thus produce regular, self-organized patterns. Due to the specificity of enzymatic reactions, the posts display controllable kaleidoscopic behavior where one regular pattern is smoothly morphed into another with the addition of certain reactants. These spatiotemporal patterns also form “fingerprints” that distinctly characterize the system, reflecting the type of enzymes used, placement of the enzyme-coated posts, height of the chamber, and bending modulus of the elastic posts. The results reveal how reaction-convection provides concepts for designing soft matter that readily switches among multiple morphologies. This behavior enables microfluidic devices to be spontaneously reconfigured for specific applications without construction of new chambers and the fabrication of standalone sensors that operate without extraneous power sources. 

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. 

Biological species routinely collaborate for their mutual benefit or compete for available resources, thereby displaying dynamic behavior that is challenging to replicate in synthetic systems. Here we use computational modeling to design microscopic, chemically active sheets and self-propelled particles encompassing the appropriate synergistic interactions to exhibit bioinspired feeding, fleeing, and fighting. This design couples two different mechanisms for chemically generating motion in fluid-filled microchambers: solutal buoyancy and diffusiophoresis. Catalyst-coated sheets, which resemble crabs with four distinct claws, convert reactants in solution into products and thereby create local variations in the density and chemical composition of the fluid. Via the solutal buoyancy mechanism, the density variations generate fluid flows, which modify the shape and motility of the crabs. Concomitantly, the chemical variations propel the motion of the particles via diffusiophoresis, and thus, the crabs’ and particles’ motion becomes highly interconnected. For crabs with restricted lateral mobility, these two mechanisms can be modulated to either drive a crab to catch and appear to feed on all of the particles or enable the particles to flee from this sheet. Moreover, by adjusting the sheet’s size and the catalytic coating, two crabs can compete and fight over the motile, diffusiophoretic particles. Alternatively, the crabs can temporally share resources by shuttling the particles back and forth between themselves. With completely mobile sheets, four crabs can collaborate to perform a function that one alone cannot accomplish. These findings provide design rules for creating chemically driven soft robotic sheets that significantly expand the functionality of microfluidic devices.