Self-Organization of Fluids in a Multienzymatic Pump System

The nascent field of microscale flow chemistry focuses on harnessing flowing fluids to optimize chemical reactions in microchambers and establish new routes for chemical synthesis. With enzymes and other catalysts anchored to the surface of microchambers, the catalytic reactions can act as pumps and propel the fluids through the containers. Hence, the flows not only affect the catalytic reactions, but these reactions also affect the flows. Understanding this dynamic interplay is vital to enhancing the accuracy and utility of flow technology. Through experiments and simulation, we design a system of three different enzymes, immobilized in separate gels, on the surface of a microchamber; with the appropriate reactants in the solution, each enzyme-filled gel acts as a pump. The system also exploits a reaction cascade that controls the temporal interactions between two pumps. With three pumps in a triangular arrangement, the spatio-temporal interactions among the chemical reactions become highly coordinated and produce well-defined fluid streams, which transport chemicals and form a fluidic "circuit". The circuit layout and flow direction of each constituent stream can be controlled through the number and placement of the gels and the types of catalysts localized in the gels. These studies provide a new route for forming self-organizing and bifurcating fluids that can yield fundamental insight into nonequilibrium, dynamical systems. Because the flows and fluidic circuits are generated by internal chemical reactions, the fluids can autonomously transport cargo to specific locations in the device. Hence, the findings also provide guidelines to facilitate further automation of microfluidic devices.