Moradi Moslem, Shklyaev Oleg E, Balazs Anna C
Department of Chemical Engineering, University of Pittsburgh, Pittsburgh, Pennsylvania 15261, United States.
Langmuir. 2025 Mar 18;41(10):6633-6643. doi: 10.1021/acs.langmuir.4c04567. Epub 2025 Mar 4.
Solutal buoyancy forces in solution arise from density gradients, which occur when the reactants and products of a chemical reaction occupy different volumes in the fluid. These forces drive fluids to spontaneously perform self-directed mechanical work such as shaping and organizing flexible objects in fluid-filled microchambers. Here, we use theory and simulation to show that chemical reactions are not necessary to generate useful solutal buoyancy forces; it is sufficient to just add reactants to aqueous solutions that have a different mass-to-volume ratio than water to drive such spontaneous mechanical action. To demonstrate this behavior, we model arrays of tethered, nonreactive posts in a fluid-filled chamber. Relatively dense chemicals released from the chamber's side walls diffuse into the solution and generate buoyancy-driven flows, which spontaneously trigger the posts to undergo collective dynamics. The posts' dynamics can be controllably programmed by staging the sequence of chemical release from the different walls. With chemically active posts within the array, turning on and off the influx of chemicals from the side walls leads to propagating waves that drive the posts to exhibit biomimetic coordinated motion. The introduction of cascade reactions dynamically shifts the direction of wave propagation. Our findings show how diffusion-convection and diffusion-reaction-convection processes can be used to regulate nonequilibrium spatiotemporal behavior in fluidic systems. This level of control is vital for creating portable microfluidic devices that operate without external power sources and thus function in remote or resource-poor locations.
溶液中的溶质浮力源于密度梯度,当化学反应的反应物和产物在流体中占据不同体积时就会出现这种情况。这些力促使流体自发地进行自我导向的机械功,例如在充满流体的微腔中塑造和组织柔性物体。在此,我们运用理论和模拟表明,产生有用的溶质浮力并不一定需要化学反应;只需向质量体积比与水不同的水溶液中添加反应物,就能驱动这种自发的机械作用。为证明这种行为,我们对充满流体的腔室内一系列系留的非反应性柱体进行建模。从腔室侧壁释放的相对高密度化学物质扩散到溶液中,产生浮力驱动的流动,这会自发地促使柱体发生集体动力学行为。通过安排从不同壁面释放化学物质的顺序,可以可控地对柱体的动力学行为进行编程。在阵列中有化学活性柱体时,开启和关闭来自侧壁的化学物质流入会导致传播波,从而驱动柱体展现出仿生协调运动。级联反应的引入会动态改变波的传播方向。我们的研究结果表明了扩散 - 对流以及扩散 - 反应 - 对流过程如何用于调节流体系统中的非平衡时空行为。这种控制水平对于制造无需外部电源就能运行、因而可在偏远或资源匮乏地区发挥作用的便携式微流控设备至关重要。