Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States.
College of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan 430200, China.
ACS Appl Mater Interfaces. 2024 Aug 28;16(34):45660-45670. doi: 10.1021/acsami.4c07865. Epub 2024 Aug 13.
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 modeling, 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 a maximal speed. The performed simulations suggest that the solutal buoyancy mechanism causes fluid motion and is responsible for all of the observed effects. More broadly, our studies provide a new route for forming self-organizing flow systems that can yield fundamental insight into nonequilibrium, dynamical systems.
在适当的底物存在下,表面锚定的酶可以作为泵,推动流体通过微腔。了解催化反应和流体流动之间的动态相互作用对于提高流动技术的准确性和实用性至关重要。通过实验观察和数值模拟的结合,我们表明耦合酶泵可以表现出增强的流动、抑制的流动以及流动方向(反转)的变化。泵调节流动路径的能力归因于酶的反应选择性;只有存在某些反应物时,才会引发流体运动。因此,反应物及其在溶液中的存在顺序以及附着在酶上的补丁的布局形成了一个“指令集”,指导流动的溶液流向系统中的特定位置。这样的系统可以作为传感器,通过测量流动显示最大速度的轨迹来指示反应物的浓度。所进行的模拟表明,溶质浮力机制引起了流体运动,并负责所有观察到的效应。更广泛地说,我们的研究为形成自组织流动系统提供了一条新途径,可以深入了解非平衡、动力学系统。