Self-Organization of Fluids in a Multienzymatic Pump System
Self-Organization of Fluids in a Multienzymatic Pump System
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DOI：
10.1021/acs.langmuir.8b03607
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发表时间：
2019-03-12
期刊：
影响因子：
3.9
通讯作者：
Sen, Ayusman
中科院分区：
文献类型：
--
作者：
Maiti, Subhabrata;Shklyaev, Oleg E.;Sen, Ayusman
微尺度流动化学的新兴领域专注于利用流动的流体来优化微室中的化学反应，并建立新的化学合成路线。由于酶和其他催化剂固定在微室的表面，催化反应可以充当泵并推动流体通过容器。因此，流动不仅影响催化反应，而且这些反应也影响流动。了解这种动态相互作用对于提高流量技术的准确性和实用性至关重要。通过实验和模拟，我们设计了一个系统的三种不同的酶，固定在单独的凝胶，在一个微室的表面上;与适当的反应物在溶液中，每个酶填充的凝胶作为一个泵。该系统还利用了控制两个泵之间的时间相互作用的反应级联。三个泵呈三角形排列，化学反应之间的时空相互作用变得高度协调，并产生明确的流体流，这些流体流输送化学品并形成流体“回路”。每个组成流的回路布局和流动方向可以通过凝胶的数量和放置以及凝胶中定位的催化剂的类型来控制。这些研究为形成自组织和分叉流体提供了一条新的途径，这些流体可以产生对非平衡动力系统的基本见解。由于流动和流体回路是由内部化学反应产生的，因此流体可以自主地将货物运输到设备中的特定位置。因此，这些发现也为促进微流体设备的进一步自动化提供了指导。
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.