NSF-DFG Confine: Sculpting Confined Fluids for Transport using Self-Organization and Information Transfer

我们将创建“活跃的”、自组织的流体系统，这些系统进行仿生能量转换，将反应产生的能量转化为机械力，从而触发受限流体的自发运动。为了实现这种丰富的动态行为，我们将酶固定在充满流体的微室中的3D打印贴片阵列上。合适的反应物激活催化反应，释放化学能来“泵”和“塑造”流体流动，调节流体-后相互作用，驱动自组织，以及在整个系统中传播化学信号。我们还将引入上游信号处理计算层来构建酶模式，使用贴片选择性生长来调节贴片之间的距离，并引入选择性释放化学物质的移动微载体。这将使我们能够进一步协调化学-机械相互作用，并控制流体流动的时空特征。自发运动和信号传递赋予了这些流体平台在材料系统中实现仿生功能的可行机制。在我们的协作工作计划中，WP1专注于微流体系统的多材料3D微打印，WP2针对表面和可变形柱子上由酶启用的主动泵送机制，WP3在柱子阵列上实施叠加的自组织信号构图过程，该过程产生于DNA链置换反应网络，然后可以耦合到酶的主动泵送和流体流动的雕刻。我们的方法利用了充液腔内丰富的动力学，其中包含催化剂涂层的贴片、贴片和化学诱导的运动和自组织。通过联合研究，我们将明确分子尺度化学对受限流体微尺度流动的基本影响，反之，微观流动对微腔内化学动力学的影响。很少有单独的小组拥有专门知识和仪器来探索受限流体中的化学-机械转导与化学驱动的自组织相结合的影响。这种合作使我们能够：以所需的规模制造系统(Blasco，Heidelberg)，对系统进行化学定制以进行系统研究(Sen，Penn State和Walther，Mainz)，并开发预测模型(Balazs，匹兹堡)。每个基团都需要与其他基团协同作用，才能在活性微流控、流动化学和理论建模方面取得显著进展。展望未来，响应特定信号的流体流动和传输的(自我)调节是实现下一代智能微纳器件的关键，以实现高效和自主的化学合成、传感和输送模式。由于流动和反馈是非平衡过程，这些研究也将为探索结构、动力学和非平衡行为之间的关系提供新的平台。

We will create “active”, self-organizing fluidic systems that undergo biomimetic energy transduction, converting energy from reactions into mechanical forces, which trigger the spontaneous motion of the confined fluid. To realize this rich dynamic behavior, we will anchor enzymes to 3D-printed patch arrays in fluid-filled microchambers. Appropriate reactants activate the catalytic reactions, which release the chemical energy to “pump” and “sculpt” the fluid flow, modulate fluid-post interactions, drive self-organization, as well as propagate chemical signals throughout the system. We will also introduce upstream signal-processing computational layers to structure enzyme patterns, use patch-selective growth to modulate inter-patch distances, and introduce mobile microcarriers that selectively release chemicals. This will allow us to further orchestrate chemo-mechanical interactions and control the spatiotemporal features of the fluid flow. The spontaneous motion and signaling endow these fluidic platforms with viable mechanisms for achieving life-like functionality in materials systems. In our collaborative work plan, WP1 concentrates on multi-material 3D microprinting of the microfluidic systems, WP2 targets active pumping mechanisms enabled by enzymes on surfaces and deformable posts, and WP3 implements a superimposed self-organizing signal patterning process at the post arrays, arising from DNA strand displacement reaction networks, which can then be coupled to active pumping by enzymes and sculpting of fluid flows. Our approach exploits the rich dynamics within fluid-filled chambers containing catalyst-coated patches, posts, and chemically induced motion and self-organization. Through the combined studies, we will pinpoint the fundamental effects of molecular-scale chemistry on microscale flow of confined fluids, and, conversely, the effect of microscopic flow on chemical kinetics in microchambers. Few individual groups have the expertise and instrumentation to probe the effects of chemo-mechanical transduction in confined fluids in combination with chemically-driven self-organization. This collaboration allows us to: fabricate systems at the desired size scales (Blasco, Heidelberg), chemically tailor the systems to perform systematic studies (Sen, Penn State and Walther, Mainz) and develop predictive models (Balazs, Pittsburgh). Each group requires synergistic interactions with the others to make dramatic advances in active microfluidics, flow chemistry, and theoretical modeling. Looking to the future, the (self-)regulation of fluid flow and transport across length scales in response to specific signals is critical for realizing the next generation smart micro- & nano-scale devices for efficient, and autonomous modes of chemical synthesis, sensing, and delivery. Since flow and feedback are non-equilibrium processes, these studies will also provide new platforms for probing relationships among structure, dynamics, and non-equilibrium behavior.