Active matter consumes local fuels to self-propel. When confined in a closed circular boundary, they can self-organize into a circulatory flow. Such coherence originates from the interactions between the active matter and boundaries, and boundary conditions play an important role on self-organization of active fluid. Herein, we probed how fluid boundaries influenced the self-organization of active fluid. The fluid boundaries were created by confining the active fluid in a compressed water-in-oil droplet. Due to surface tension, the droplet shaped into a cylinder-like geometry. Since water and oil were both fluids, their interface was fluid. We systematically probed how droplet shapes and the amount of oil surrounding the droplet influenced the development of circulation. We found that the formation of circulatory flows depended on the thickness of the oil layer surrounding the droplet, implying that the fluid dynamics between the active fluid within the droplet and the oil outside the droplet were coupled. We used a 3D COMSOL-based simulation successfully reproduced such oil-layer dependence. Finally, we developed two milli-fluidic devices to deform the droplet and alter the oil layer thickness manually to trigger and suppress the intra-droplet circulatory flow in real time.
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Using Curved Fluid Boundaries to Confine Active Nematic Flows
Actively driven, bundled microtubule networks, powered by molecular motors have become a useful framework in which to study the dynamics of energy-driven defects, but achieving control of defect motions is still a challenging problem. In this paper, we present a method to confine active nematic fluid using wetting to curve a layer of oil over circular pillars. This geometry, in which submersed pillars impinge on an oil-water interface, creates a two-tier continuous active layer in which the material is confined above, and surrounds the pillars. Active flows above the pillars are influenced by the circular geometry and exhibit dynamics similar to those observed for active material confined by hard boundaries, e.g., inside circular wells. The thin oil layer beneath the active material is even thinner in the region above the pillars than outside their boundary, consequently producing an area of higher effective friction. Within the pillar region, active length scales and velocities are decreased, while defect densities increase relative to outside the pillar boundary. This new way to confine active flows opens further opportunities to control and organize topological defects and study their behavior in active systems.
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- NSF-PAR ID:
- 10359509
- Date Published:
- Journal Name:
- Frontiers in Physics
- Volume:
- 10
- ISSN:
- 2296-424X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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We study how confinement transforms the chaotic dynamics of bulk microtubule-based active nematics into regular spatiotemporal patterns. For weak confinements in disks, multiple continuously nucleating and annihilating topological defects self-organize into persistent circular flows of either handedness. Increasing confinement strength leads to the emergence of distinct dynamics, in which the slow periodic nucleation of topological defects at the boundary is superimposed onto a fast procession of a pair of defects. A defect pair migrates toward the confinement core over multiple rotation cycles, while the associated nematic director field evolves from a distinct double spiral toward a nearly circularly symmetric configuration. The collapse of the defect orbits is punctuated by another boundary-localized nucleation event, that sets up long-term doubly periodic dynamics. Comparing experimental data to a theoretical model of an active nematic reveals that theory captures the fast procession of a pair of
defects, but not the slow spiral transformation nor the periodic nucleation of defect pairs. Theory also fails to predict the emergence of circular flows in the weak confinement regime. The developed confinement methods are generalized to more complex geometries, providing a robust microfluidic platform for rationally engineering 2D autonomous flows. -
Fluid dynamics of conventional passive fluid are known to be affected by boundary condition. For example, flow rates in a pipe depend on slipperiness of pipe surface. Similarly, active fluid, which consumes fuels locally to flow spontaneously, was reported to self-flow along a meter-long tubing with the flow rate depending on tubing geometry. However, how boundary condition influences fluid dynamics in an active fluid system remains poorly understood. Here, we investigated how a fluid boundary influenced self-organization of confined active fluid by establishing a 3D COMSOL-based nemato-hydrodynamic simulation platform where active fluid was confined in a compressed cylindrical water-in-oil droplet. Since the droplet interface was fluid, the fluid dynamics within and outside the droplet were coupled. Our simulation demonstrated that flow behaviors of intra-droplet active fluid were influenced by the amount of oil that surrounded the droplet: Without altering the droplet geometry, expanding the volume of oil could induce a circulatory flow within the droplet, which resembled our experimental observation. Our work suggested the feasibility of controlling the fluid dynamics of a confined active fluid system across a fluid interface.more » « less
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Conventional lithium-ion batteries are unable to meet the increasing demands for high-energy storage systems, because of their limited theoretical capacity. 1 In recent years, intensive attention has been paid to enhancing battery energy storage capability to satisfy the increasing energy demand in modern society and reduce the average energy capacity cost. Among the candidates for next generation high energy storage systems, the lithium sulfur battery is especially attractive because of its high theoretical specific energy (around 2600 W h kg-1) and potential cost reduction. In addition, sulfur is a cost effective and environmentally friendly material due to its abundance and low-toxicity. 2 Despite all of these advantages, the practical application of lithium sulfur batteries to date has been hindered by a series of obstacles, including low active material loading, poor cycle life, and sluggish sulfur conversion kinetics. 3 Achieving high mass loading cathode in the traditional 2D planar thick electrode has been challenged. The high distorsion of the traditional planar thick electrodes for ion/electron transfer leads to the limited utilization of active materials and high resistance, which eventually results in restricted energy density and accelerated electrode failure. 4 Furthermore, of the electrolyte to pores in the cathode and utilization ratio of active materials. Catalysts such as MnO 2 and Co dopants were employed to accelerate the sulfur conversion reaction during the charge and discharge process. 5 However, catalysts based on transition metals suffer from poor electronic conductivity. Other catalysts such as transition metal dopants are also limited due to the increased process complexities. . In addition, the severe shuttle effects in Li-S batteries may lead to fast failures of the battery. Constructing a protection layer on the separator for limiting the transmission of soluble polysulfides is considered an effective way to eliminate the shuttle phenomenon. However, the soluble sulfides still can largely dissolve around the cathode side causing the sluggish reaction condition for sulfur conversion. 5 To mitigate the issues above, herein we demonstrate a novel sulfur electrode design strategy enabled by additive manufacturing and oxidative vapor deposition (oCVD). Specifically, the electrode is strategically designed into a hierarchal hollow structure via stereolithography technique to increase sulfur usage. The active material concentration loaded to the battery cathode is controlled precisely during 3D printing by adjusting the number of printed layers. Owing to its freedom in geometry and structure, the suggested design is expected to improve the Li ions and electron transport rate considerably, and hence, the battery power density. The printed cathode is sintered at 700 °C at N 2 atmosphere to achieve carbonization of the cathode during which intrinsic carbon defects (e.g., pentagon carbon) as catalytic defect sites are in-situ generated on the cathode. The intrinsic carbon defects equipped with adequate electronic conductivity. The sintered 3D cathode is then transferred to the oCVD chamber for depositing a thin PEDOT layer as a protection layer to restrict dissolutions of sulfur compounds in the cathode. Density functional theory calculation reveals the electronic state variance between the structures with and without defects, the structure with defects demonstrates the higher kinetic condition for sulfur conversion. To further identify the favorable reaction dynamic process, the in-situ XRD is used to characterize the transformation between soluble and insoluble polysulfides, which is the main barrier in the charge and discharge process of Li-S batteries. The results show the oCVD coated 3D printed sulfur cathode exhibits a much higher kinetic process for sulfur conversion, which benefits from the highly tailored hierarchal hollow structure and the defects engineering on the cathode. Further, the oCVD coated 3D printed sulfur cathode also demonstrates higher stability during long cycling enabled by the oCVD PEDOT protection layer, which is verified by an absorption energy calculation of polysulfides at PEDOT. Such modeling and analysis help to elucidate the fundamental mechanisms that govern cathode performance and degradation in Li-S batteries. The current study also provides design strategies for the sulfur cathode as well as selection approaches to novel battery systems. References: Bhargav, A., (2020). Lithium-Sulfur Batteries: Attaining the Critical Metrics. Joule 4 , 285-291. Chung, S.-H., (2018). Progress on the Critical Parameters for Lithium–Sulfur Batteries to be Practically Viable. Advanced Functional Materials 28 , 1801188. Peng, H.-J.,(2017). Review on High-Loading and High-Energy Lithium–Sulfur Batteries. Advanced Energy Materials 7 , 1700260. Chu, T., (2021). 3D printing‐enabled advanced electrode architecture design. Carbon Energy 3 , 424-439. Shi, Z., (2021). Defect Engineering for Expediting Li–S Chemistry: Strategies, Mechanisms, and Perspectives. Advanced Energy Materials 11 . Figure 1more » « less
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Surfaces with micrometer-scale pillars have shown great potential in delaying the boiling crisis and enhancing the critical heat flux (CHF). However, physical mechanisms enabling this enhancement remain unclear. This knowledge gap is due to a lack of diagnostics that allow elucidating how micro-pillars affect thermal transport phenomena on the engineered surface. In this study, for the first time, we are able to measure time-dependent temperature and heat flux distributions on a boiling surface with engineered micro-pillars using infrared thermometry. Using these data, we reveal the presence of an intra-pillar liquid layer, created by the nucleation of bubbles and partially refilled by capillary effects. However, contrarily to conventional wisdom, the energy removed by the evaporation of this liquid cannot explain the observed CHF enhancement. Yet, predicting its dry out is the key to delaying the boiling crisis. We achieve this goal using simple analytic models and demonstrate that this process is driven by conduction effects in the boiling substrates and, importantly, in the intra-pillar liquid layer itself. Importantly, these effects also control the wicking flow rate and its penetration length. The boiling crisis occurs when, by coalescing, the size of the intra-pillar liquid layer becomes too large for the wicking flow to reach its innermost region. Our study reveals and quantifies unidentified physical aspects, key to the performance optimization of boiling surfaces for cooling applications.
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.3389/fphy.2022.880941
