Patterning Wettability for Open-Surface Fluidic Manipulation: Fundamentals and Applications.

Effective manipulation of liquids on open surfaces without external energy input is indispensable for the advancement of point-of-care diagnostic devices. Open-surface microfluidics has the potential to benefit health care, especially in the developing world. This review highlights the prospects for harnessing capillary forces on surface-microfluidic platforms, chiefly by inducing smooth gradients or sharp steps of wettability on substrates, to elicit passive liquid transport and higher-order fluidic manipulations without off-the-chip energy sources. A broad spectrum of the recent progress in the emerging field of passive surface microfluidics is highlighted, and its promise for developing facile, low-cost, easy-to-operate microfluidic devices is discussed in light of recent applications, not only in the domain of biomedical microfluidics but also in the general areas of energy and water conservation.

Jet Impact on Superhydrophobic Metal Mesh.

Liquid-jet impact on porous, relatively thin solids has a variety of applications in heat transfer, filtration, liquid-fuel atomization, incontinence products, and solid-substrate erosion, among others. Many prior studies focused on liquid-jet impact on impermeable substrates, and some have investigated the hydraulic jump phenomenon. In the present work, the liquid jet strikes a superhydrophobic, permeable, metal mesh orthogonally, and the radial spreading and throughflow of the liquid are characterized. The prebreakthrough hydraulic jump, the breakthrough velocity, and the postbreakthrough spatial distributions of the liquid are investigated by varying the liquid properties (density, surface tension, and viscosity) and the openness of the metal mesh. The hydraulic jump radius in the prebreakthrough regime increases with jet velocity and is independent of the liquid properties and mesh geometry (pore size, wire diameter and pitch). The breakthrough velocity increases with surface tension of the liquid and decreases with the mesh opening diameter and liquid viscosity. A simple analytical model predicts the jet breakthrough velocity; its predictions are in accordance with the experimental observations. In the postbreakthrough regime, as the jet velocity increases, the liquid flow rate penetrating the mesh shows an initially steep increase, followed by a plateau, which is attributed to a Cassie-Baxter-to-Wenzel transition at the impact area of the mesh.

Lateral Spreading of Gas Bubbles on Submerged Wettability-Confined Tracks.

Spreading of liquid droplets on wettability-confined paths has attracted considerable attention in the past decade. On the other hand, the inverse scenario of a gas bubble spreading on a submerged, wettability-confined track has rarely been studied. In the present work, an experimental investigation of the spreading of millimetric gas bubbles on horizontally submerged, textured, wettability-confined tracks is carried out. The width of the track is kept fixed along its entire length, and the spreading behavior of a gas bubble, dispensed at one end of the track, is studied. The effects of varying track width, bubble diameter, and ambient liquid are investigated. Post-contact, the gas bubble spreads along the track at a linear rate with time, while remaining pinned at its back end; the recorded spreading speed is O(0.5 m/s). An inertio-capillary force balance describes the experimentally observed spreading dynamics with excellent agreement.

Post-Impact Behavior of a Droplet Impacting on a Permeable Metal Mesh with a Sharp Wettability Step.

The impact of liquid droplets on permeable substrates is important for a number of applications, such as fog collection, liquid atomization, and interaction of liquids with filters and textiles. When a water droplet impacts a wettable mesh, it penetrates the mesh easily with a part of the liquid remaining pinned. On the other hand, when striking a superhydrophobic mesh, part of the water droplet may penetrate and detach from the parent droplet, depending upon the impact velocity and the relative length scales of the droplet and the mesh. In most cases, the remaining droplet would rebound from the top of the superhydrophobic mesh. In this work, we study the impact of a water droplet on a wettability-patterned mesh, with the droplet centrally impacting the wettability-contrast line between the superhydrophobic and superhydrophilic semi-infinite domains. Half of the droplet seeing the superhydrophobic domain responds to it in a fashion that differs from the half hitting the superhydrophilic mesh side. This creates a wide range of post-impact scenarios, depending on the impact conditions and the relative characteristics of the droplet and the mesh. The difference in mesh wettability leads to a net unbalanced surface-tension force that makes the droplet rebound with a horizontal momentum component directed from the non-wettable to the wettable side. Some part of the droplet may even detach during such directional rebounding (i.e., vectoring). Along with the experimental results, a simplified analytical model is presented, which differentiates the cases of detachment or no detachment during vectoring.

Scaling Laws in Directional Spreading of Droplets on Wettability-Confined Diverging Tracks.

Spontaneous pumpless transport of droplets on wettability-confined tracks is important for various applications, such as rapid transport and mixing of fluid droplets, enhanced dropwise condensation, biomedical devices, and so forth. Recent studies have shown that on an open surface, a superhydrophilic track of diverging width, laid on a superhydrophobic background, facilitates the transport of water from the narrower end to the wider end at unprecedented rates (up to 40 cm/s) without external actuation. The spreading behavior on such surfaces, however, has only been characterized for water. Keeping in mind that such designs play a key role for a diverse range of applications, such as handling organic liquids and in point-of-care devices, the importance of characterizing the spreading behavior of viscous liquids on such surfaces cannot be overemphasized. In the present work, the spreading behavior on the aforementioned wettability-patterned diverging tracks was observed for fluids of different viscosities. Two dimensionless variables were identified, and a comprehensive relationship was obtained. Three distinct temporal regimes of droplet spreading were established: I), a Washburn-type slow spreading, II) a much faster Laplace pressure-driven spreading, and III), a sluggish density-augmented Tanner-type film spreading. The results offer design guidance for tracks that can pumplessly manage fluids of various viscosities and surface tensions.

Precise Liquid Transport on and through Thin Porous Materials.

Porous substrates have the ability to transport liquids not only laterally on their open surfaces but also transversally through their thickness. Directionality of the fluid transport can be achieved through spatial wettability patterning of these substrates. Different designs of wettability patterns are implemented herein to attain different schemes (modes) of three-dimensional transport in a high-density paper towel, which acts as a thin porous matrix directing the fluid. All schemes facilitate precise transport of metered liquid microvolumes (dispensed as droplets) on the surface and through the substrate. One selected mode features lateral fluid transport along the bottom surface of the substrate, with the top surface remaining dry, except at the initial droplet dispension point. This configuration is investigated in further detail, and an analytical model is developed to predict the temporal variation of the penetrating drop shape. The analysis and respective measurements agree within the experimental error limits, thus confirming the model's ability to account for the main transport mechanisms.

Combating Frosting with Joule-Heated Liquid-Infused Superhydrophobic Coatings.

Frost formation is omnipresent when suitable environmental conditions are met. A good portion of research on combating frost formation has revolved around the passive properties of superhydrophobic (SHPO) and slippery lubricant-impregnated porous (SLIP) surfaces. Despite much progress, the need for surfaces that can effectively combat frost formation over prolonged periods still remains. In this work, we report, for the first time, the use of electrically conductive SHPO/SLIP surfaces for active mitigation of frost formation. First, we demonstrate the failure of these surfaces to passively avert prolonged (several hours) frosting. Next, we make use of their electroconductive property for active Joule heating, which results in the removal of any formed frost. We study the role of the impregnating lubricant in the heat transfer across the interface, the surface, and the ambient. We show that, even though the thermal properties of the impregnating lubricant may vary drastically, the lubricant type does not noticeably affect the defrosting behavior of the surface. We attribute this outcome to the dominant thermal resistance of the thick frost layer formed on the cooled surface. We support this claim by drawing parallels between the present system and heat transfer through a one-dimensional (1D) composite medium, and solving the appropriate transient transport equations. Lastly, we propose periodic thermal defrosting for averting frost formation altogether. This methodology utilizes the coating's passive repellent capabilities, while eliminating the dominant effect of thick deposited frost layers. The periodic heating approach takes advantage of lubricants with higher thermal conductivities, which effectively enhance heat transfer through the porous multiphase surface that forms the first line of defense against frosting.

Enhancing dropwise condensation through bioinspired wettability patterning.

Dropwise condensation (DWC) heat transfer depends strongly on the maximum diameter (Dmax) of condensate droplets departing from the condenser surface. This study presents a facile technique implemented to gain control of Dmax in DWC within vapor/air atmospheres. We demonstrate how this approach can enhance the corresponding heat transfer rate by harnessing the capillary forces in the removal of the condensate from the surface. We examine various hydrophilic-superhydrophilic patterns, which, respectively, sustain and combine DWC and filmwise condensation on the substrate. The material system uses laser-patterned masking and chemical etching to achieve the desired wettability contrast and does not employ any hydrophobizing agent. By applying alternating straight parallel strips of hydrophilic (contact angle ∼78°) mirror-finish aluminum and superhydrophilic regions (etched aluminum) on the condensing surface, we show that the average maximum droplet size on the less-wettable domains is nearly 42% of the width of the corresponding strips. An overall improvement in the condensate collection rate, up to 19% (as compared to the control case of DWC on mirror-finish aluminum) was achieved by using an interdigitated superhydrophilic track pattern (on the mirror-finish hydrophilic surface) inspired by the vein network of plant leaves. The bioinspired interdigitated pattern is found to outperform the straight hydrophilic-superhydrophilic pattern design, particularly under higher humidity conditions in the presence of noncondensable gases (NCG), a condition that is more challenging for maintaining sustained DWC.

Barriers to superfast water transport in carbon nanotube membranes.

Carbon nanotube (CNT) membranes hold the promise of extraordinary fast water transport for applications such as energy efficient filtration and molecular level drug delivery. However, experiments and computations have reported flow rate enhancements over continuum hydrodynamics that contradict each other by orders of magnitude. We perform large scale molecular dynamics simulations emulating for the first time the micrometer thick CNTs membranes used in experiments. We find transport enhancement rates that are length dependent due to entrance and exit losses but asymptote to 2 orders of magnitude over the continuum predictions. These rates are far below those reported experimentally. The results suggest that the reported superfast water transport rates cannot be attributed to interactions of water with pristine CNTs alone.

Real-time TEM observations of ice formation in graphene liquid cell.

The study of ice nucleation and growth at the nanoscale is of utmost importance in geological and atmospheric sciences. However, existing transmission electron microscopy (TEM) approaches have been unsuccessful in imaging ice formation directly. Herein, we demonstrate how radical scavengers - such as TiO2 - encased with water in graphene liquid cells (GLCs) facilitate the observation of ice nucleation phenomena at low temperatures. Atomic-resolution imaging reveals the nucleation and growth of cubic ice-phase crystals at close proximity to TiO2-water nanointerfaces at low temperatures. Interestingly, both heterogeneously and homogeneously nucleated ice crystals exhibited this cubic phase. Ice crystal nuclei were observed to be more stable at the TiO2-water nanointerface, as compared with crystals in the bulk liquid (homogeneous nucleation), suggesting the radical scavenging efficacy of TiO2 nanoparticles mitigating the electron beam by-products. The present work demonstrates that the use of radical scavengers in GLC TEM shows great promise towards unveiling the nanoscale pathways for ice nucleation and growth dynamic events.

A new approach of microbiome monitoring in the built environment: feasibility analysis of condensation capture.

BACKGROUND: Humans emit approximately 30 million microbial cells per hour into their immediate vicinity. However, sampling of aerosolized microbial taxa (aerobiome) remains largely uncharacterized due to the complexity and limitations of sampling techniques, which are highly susceptible to low biomass and rapid sample degradation. Recently, there has been an interest in developing technology that collects naturally occurring water from the atmosphere, even within the built environment. Here, we analyze the feasibility of indoor aerosol condensation collection as a method to capture and analyze the aerobiome. METHODS: Aerosols were collected via condensation or active impingement in a laboratory setting over the course of 8 h. Microbial DNA was extracted from collected samples and sequenced (16S rRNA) to analyze microbial diversity and community composition. Dimensional reduction and multivariate statistics were employed to identify significant (p < 0.05) differences in relative abundances of specific microbial taxa observed between the two sampling platforms. RESULTS: Aerosol condensation capture is highly efficient with a yield greater than 95% when compared to expected values. Compared to air impingement, aerosol condensation showed no significant difference (ANOVA, p > 0.05) in microbial diversity. Among identified taxa, Streptophyta and Pseudomonadales comprised approximately 70% of the microbial community composition. CONCLUSION: The results suggest that condensation of atmospheric humidity is a suitable method for the capture of airborne microbial taxa reflected by microbial community similarity between devices. Future investigation of aerosol condensation may provide insight into the efficacy and viability of this new tool to investigate airborne microorganisms. IMPORTANCE: On average, humans shed approximately 30 million microbial cells each hour into their immediate environment making humans the primary contributor to shaping the microbiome found within the built environment. In addition, recent events have highlighted the importance of understanding how microorganisms within the built environment are aerosolized and dispersed, but more importantly, the lack in development of technology that is capable of actively sampling the ever-changing aerosolized microbiome, i.e., aerobiome. This research highlights the capability of sampling the aerobiome by taking advantage of naturally occurring atmospheric humidity. Our novel approach reproduces the biological content in the atmosphere and can provide insight into the environmental microbiology of indoor spaces. Video Abstract.

A new methodology for measuring solid/liquid interfacial energy.

HYPOTHESIS: The interfacial energy γsl between a solid and a liquid designates the affinity between these two phases, and in turn, the macroscopic wettability of the surface by the fluid. This property is needed for precise control of fluid-transport phenomena that affect the operation/quality of commercial devices/products. Although several indirect or theoretical approaches can quantify the solid/liquid interfacial energy, no direct experimental procedure exists to measure this property for realistic (i.e. rough) surfaces. Makkonen hypothesized that the frictional resistance force per unit contact-line length is equal to the interfacial energy on smooth surfaces, which, however, are rarely found in practice. Consequently, the hypothesis that Makkonen's assumption may also hold for rough surfaces (which are far more common in practice) arises naturally. If so, a reliable and simple experimental methodology of obtaining γsl for rough surfaces can be put forth. This is accomplished by performing dynamic contact-angle experiments on rough surfaces that quantify the relationship between the frictional resistance force per unit contact-line length acting on an advancing liquid (Fp,a) and the surface roughness in wetting configurations. EXPERIMENT: We perform static and advancing contact-line experiments with aqueous and organic liquids on different hydrophilic surfaces (Al, Cu, Si) with varying Wenzel roughnesses in the range 1-2. These parameters are combined with the liquid's known surface tension to determine Fp,a. FINDINGS: Fp,a rises linearly with the surface roughness. Analysis based on existing theories of wetting and contact-angle hysteresis reveals that the slope of Fp,a vs.Wenzel roughness is equal to the solid/liquid interfacial energy, which is thus determined experimentally with the present measurements. Interfacial energies obtained with this experimental approach are within 12% of theoretically predicted values for several solid/liquid pairs, thereby validating this methodology.

Nanopumps without Pressure Gradients: Ultrafast Transport of Water in Patterned Nanotubes.

The extreme liquid transport properties of carbon nanotubes present new opportunities for surpassing conventional technologies in water filtration and purification. We demonstrate that carbon nanotubes with wettability surface patterns act as nanopumps for the ultrafast transport of picoliter water droplets without requiring externally imposed pressure gradients. Large-scale molecular dynamics simulations evidence unprecedented speeds and accelerations on the order of 1010 g of droplet propulsion caused by interfacial energy gradients. This phenomenon is persistent for nanotubes of varying sizes, stepwise pattern configurations, and initial conditions. We present a scaling law for water transport as a function of wettability gradients through simple models for the droplet dynamic contact angle and friction coefficient. Our results show that patterned nanotubes are energy-efficient nanopumps offering a realistic path toward ultrafast water nanofiltration and precision drug delivery.

Are superhydrophobic surfaces best for icephobicity?

Ice formation can have catastrophic consequences for human activity on the ground and in the air. Here we investigate water freezing delays on untreated and coated surfaces ranging from hydrophilic to superhydrophobic and use these delays to evaluate icephobicity. Supercooled water microdroplets are inkjet-deposited and coalesce until spontaneous freezing of the accumulated mass occurs. Surfaces with nanometer-scale roughness and higher wettability display unexpectedly long freezing delays, at least 1 order of magnitude longer than typical superhydrophobic surfaces with larger hierarchical roughness and low wettability. Directly related to the main focus on heterogeneous nucleation and freezing delay of supercooled water droplets, the observed ensuing crystallization process consisted of two distinct phases: one very rapid recalescent partial solidification phase and a subsequent slower phase. Observations of the droplet collision process employed for the continuous liquid mass accumulation up to the point of ice formation reveal a previously unseen atmospheric-pressure, subfreezing-temperature regime for liquid-on-liquid bounce. On the basis of the entropy reduction of water near a solid surface, we formulate a modification to the classical heterogeneous nucleation theory, which predicts the observed freezing delay trends. Our results bring to question recent emphasis on super water-repellent surface formulations for ice formation retardation and suggest that anti-icing design must optimize the competing influences of both wettability and roughness.

Revisiting the supplementary relationship of dynamic contact angles measured by sessile-droplet and captive-bubble methods: Role of surface roughness.

HYPOTHESIS: Quantitative characterization of surface wettability through contact angle (CA) measurement using the sessile droplet (SD) or captive bubble (CB) methods is often limited by the intrinsic wetting properties of the substrate. Situations may arise when an extreme surface wettability may preclude using one of the two methods for predicting the behaviors of droplets or bubbles on the surface. This warrants a relationship between the dynamic CAs measured via the SD and CB methods. While the two dynamic CAs (e.g., the advancing CA of SD and receding CA of CB) add up to 180° on a smooth surface, the simple geometric supplementary principle may not apply for rough surfaces. EXPERIMENTS: We perform a systematic wettability characterization of solid substrates with varying degrees of roughness using the sessile-droplet and captive-bubble methods, and interpret the experimental observations using a theoretical model. FINDINGS: The dynamic contact angles measured by the sessile-droplet and captive-bubble methods deviate from the supplementary principle as the surface roughness is increased. We present a theoretical explanation for this disparity and predict the values of the contact angles using prevalent thermodynamic models of wetting and contact-angle hysteresis on rough substrates. The theoretical prediction is in good agreement with the experimental observations.

Machine Learning Prediction of TiO2-Coating Wettability Tuned via UV Exposure.

Surfaces with extreme wettability (too low, superhydrophobic; too high, superhydrophilic) have attracted considerable attention over the past two decades. Titanium dioxide (TiO2) has been one of the most popular components for generating superhydrophobic/hydrophilic coatings. Combining TiO2 with ethanol and a commercial fluoroacrylic copolymer dispersion, known as PMC, can produce coatings with water contact angles approaching 170°. Another property of interest for this specific TiO2 formulation is its photocatalytic behavior, which causes the contact angle of water to be gradually reduced with rising timed exposure to UV light. While this formulation has been employed in many studies, there exists no quantitative guidance to determine or tune the contact angle (and thus wettability) with the composition of the coating and UV exposure time. In this article, machine learning models are employed to predict the required UV exposure time for any specified TiO2/PMC coating composition to attain a certain wettability (UV-reduced contact angle). For that purpose, eight different coating compositions were applied to glass slides and exposed to UV light for different time intervals. The collected contact-angle data was supplied to different regression models to designate the best method to predict the required UV exposure time for a prespecified wettability. Two types of machine learning models were used: (1) parametric and (2) nonparametric. The results showed a nonlinear behavior between the coating formulation and its contact angle attained after timed UV exposure. Nonparametric methods showed high accuracy and stability with general regression neural network (GRNN) performing best with an accuracy of 0.971, 0.977, and 0.933 on the test, train, and unseen data set, respectively. The present study not only provides quantitative guidance for producing coatings of specified wettability, but also presents a generalized methodology that could be employed for other functional coatings in technological applications requiring precise fluid/surface interactions.

Computer simulation of the SARS-CoV-2 contamination risk in a large dental clinic.

COVID-19, caused by the SARS-CoV-2 (severe acute respiratory syndrome coronavirus 2) virus, has been rapidly spreading worldwide since December 2019, causing a public health crisis. Recent studies showed SARS-CoV-2's ability to infect humans via airborne routes. These motivated the study of aerosol and airborne droplet transmission in a variety of settings. This study performs a large-scale numerical simulation of a real-world dentistry clinic that contains aerosol-generating procedures. The simulation tracks the dispersion of evaporating droplets emitted during ultrasonic dental scaling procedures. The simulation considers 25 patient treatment cubicles in an open plan dentistry clinic. The droplets are modeled as having a volatile (evaporating) and nonvolatile fraction composed of virions, saliva, and impurities from the irrigant water supply. The simulated clinic's boundary and flow conditions are validated against experimental measurements of the real clinic. The results evaluate the behavior of large droplets and aerosols. We investigate droplet residence time and travel distance for different droplet diameters, surface contamination due to droplet settling and deposition, airborne aerosol mass concentration, and the quantity of droplets that escape through ventilation. The simulation results raise concerns due to the aerosols' long residence times (averaging up to 7.31 min) and travel distances (averaging up to 24.45 m) that exceed social distancing guidelines. Finally, the results show that contamination extends beyond the immediate patient treatment areas, requiring additional surface disinfection in the clinic. The results presented in this research may be used to establish safer dental clinic operating procedures, especially if paired with future supplementary material concerning the aerosol viral load generated by ultrasonic scaling and the viral load thresholds required to infect humans.

Wettability-Engineered Meshes for Gas Microvolume Precision Handling in Liquids.

The interaction of rising gas bubbles with submerged air-repelling or air-attracting surfaces is relevant to various technological applications that rely on gas-microvolume handling or removal. This work demonstrates how submerged metal meshes with super air-attracting/repelling properties can be employed to manipulate microvolumes of air, rising buoyantly in the form of bubbles in water. Superaerophobic meshes are observed to selectively allow the passage of air bubbles depending on the mesh pore size, the bubble volume-equivalent diameter, and the bubble impact velocity on the mesh. On the other hand, superaerophilic meshes reduce or amplify the volume captured from a train of incoming bubbles. Finally, a spatial wettability pattern on the mesh is used to control the size of the outgoing bubble, and an empirical relation is formulated to predict the released gas volume. The study demonstrates how porous materials with controlled wettability can be used to precisely modulate and control the outcome of bubble/mesh interactions.

Surface Treatments to Enhance the Functionality of PPEs.

The outbreak of unknown viral pneumonia in Wuhan China in December 2019 led to a new coronavirus (SARS-CoV-2), which attracted worldwide attention, with the related COVID-19 disease quickly becoming a global pandemic. In about 5 months, this disease has led to ~ 4 million cases and claimed more than 200 k deaths as a result of its highly contagious nature. The present understanding is that SARS-CoV-2 is a type of influenza virus that can be transmitted through respiratory droplets and aerosols; Lewis (Nature 580:175, 2020). The primary methodology to prevent the spreading of this disease has been "social distancing" and usage of personal protective equipment (PPE) at the front lines of healthcare and other critical operations. The scale of the disease has led to unprecedented demand for PPEs and increased functionality of the same. This paper focuses on improving PPE functionality in a scalable manner by surface treatment and coating with appropriate materials and other functional enhancements, such as exposure to UV rays or other sterilizing agents (e.g., hydrogen peroxide).

Correlative ex situ and Liquid-Cell TEM Observation of Bacterial Cell Membrane Damage Induced by Rough Surface Topology.

BACKGROUND: Nanoscale surface roughness has been suggested to have antibacterial and antifouling properties. Several existing models have attempted to explain the antibacterial mechanism of nanoscale rough surfaces without direct observation. Here, conventional and liquid-cell TEM are implemented to observe nanoscale bacteria/surface roughness interaction. The visualization of such interactions enables the inference of possible antibacterial mechanisms. METHODS AND RESULTS: Nanotextures are synthesized on biocompatible polymer microparticles (MPs) via plasma etching. Both conventional and liquid-phase transmission electron microscopy observations suggest that these MPs may cause cell lysis via bacterial binding to a single protrusion of the nanotexture. The bacterium/protrusion interaction locally compromises the cell wall, thus causing bacterial death. This study suggests that local mechanical damage and leakage of the cytosol kill the bacteria first, with subsequent degradation of the cell envelope. CONCLUSION: Nanoscale surface roughness may act via a penetrative bactericidal mechanism. This insight suggests that future research may focus on optimizing bacterial binding to individual nanoscale projections in addition to stretching bacteria between nanopillars. Further, antibacterial nanotextures may find use in novel applications employing particles in addition to nanotextures on fibers or films.