On-Demand, Contact-Less and Loss-Less Droplet Manipulation via Contact Electrification.

While there are many droplet manipulation techniques, all of them suffer from at least one of the following drawbacks - complex fabrication or complex equipment or liquid loss. In this work, a simple and portable technique is demonstrated that enables on-demand, contact-less and loss-less manipulation of liquid droplets through a combination of contact electrification and slipperiness. In conjunction with numerical simulations, a quantitative analysis is presented to explain the onset of droplet motion. Utilizing the contact electrification technique, contact-less and loss-less manipulation of polar and non-polar liquid droplets on different surface chemistries and geometries is demonstrated. It is envisioned that the technique can pave the way to simple, inexpensive, and portable lab on a chip and point of care devices.

A gravity-driven droplet fluidic point-of-care test.

We report a simple droplet fluidic point-of-care test (POCT) that uses gravity to manipulate the sequence, timing, and motion of droplets on a surface. To fabricate this POCT, we first developed a surface coating toolbox of nine different coatings with three levels of wettability and three levels of slipperiness that can be independently tailored. We then fabricated a device that has interconnected fluidic elements-pumps, flow resistors and flow guides-on a highly slippery solid surface to precisely control the timing and sequence of motion of multiple droplets and their interactions on the surface. We then used this device to carry out a multi-step enzymatic assay of a clinically relevant analyte-lactate dehydrogenase (LDH)-to demonstrate the application of this technology for point-of-care diagnosis.

Designing Non-Textured, All-Solid, Slippery Hydrophilic Surfaces.

Slippery surfaces are sought after due to their wide range of applications in self-cleaning, drag reduction, fouling-resistance, enhanced condensation, biomedical implants etc. Recently, non-textured, all-solid, slippery surfaces have gained significant attention because of their advantages over super-repellent surfaces and lubricant-infused surfaces. Currently, almost all non-textured, all-solid, slippery surfaces are hydrophobic. In this work, we elucidate the systematic design of non-textured, all-solid, slippery hydrophilic (SLIC) surfaces by covalently grafting polyethylene glycol (PEG) brushes to smooth substrates. Furthermore, we postulate a plateau in slipperiness above a critical grafting density, which occurs when the tethered brush size is equal to the inter-tether distance. Our SLIC surfaces demonstrate exceptional performance in condensation and fouling-resistance compared to non-slippery hydrophilic surfaces and slippery hydrophobic surfaces. Based on these results, SLIC surfaces constitute an emerging class of surfaces with the potential to benefit multiple technological landscapes ranging from thermofluidics to biofluidics.

On-demand, remote and lossless manipulation of biofluid droplets.

The recent global outbreaks of epidemics and pandemics have shown us that we are severely under-prepared to cope with infectious agents. Exposure to infectious agents present in biofluids (e.g., blood, saliva, urine etc.) poses a severe risk to clinical laboratory personnel and healthcare workers, resulting in hundreds of millions of hospital-acquired and laboratory-acquired infections annually. Novel technologies that can minimize human exposure through remote and automated handling of infectious biofluids will mitigate such risk. In this work, we present biofluid manipulators, which allow on-demand, remote and lossless manipulation of virtually any liquid droplet. Our manipulators are designed by integrating thermo-responsive soft actuators with superomniphobic surfaces. Utilizing our manipulators, we demonstrate on-demand, remote and lossless manipulation of biofluid droplets. We envision that our biofluid manipulators will not only reduce manual operations and minimize exposure to infectious agents, but also pave the way for developing inexpensive, simple and portable robotic systems, which can allow point-of-care operations, particularly in developing nations.

Droplet Evaporation Dynamics of Low Surface Tension Fluids Using the Steady Method.

Droplet evaporation governs many heat- and mass-transfer processes germane in nature and industry. In the past 3 centuries, transient techniques have been developed to characterize the evaporation of sessile droplets. These methods have difficulty in reconciling transient effects induced by the droplet shape and size changes during evaporation. Furthermore, investigation of evaporation of microdroplets residing on wetting substrates, or fluids having low surface tensions (<30 mN/m), is difficult to perform using established approaches. Here, we use the steady method to study the microdroplet evaporation dynamics of low surface tension liquids. We start by employing the steady method to benchmark with water droplets having base radii (20 ≤ Rb ≤ 260 µm), apparent advancing contact angle (45° ≤ θa,app ≤ 162°), surface temperature (30 < Ts < 60 °C), and relative humidity (40% < ϕ < 60%). Following validation, evaporation of ethanol (≈22 mN/m), hexane (≈18 mN/m), and dodecane (≈25 mN/m) were studied for 90 ≤ Rb ≤ 400 µm and 10 < Ts < 25 °C. We elucidate the mechanisms governing the observed behavior using heat and mass transport scaling analysis during evaporation, demonstrating our steady technique to be particularly advantageous for microdroplets, where Marangoni and buoyant forces are negligible. Our work not only elucidates the droplet evaporation mechanisms of low surface tension liquids but also demonstrates the steady method as a means to study phase change processes.

Dropwise condensation on solid hydrophilic surfaces.

Droplet nucleation and condensation are ubiquitous phenomena in nature and industry. Over the past century, research has shown dropwise condensation heat transfer on nonwetting surfaces to be an order of magnitude higher than filmwise condensation heat transfer on wetting substrates. However, the necessity for nonwetting to achieve dropwise condensation is unclear. This article reports stable dropwise condensation on a smooth, solid, hydrophilic surface (θa = 38°) having low contact angle hysteresis (<3°). We show that the distribution of nano- to micro- to macroscale droplet sizes (about 100 nm to 1 mm) for coalescing droplets agrees well with the classical distribution on hydrophobic surfaces and elucidate that the wettability-governed dropwise-to-filmwise transition is mediated by the departing droplet Bond number. Our findings demonstrate that achieving stable dropwise condensation is not governed by surface intrinsic wettability, as assumed for the past eight decades, but rather, it is dictated by contact angle hysteresis.

Trade-off in membrane distillation with monolithic omniphobic membranes.

Omniphobic membranes are attractive for membrane distillation (MD) because of their superior wetting resistance. However, a design framework for MD membrane remains incomplete, due to the complexity of omniphobic membrane fabrication and the lack of fundamental relationship between wetting resistance and water vapor permeability. Here we present a particle-free approach that enables rapid fabrication of monolithic omniphobic membranes for MD desalination. Our monolithic omniphobic membranes display excellent wetting resistance and water purification performance in MD desalination of hypersaline feedwater containing surfactants. We identify that a trade-off exists between wetting resistance and water vapor permeability of our monolithic MD membranes. Utilizing membranes with tunable wetting resistance and permeability, we elucidate the underlying mechanism of such trade-off. We envision that our fabrication method as well as the mechanistic insight into the wetting resistance-vapor permeability trade-off will pave the way for smart design of MD membranes in diverse water purification applications.

Droplet Jumping: Effects of Droplet Size, Surface Structure, Pinning, and Liquid Properties.

Coalescence-induced droplet jumping has the potential to enhance the efficiency of a plethora of applications. Although binary droplet jumping is quantitatively understood from energy and hydrodynamic perspectives, multiple aspects that affect jumping behavior, including droplet size mismatch, droplet-surface interaction, and condensate thermophysical properties, remain poorly understood. Here, we develop a visualization technique utilizing microdroplet dispensing to study droplet jumping dynamics on nanostructured superhydrophobic, hierarchical superhydrophobic, and hierarchical biphilic surfaces. We show that on the nanostructured superhydrophobic surface the jumping velocity follows inertial-capillary scaling with a dimensionless velocity of 0.26 and a jumping direction perpendicular to the substrate. A droplet mismatch phase diagram was developed showing that jumping is possible for droplet size mismatch up to 70%. On the hierarchical superhydrophobic surface, jumping behavior was dependent on the ratio between the droplet radius Ri and surface structure length scale L. For small droplets ( Ri ≤ 5 L), the jumping velocity was highly scattered, with a deviation of the jumping direction from the substrate normal as high as 80°. Surface structure length scale effects were shown to vanish for large droplets ( Ri > 5 L). On the hierarchical biphilic surface, similar but more significant scattering of the jumping velocity and direction was observed. Droplet-size-dependent surface adhesion and pinning-mediated droplet rotation were responsible for the reduced jumping velocity and scattered jumping direction. Furthermore, droplet jumping studies of liquids with surface tensions as low as 38 mN/m were performed, further confirming the validity of inertial-capillary scaling for varying condensate fluids. Our work not only demonstrates a powerful platform to study droplet-droplet and droplet-surface interactions but provides insights into the role of fluid-substrate coupling as well as condensate properties during droplet jumping.

Superomniphobic Surfaces with Improved Mechanical Durability: Synergy of Hierarchical Texture and Mechanical Interlocking.

Due to their unique functionality, superomniphobic surfaces that display extreme repellency toward virtually any liquid, have a wide range of potential applications. However, to date, the mechanical durability of superomniphobic surfaces remains a major obstacle that prevents their practical deployment. In this work, a two-layer design strategy was developed to fabricate superomniphobic surfaces with improved durability via synergistic effect of interconnected hierarchical porous texture and micro/nano-mechanical interlocking. The improved mechanical robustness of these surfaces was assessed through water shear test, ultrasonic washing test, blade scratching test, and Taber abrasion test.

Coalescence-induced jumping of droplets on superomniphobic surfaces with macrotexture.

When two liquid droplets coalesce on a superrepellent surface, the excess surface energy is partly converted to upward kinetic energy, and the coalesced droplet jumps away from the surface. However, the efficiency of this energy conversion is very low. In this work, we used a simple and passive technique consisting of superomniphobic surfaces with a macrotexture (comparable to the droplet size) to experimentally demonstrate coalescence-induced jumping with an energy conversion efficiency of 18.8% (i.e., about 570% increase compared to superomniphobic surfaces without a macrotexture). The higher energy conversion efficiency arises primarily from the effective redirection of in-plane velocity vectors to out-of-plane velocity vectors by the macrotexture. Using this higher energy conversion efficiency, we demonstrated coalescence-induced jumping of droplets with low surface tension (26.6 mN m-1) and very high viscosity (220 mPa·s). These results constitute the first-ever demonstration of coalescence-induced jumping of droplets at Ohnesorge number >1.

Coalescence-Induced Self-Propulsion of Droplets on Superomniphobic Surfaces.

We utilized superomniphobic surfaces to systematically investigate the different regimes of coalescence-induced self-propulsion of liquid droplets with a wide range of droplet radii, viscosities, and surface tensions. Our results indicate that the nondimensional jumping velocity Vj* is nearly constant (Vj* ≈ 0.2) in the inertial-capillary regime and decreases in the visco-capillary regime as the Ohnesorge number Oh increases, in agreement with prior work. Within the visco-capillary regime, decreasing the droplet radius R0 results in a more rapid decrease in the nondimensional jumping velocity Vj* compared to increasing the viscosity µ. This is because decreasing the droplet radius R0 increases the inertial-capillary velocity Vic in addition to increasing the Ohnesorge number Oh.

Metamorphic Superomniphobic Surfaces.

Superomniphobic surfaces are extremely repellent to virtually all liquids. By combining superomniphobicity and shape memory effect, metamorphic superomniphobic (MorphS) surfaces that transform their morphology in response to heat are developed. Utilizing the MorphS surfaces, the distinctly different wetting transitions of liquids with different surface tensions are demonstrated and the underlying physics is elucidated. Both ex situ and in situ wetting transitions on the MorphS surfaces are solely due to transformations in morphology of the surface texture. It is envisioned that the robust MorphS surfaces with reversible wetting transition will have a wide range of applications including rewritable liquid patterns, controlled drug release systems, lab-on-a-chip devices, and biosensors.

Hemodynamic Performance and Thrombogenic Properties of a Superhydrophobic Bileaflet Mechanical Heart Valve.

In this study, we explore how blood-material interactions and hemodynamics are impacted by rendering a clinical quality 25 mm St. Jude Medical Bileaflet mechanical heart valve (BMHV) superhydrophobic (SH) with the aim of reducing thrombo-embolic complications associated with BMHVs. Basic cell adhesion is evaluated to assess blood-material interactions, while hemodynamic performance is analyzed with and without the SH coating. Results show that a SH coating with a receding contact angle (CA) of 160° strikingly eliminates platelet and leukocyte adhesion to the surface. Alternatively, many platelets attach to and activate on pyrolytic carbon (receding CA = 47), the base material for BMHVs. We further show that the performance index increases by 2.5% for coated valve relative to an uncoated valve, with a maximum possible improved performance of 5%. Both valves exhibit instantaneous shear stress below 10 N/m2 and Reynolds Shear Stress below 100 N/m2. Therefore, a SH BMHV has the potential to relax the requirement for antiplatelet and anticoagulant drug regimens typically required for patients receiving MHVs by minimizing blood-material interactions, while having a minimal impact on hemodynamics. We show for the first time that SH-coated surfaces may be a promising direction to minimize thrombotic complications in complex devices such as heart valves.

Free-Standing, Flexible, Superomniphobic Films.

Fabrication of most superomniphobic surfaces requires complex process conditions or specialized and expensive equipment or skilled personnel. In order to circumvent these issues and make them end-user-friendly, we developed the free-standing, flexible, superomniphobic films. These films can be stored and delivered to the end-users, who can readily attach them to virtually any surface (even irregular shapes) and impart superomniphobicity. The hierarchical structure, the re-entrant texture, and the low solid surface energy render our films superomniphobic for a wide variety of liquids. We demonstrate that our free-standing, flexible, superomniphobic films have applications in enhanced chemical resistance and enhanced weight bearing.

Superhydrophobic Coatings with Edible Materials.

We used FDA-approved, edible materials to fabricate superhydrophobic coatings in a simple, low cost, scalable, single step process. Our coatings display high contact angles and low roll off angles for a variety of liquid products consumed daily and facilitate easy removal of liquids from food containers with virtually no residue. Even at high concentrations, our coatings are nontoxic, as shown using toxicity tests.