Biofilm formation of Pseudomonas aeruginosa in spaceflight is minimized on lubricant impregnated surfaces.

The undesirable, yet inevitable, presence of bacterial biofilms in spacecraft poses a risk to the proper functioning of systems and to astronauts' health. To mitigate the risks that arise from them, it is important to understand biofilms' behavior in microgravity. As part of the Space Biofilms project, biofilms of Pseudomonas aeruginosa were grown in spaceflight over material surfaces. Stainless Steel 316 (SS316) and passivated SS316 were tested for their relevance as spaceflight hardware components, while a lubricant impregnated surface (LIS) was tested as potential biofilm control strategy. The morphology and gene expression of biofilms were characterized. Biofilms in microgravity are less robust than on Earth. LIS strongly inhibits biofilm formation compared to SS. Furthermore, this effect is even greater in spaceflight than on Earth, making LIS a promising option for spacecraft use. Transcriptomic profiles for the different conditions are presented, and potential mechanisms of biofilm reduction on LIS are discussed.

Reducing Cancer Cell Adhesion using Microtextured Surfaces.

For the past century, trypsin has been the primary method of cell dissociation, largely without any major changes to the process. Enzymatic cell detachment strategies for large-scale cell culturing processes are popular but can be labor-intensive, potentially lead to the accumulation of genetic mutations, and produce large quantities of liquid waste. Therefore, engineering surfaces to lower cell adhesion strength could enable the next generation of cell culture surfaces for delicate primary cells and automated, high-throughput workflows. In this study, a process for creating microtextured polystyrene (PS) surfaces to measure the impact of microposts on the adhesion strength of cells is developed. Cell viability and proliferation assays show comparable results in two cancer cell lines between micropost surfaces and standard cell culture vessels. However, cell image analysis on microposts reveals that cell area decreases by half, and leads to an average twofold increase in cell length per area. Using a microfluidic-based method up to a seven times greater percentage of cells are removed from micropost surfaces than the flat control surfaces. These results show that micropost surfaces enable decreased cell adhesion strength while maintaining similar cell viabilities and proliferation as compared to flat PS surfaces.

Self-ejection of salts and other foulants from superhydrophobic surfaces to enable sustainable anti-fouling.

A recently discovered phenomenon in which crystalline structures grown from evaporating drops of saline water self-eject from superhydrophobic materials has introduced new possibilities for the design of anti-fouling materials and sustainable processes. Some of these possibilities include evaporative heat exchange systems using drops of saline water and new strategies for handling/processing waste brines. However, the practical limits of this effect using realistic, non-ideal source waters have yet to be explored. Here, we explore how the presence of various model aquatic contaminants (colloids, surfactants, and calcium salt) influences the self-ejection phenomena. Counterintuitively, we find that the addition of "contaminant" chemistries can enable ejection under conditions where ejection was not observed for waters containing only sodium chloride salt (e.g., from smooth hydrophobic surfaces), and that increased concentrations of both surfactants and colloids lead to longer ejection lengths. This result can be attributed to decreased crystallization nucleation time caused by the presence of other species in water.

Enhancing Protein Crystal Nucleation Using In Situ Templating on Bioconjugate-Functionalized Nanoparticles and Machine Learning.

Although protein crystallization offers a promising alternative to chromatography for lower-cost protein purification, slow nucleation kinetics and high protein concentration requirements are major barriers for using crystallization as a viable strategy in downstream protein purification. Here, we demonstrate that nanoparticles functionalized with bioconjugates can result in an in situ template for inducing rapid crystallization of proteins at low protein concentration conditions. We use a microbatch crystallization setup to show that the range of successful crystallization conditions is expanded by the presence of functionalized nanoparticles. Furthermore, we use a custom machine learning-enabled emulsion crystallization setup to rigorously quantify nucleation parameters. We show that bioconjugate-functionalized nanoparticles can result in up to a 7-fold decrease in the induction time and a 3-fold increase in the nucleation rate of model proteins compared to those in control environments. We thus provide foundational insight that could enable crystallization to be used in protein manufacturing by reducing both the protein concentration and the time required to nucleate protein crystals.

Dynamics of an impacting emulsion droplet.

Emulsions are widely used in agriculture where oil-based pesticides are sprayed as an emulsion. However, emulsion droplets can bounce off hydrophobic plant surfaces, leading to major health and environmental issues as pesticides pollute water sources and soils. Here, we report an unexpected transition from bouncing to sticking to bouncing as the droplet impact speed increases. We show that the physics are governed by an in situ, self-generated lubrication of the surface leading to a suction force from the nascent oil layer around the droplet. We demonstrate that this phenomenon can be controlled by a careful balance of three time scales: the contact time of the droplet, the impregnation time scale of the oil, and the oil ridge formation time scale. We lastly build a design map to precisely control the bouncing of droplets and the oil coverage of the target surface. These insights have broad applicability in agriculture, cooling sprays, combustion, and additive manufacturing.

Electrostatic dust removal using adsorbed moisture-assisted charge induction for sustainable operation of solar panels.

Dust accumulation on solar panels is a major challenge, as it blocks a large portion of sunlight. Solar panels are therefore cleaned regularly using large quantities of pure water. Consumption of water for cleaning, especially in deserts, poses a substantial sustainability challenge. Here, we present a waterless approach for dust removal from solar panels using electrostatic induction. We find that dust particles, despite primarily consisting of insulating silica, can be electrostatically repelled from electrodes due to charge induction assisted by adsorbed moisture. We experimentally determine dust particle charge by conducting Stokes experiments under an electrostatic field. By considering electrostatic, van der Waals, and gravitational forces, we define the threshold electric potential for particle removal. We also demonstrate dust removal over a broad range of relative humidity, making our approach widely applicable. Last, we develop a lab-scale prototype and demonstrate up to 95% recovery of lost power output using our approach.

Impact of Bubbles on Electrochemically Active Surface Area of Microtextured Gas-Evolving Electrodes.

The adverse effects of electrochemical bubbles on the performance of gas-evolving electrodes have been extensively studied. However, the ways in which bubbles dynamically alter the electrochemically active surface area during bubble evolution are not well understood. Here, we study hydrogen evolution at industrially relevant current densities by using controlled microtexture to examine this fundamental relationship. Surprisingly, the most densely microtextured electrodes have the lowest performance on an active surface area basis. Using high-speed imaging, we show that the benefits of microtexture to release smaller bubbles more consistently are outweighed by the inactivation induced by bubbles growing within the denser microtexture, causing these performance limitations. Additionally, we show that the area beneath adhered bubbles is electrochemically active, contrary to currently held assumptions. Our study therefore has broad implications for electrode design to avoid ineffective use of precious catalyst materials, which is especially critical for porous electrodes and three-dimensional structures with high specific surface areas.

Transient Effects Caused by Gas Depletion during Carbon Dioxide Electroreduction.

The novel use of carbon dioxide (CO2) electroreduction to generate carbon-based products which do not contribute to the greenhouse effect has promoted the vision of carbon dioxide as a renewable feedstock for future clean fuel production. Depending on the material choice for the electrocatalysis, a certain variety of products is expected from the carbon dioxide reduction reaction (CO2RR). However, as the CO2 concentration in areas close to the working electrode (relative to the diffusive boundary layer) decreases as it is being consumed and transformed into other products, the generation of H2 is favored to the detriment of CO2 electroreduction. Therefore, the extent to which H2 is produced can be used as a metric to evaluate the efficiency of CO2RR. This article proposes a model that accounts for the modes in which aqueous gas depletion evolves over time and affects the long-term CO2 electroreduction and the corresponding pH evolution near the electrode's surface. For the latter, two main contributions are distinguished: gas depletion due to CO2 consumption and ion generation in areas close to the electrocatalyst surface. pH is then suggested as an accurate and indirect means to measure CO2 concentration in a liquid electrolyte. We conclude that CO2 depletion causes a strong decay in the electrochemical reaction efficiency. In the end, we discuss several methods which may delay the onset of the adverse effects caused by gas depletion, such as the utilization of pulsed electroreduction, cycling the applied current to electrodes on and off periodically.

Phase Change Dispersion Made by Condensation-Emulsification.

Cooling processes require heat transfer fluids with high specific heat capacity. For cooling processes below 0 °C, water has to be diluted with organic liquids to prevent freezing, with the undesired effect of reduced specific heat capacity. Phase change dispersions, PCDs, consist of a phase change material, PCM, being dispersed in a continuous phase. This allows for using the PCD as heat transfer fluid with a very high apparent specific heat capacity within a specified, limited temperature range. So far, the PCMs being reported in the literature are paraffins, fatty acids, or esters and are used for isothermal cooling applications between +4 and +50 °C. They are manufactured by high shear equipment like rotor-stator systems. A recently published method to produce emulsions by the direct condensation of the dispersed phase into the emulsifier-containing continuous phase is applied on this PCD. n-Decane is used as PCM, and the melting temperature is -30 °C. The achieved apparent specific heat capacity lies above 15 kJ/kg·K, more than 3 times the value of water. This paper presents experimental methods and data, formulation details, and thermophysical and rheological properties of such new PCD. Food conservation or isothermal cooling of lithium-ion batteries is a potential application for the presented method. The properties of the developed PCD were determined, and the successful application of such a PCD at -30 °C has been demonstrated.

Self-Propulsion of Boiling Droplets on Thin Heated Oil Films.

We report on the self-propulsion of boiling droplets which, despite their contact with viscous, immiscible oil films, attain high velocities comparable to those of levitating Leidenfrost droplets. Experiments and model reveal that droplet propulsion originates from a coupling between seemingly disparate short and long timescale phenomena due to microsecond fluctuations induced by boiling events at the droplet-oil interface. This interplay of phenomena leads to continuous asymmetric vapor release and momentum transfer for high droplet velocities.

Levitation of fizzy drops.

As first described by Leidenfrost, liquid droplets levitate over their own vapor when placed on a sufficiently hot substrate. The Leidenfrost effect not only confers remarkable properties such as mechanical and thermal insulation, zero adhesion, and extreme mobility but also requires a high energetic thermal cost. We describe here a previously unexplored approach using active liquids able to sustain levitation in the absence of any external forcing at ambient temperature. We focus on the particular case of carbonated water placed on a superhydrophobic solid and demonstrate how millimetric fizzy drops self-generate a gas cushion that provides levitation on time scales on the order of a minute. Last, we generalize this new regime to different kinds of chemically reactive droplets able to jump from the Cassie-Baxter state to a levitating regime, paving the way to the levitation of nonvolatile liquids.

Crystal critters: Self-ejection of crystals from heated, superhydrophobic surfaces.

Mineral or crystal fouling (the accumulation of precipitants on a material and damage associated with the same) is a pervasive problem in water treatment, thermoelectric power production, and numerous industrial processes. Growing efforts have focused on materials engineering strategies (e.g., superhydrophobicity) to prevent fouling. Here, we present a curious phenomenon in which crystals self-eject from heated, nanotextured superhydrophobic materials during evaporation of saline water drops. These crystal structures (crystal critters) have exceedingly minimal contact with the substrate and thus pre-empt crystal fouling. This unusual phenomenon is caused by cooperative effects of crystallization, evaporative flows, and nanoscale effects. The temperature dependence of the critter effect can be predicted using principles of mass conservation, and we demonstrate that self-propulsion can be generated via temperature gradients, which promote asymmetric growth. The insights on confinement-driven evaporative crystallization can be applied for antifouling by self-ejection of mineral foulants, for drop-based fluidic machines, or even for self-propulsion.

Differences between Colloidal and Crystalline Evaporative Deposits.

Evaporative deposits from drops are widely studied due to their numerous applications in low-effort self-assembly, including for inkjet printing, microscale separations, and sensing/diagnostics. This phenomenon has been broadly explored for drops containing suspended colloidal particles but has been less quantified for drops with dissolved solutes. When a drop of solute/solvent mixture is evaporated on a substrate, nonvolatile solutes become supersaturated as the solvent evaporates, which then leads to crystal nucleation at the substrate-drop contact line. Emerging crystals alter the local wettability and fundamentally alter the dynamics of evaporation, which, in turn, influences the resultant evaporative deposit. Here we investigate the role of interactions between the substrate, crystals, and solution by comparing the evaporative deposition of three different salts as solutes against an evaporating colloidal solution. We show that nucleation effects can cause crystalline deposits to have a temperature relationship that is opposite to that of colloidal deposits and demonstrate how a balance between the contact-line pinning force and nucleation controls the deposit size.

Enhancing the Injectability of High Concentration Drug Formulations Using Core Annular Flows.

Highly concentrated biological drug formulations would offer tremendous benefits to global health, yet they cannot be manually injected using commercial syringes and needles due to their high viscosities. Current approaches to address this problem face several challenges such as crosscontamination, high cost, needle clogging, and protein inactivation. This work reports a simple method to enhance formulation injectability using a core annular flow, where the transport of highly viscous fluids through a needle is enabled by coaxial lubrication by a less viscous fluid. A phase diagram to ensure optimally lubricated flow while minimizing the volume fraction of lubricant injected is established. The technique presented here allows for up to a 7x reduction in injection force for the highest viscosity ratio tested. The role of buoyancy-driven eccentricity in governing nominal pressure reduction is also examined. Finally, the findings are implemented into the development of a double barreled syringe that significantly expands the range of injectable concentrations of several biologic formulations.

Author Correction: Enhancing droplet deposition through in-situ precipitation.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Lubricant-Impregnated Surfaces for Mitigating Asphaltene Deposition.

Asphaltenes are heavy aromatic components of crude oil. Their complex chemical makeup-an aromatic core surrounded by aliphatic side chains-enables them to adhere to most surfaces. Their buildup in pipes can result in clogging and lead to interruption of production operations and expensive mechanical cleaning. We demonstrate the use of liquid-impregnated surfaces (LIS) to prevent asphaltene deposition and buildup on substrates. Indeed, these surfaces expose a liquid interface to the working fluid, which combines the benefits of a dynamic defect-free surface and tunable interfacial properties. In contrast to bulk additives that are typically mixed into the oil phase, the impregnating liquid also provides the great benefit of protecting the underlying solid surface with a stable and minimal layer of lubricant, thereby reducing costs and eliminating the need for subsequent downstream removal. We first select and confirm the thermodynamic stability of a suitable lubricant and its lack of interaction with asphaltenes. By using a carefully selected system composed of a textured and functionalized solid substrate in conjunction with a fluorinated lubricant, we show that asphaltene adsorption is prevented over long time scales. We further demonstrate the possibility of building such a system with representative industrial materials such as aluminum and expose the resulting substrate to an external shear flow to simulate pipe flow conditions.

Asphaltene Adsorption on Functionalized Solids.

Asphaltenes, heavy aromatic components of crude oil, are known to adsorb on surfaces and can lead to pipe clogging or hinder oil recovery. Because of their multicomponent structure, the details of their interactions with surfaces are complex. We investigate the effect of the physicochemical properties of the substrate on the extent and mechanism of this adsorption. Using wetting measurements, we relate the initial kinetics of deposition to the interfacial energy of the surface. We then quantify the long-term adsorption dynamics using a quartz crystal microbalance and ellipsometry. Finally, we investigate the mechanism and morphology of adsorption with force spectroscopy measurements as a function of surface chemistry. We determine different adsorption regimes differing in orientation, packing density, and initial kinetics on different substrate functionalizations. Specifically, we find that alkane substrates delay the initial monolayer formation, fluorinated surfaces exhibit fast adsorption but low bonding strength, and hydroxyl substrates lead to a different adsorption orientation and a high packing density of the asphaltene layer.

Low-Voltage Surface Electrocoalescence Enabled by High-K Dielectrics and Surfactant Bilayers for Oil-Water Separation.

Processes for separating oil-water mixtures are critical to operations in energy and water. However, existing separation methods pose efficiency limitations as well as environmental and safety challenges. Here, we present a low-voltage surface electrocoalescence approach that triggers coalescence of surfactant-stabilized emulsions by combining high-K dielectrics with surfactant bilayers. In this system, the high-K dielectric reduces the electrocoalescence voltage, while the surfactant bilayer functions as a self-healing, high capacitance film that prevents pinning of droplets on the dielectric surface. This high capacitance system maximizes the electric field between neighboring droplets, exerting high electrostatic pressure that overcomes the disjoining pressure between droplets, thereby enabling rapid electrocoalescence. We demonstrate electrocoalescence of surfactant-stabilized microscale droplets of saline water in oil using single volts. We expect our results may find application in the energy sector, wastewater treatment, and purification industries.

Evaporative Crystallization of Spirals.

Spiral motifs are pervasive in nature, art, and technology due to their functional property of providing compact length. Nature is particularly adept at spiral patterning, and yet, the spirals observed in seashells, hurricanes, rams' horns, flower petals, etc. all evolve via disparate physical mechanisms. Here, we present a mechanism for the self-guided formation of spirals from evaporating saline drops via a coupling of crystallization and contact line dynamics. These patterns are in contrast to commonly observed patterns from evaporation of colloidal drops, which are discrete (rings, concentric rings) or continuous (clumps, uniform deposits) depending on the particle shape, contact line dynamics, and evaporation rate. Unlike the typical process of drop evaporation where the contact line moves radially inward, here, a thin film pinned by a ring of crystals ruptures radially outward. This motion is accompanied by a nonuniform pinning of the contact line due to crystallization, which generates a continuous propagation of pinning and depinning events to form a spiral. By comparing the relevant timescales of evaporation and diffusion, we show that a single dimensionless number can predict the occurrence of these patterns. These insights on self-guided crystallization of spirals could be used to create compact length templates.

Waterbowls: Reducing Impacting Droplet Interactions by Momentum Redirection.

Superhydrophobic surfaces can dramatically reduce the transport of mass or energy from impacting droplets by making them bounce off. Such transport processes are dependent on both the contact time and the contact area between the drop and the surface. To reduce transport, recent studies have focused on reducing the contact time. However, the contact area, which is dictated by the conformal spreading of the droplet, remains large, thereby limiting the reduction in the overall transport. Here, we show how surfaces can be designed to redirect the momentum of the spreading lamella causing it to lift off into 3-dimensional shapes, thereby dramatically reducing the contact area. We design superhydrophobic surfaces with an in-plane discontinuity leading to the accumulation of vertical momentum resulting in the out-of-plane ejection of the lamella into water bowls. We demonstrate a 2-fold reduction in the heat transfer between a cold rain and a warm surface. These insights can be broadly applied to other transport phenomena involving mass and energy exchange to limit heat loss under precipitation, icing of surfaces, reduce salt deposition on a surface exposed to ocean spray, or inhibit the formation of a water film on wings or wind turbine blades.