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The effect of surface contamination on contact angles and surface potentials Summary report
Surface contamination effects on behavior of liquids in space vehicle tanks at zero gravity
Effect of contact angle on rolling-element fatigue life with a fluorinated ether lubricant at a cryogenic temperature of 170 K /305 deg R/
Test of rolling element fatigue life with fluorinated ether lubricant at cryogenic temperature using five ball fatigue tester
Contact Angle Influence on Geysering Jets in Microgravity Investigated
Microgravity poses many challenges to the designer of spacecraft tanks. Chief among these are the lack of phase separation and the need to supply vapor-free liquid or liquid-free vapor to the spacecraft processes that require fluid. One of the principal problems of phase separation is the creation of liquid jets. A jet can be created by liquid filling, settling of the fluid to one end of the tank, or even closing a valve to stop the liquid flow. Anyone who has seen a fountain knows that jets occur in normal gravity also. However, in normal gravity, the gravity controls and restricts the jet flow. In microgravity, with gravity largely absent, surface tension forces must be used to contain jets. To model this phenomenon, a numerical method that tracks the fluid motion and the surface tension forces is required. Jacqmin has developed a phase model that converts the discrete surface tension force into a barrier function that peaks at the free surface and decays rapidly away. Previous attempts at this formulation were criticized for smearing the interface. This can be overcome by sharpening the phase function, double gridding the fluid function, and using a higher-order solution for the fluid function. The solution of this equation can be rewritten as two coupled Poisson equations that also include the velocity.
The determination of equivalent bearing loading for the BSMT that simulate SSME high pressure oxidizer turbopump conditions using the SHABERTH/SINDA computer programs
The MSFC bearing seal material tester (BSMT) can be used to evaluate the SSME high pressure oxygen turbopump (HPOTP) bearing performance. The four HPOTP bearings have both an imposed radial and axial load. These radial and axial loads are caused by the HPOTP's shaft, main impeller, preburner impeller, turbine and by the LOX coolant flow through the bearings, respectively. These loads coupled with bearing geometry and operating speed can define bearing contact angle, contact Hertz stress, and heat generation rates. The BSMT has the capability of operating at HPOTP shaft speeds, provide proper coolant flowrates but can only apply an axial load. Due to the inability to operate the bearings in the BSMT with an applied radial load, it is important to develop an equivalency between the applied axial loads and the actual HPOTP loadings. A shaft-bearing-thermal computer code (SHABERTH/SINDA) is used to simulate the BSMT bearing-shaft geometry and thermal-fluid operating conditions.
Motion of Drops on Surfaces with Wettability Gradients
A liquid drop present on a solid surface can move because of a gradient in wettability along the surface, as manifested by a gradient in the contact angle. The contact angle at a given point on the contact line between a solid and a liquid in a gaseous medium is the angle between the tangent planes to the liquid and the solid surfaces at that point and is measured within the liquid side, by convention. The motion of the drop occurs in the direction of increasing wettability. The cause of the motion is the net force exerted on the drop by the solid surface because of the variation of the contact angle around the periphery. This force causes acceleration of an initially stationary drop, and leads to its motion in the direction of decreasing contact angle. The nature of the motion is determined by the balance between the motivating force and the resisting hydrodynamic force from the solid surface and the surrounding gaseous medium. A wettability gradient can be chemically induced as shown by Chaudhury and Whitesides who provided unambiguous experimental evidence that drops can move in such gradients. The phenomenon can be important in heat transfer applications in low gravity, such as when condensation occurs on a surface. Daniel et al have demonstrated that the velocity of a drop on a surface due to a wettability gradient in the presence of condensation can be more than two orders of magnitude larger than that observed in the absence of condensation. In the present research program, we have begun to study the motion of a drop in a wettability gradient systematically using a model system. Our initial efforts will be restricted to a system in which no condensation occurs. The experiments are performed as follows. First, a rectangular strip of approximate dimensions 10 x 20 mm is cut out of a silicon wafer. The strip is cleaned thoroughly and its surface is exposed to the vapor from an alkylchlorosilane for a period lasting between one and two minutes inside a desiccator. This is done using an approximate line source of the vapor in the form of a string soaked in the alkylchlorosilane. Ordinarily, many fluids, including water, wet the surface of silicon quite well. This means that the contact angle is small. But the silanized surface resists wetting, with contact angles that are as large as 100 degs. Therefore, a gradient of wettability is formed on the silicon surface. The region near the string is highly hydrophobic, and the contact angle decreases gradually toward a small value at the hydrophilic end away from this region. The change in wettability occurs over a distance of several mm. The strip is placed on a platform within a Plexiglas cell. Drops of a suitable liquid are introduced on top of the strip near the hydrophobic end. An optical system attached to a video camera is trained on the drop so that images of the moving drop can be captured on videotape for subsequent analysis. We have performed preliminary experiments with water as well as ethylene glycol drops. Results from these experiments will be presented in the poster. Future plans include the refinement of the experimental system so as to permit images to be recorded from the side as well as the top, and the conduct of a systematic study in which the drop size is varied over a good range. Experiments will be conducted with different fluids so as to obtain the largest possible range of suitably defined Reynolds and Capillary numbers. Also, an effort will be initiated on theoretical modeling of this motion. The challenges in the development of the theoretical description lie in the proper analysis of the region in the vicinity of the contact line, as well as in the free boundary nature of the problem. It is known that continuum models assuming the no slip condition all the way to the contact line fail by predicting that the stress on the solid surface becomes singular as the contact line is approached. One approach for dealing with this issue has been to relax the no-slip boundary condition using the Navier model. Molecular dynamics simulations of the contact line region show that for a non-polar liquid on a solid surface, the no-slip boundary condition is in fact incorrect near the contact line. Furthermore, the same simulations also show that the usual relationship between stress and the rate of deformation breaks down in the vicinity of the contact line. In developing continuum theoretical models of the system, we shall accommodate this knowledge to the extent possible.
A Study on Surface Texture and Wettability of Femtosecond Laser Treated Aluminum Alloys
This research aims to study the effects of femtosecond laser treatment on surface texture and wettability properties. The first portion of this research studies 2024-T3 aluminum alloy concerning surface texture (e.g., roughness), wettability, and surface free energy. SEM images help aid the researchers in detecting minuscule changes in surface texture. Profilometry extracts topographical data from the surface. A contact angle goniometer measures contact angle, which follows the sessile drop method. Owens, Wendt, Rabel, and Kaelble's method calculates the surface free energy in conjunction with the contact angle. Femtosecond laser modification produces relatively uniform surface morphology at the macroscale. When looking at the microscale, surface morphology differs depending on the interplay between material melting and self-assembly, where the surface becomes rougher after laser treatment. Contact angle results show that all but the control sample and sample 7 exhibit hydrophobic behavior, i.e., contact angle >90°, with Sample 1 having the most significant angle of 115°. The effects of laser parameters on surface energy is apparent. More work is needed to establish correlations among these three quantities: contact angle, surface energy, and laser parameters. The second portion of this research studies aluminum alloy 6061 as the subject material with the primary goal of creating a superhydrophobic surface. A central composite design creates the laser surface texturing design of experiments. SEM images help aid the researchers in detecting minuscule changes in surface texture. A 3D optical profiler extracts topographical data from the surface. The sessile drop method incorporates a contact angle goniometer to measure the contact angle. The response surface method builds a second-order polynomial model for the contact angle and obtains optimized parameters to maximize the contact angle. This research shows that laser surface texturing can generate a wide range of surface profiles and roughness values with geometric features ranging from hundreds of μm to submicron. All three laser parameters (pulse energy, pulse duration, repetition rate) affect surface roughness and contact angle to some degree. To quantify the relationship between the contact angle, pulse energy, and pulse repetition rate, a response surface model for Al 6061 is identified and used to find the optimal conditions of E=214 μJ, tp=10 ps, and fp=2427 Hz with a predicted maximum contact angle of 161°. A confirmation experiment produces a contact angle of 168°, in good agreement with the predicted value.
Direct Numerical Simulation of Wetting and Spreading Behavior on Heterogeneous and Roughened Substrates
A method of calculation is presented that allows the simulation of the time-dependent three-dimensional motion of thin liquid layers on solid substrates for systems with finite equilibrium contact angles. The contact angle is a prescribed function of position on the substrate. Similar mathematical models are constructed for substrates with a pattern of roughness. Evolution equations are given, using the lubrication approximation, that include viscous, capillary and disjoining forces. Motion to and from dry substrate regions is made possible by use of a thin energetically-stable wetting layer. We simulate motion on heterogeneous substrates with periodic arrays of high contact-angle patches. Two different problems are treated for heterogenous substrates. The first is spontaneous motion driven only by wetting forces. If the contact-angle difference is sufficiently high, the droplet can find several different stable positions, depending on the previous history of the motion. A second simulation treats a forced cyclical motion. Energy dissipation per cycle for a heterogeneous substrate is found to be larger than for a uniform substrate with the same total energy. The Landau-Levich solution for plate removal from a liquid bath is extended to account for a pattern of roughness on the plate.
Further studies of propellant sloshing under low-gravity conditions
A variational integral is formulated from Hamilton's Principle and is proved to be equivalent to the usual differential equations of low-gravity sloshing in ellipsoidal tanks. It is shown that for a zero-degree contact angle the contact line boundary condition corresponds to the stuck condition, a result that is due to the linearization of the equations and the ambiguity in the definition of the wave height at the wall. The variational integral is solved by a Rayleigh-Ritz technique. Results for slosh frequency when the free surface is not bent-over compare well with previous numerical solutions. When the free surface is bent over, however, the results for slosh frequency are considerably larger than those predicted by previous finite-difference, numerical approaches: the difference may be caused by the use of a zero degree contact angle in the present theory in contrast to the nonzero contact angle used in the numerical approaches.
Dynamic condensation model of rolling droplets for high-performance heat transfer
Condensation is a critical process during vapor-liquid phase change in relation to heat transfer. To achieve a high heat transfer coefficient, the classical model for dropwise condensation requires a low contact angle and low contact angle hysteresis, failing to align with experimental observations on a hydrophobic and slippery quasi-liquid surface (QLS). Here, we report a dynamic condensation model that incorporates high-frequency condensate removal by emphasizing the role of timescale during droplet growth and shedding. Our model agrees well with the experimental result that a surface with high contact angle and low contact angle hysteresis promotes condensation, particularly during rolling-propelled condensate removal. Particle image velocimetry reveals that rolling droplets on a hydrophobic QLS exhibit 4-fold higher shedding speeds than the sliding droplets on a hydrophilic QLS, leading to significant heat transfer enhancement. This work deepens our theoretical understanding of condensation heat transfer and provides advanced physics-informed design rationales for water and energy systems.
Predictive numerical modeling of plasma-induced surface roughness and wettability evolution in LM-PAEK/CF tape
Plasma surface modification effectively enhances adhesion in thermoplastic composites, yet its impacts on high-performance polymers like low-melting polyaryletherketone (LM-PAEK) remain inadequately quantified. Here, this study integrates experimental analysis and numerical modeling to characterize surface roughness and wettability changes in LM-PAEK/carbon fiber composites treated with atmospheric plasma. Atomic Force Microscopy quantified surface topography (n = 10 per condition for contact angles), while static contact-angle assessments measured wettability. Roughness rapidly increased from ∼0.2 nm to 1.6 nm, and contact angle reduced from ∼90° to 24°, both stabilizing after 25–30 s of exposure. A semi-empirical, physics-informed framework was calibrated to these data, coupling surface chemistry via the Owens–Wendt decomposition with topography via the Wenzel roughness factor, and evaluated using out-of-sample (cross-validated) tests, while static contact angle assessments measured wettability. Numerical predictions matched experimental results closely (RMSE <5%, R 2 > 0.95). Incorporating material-specific parameters, the calibrated model supports plasma-treatment optimization and provides quantitative guidance for improving interfacial adhesion in thermoplastic composite manufacturing.
Residual Gas Effects on Detached Solidification in Microgravity
Many microgravity directional solidification experiments yielded ingots with portions that grew without contacting the ampoule wall, leading to greatly improved crystallographic perfection. Our long-term goal is to make such detached solidification reproducible, which requires a full understanding of the mechanisms underlying it. Our Moving Meniscus Model of steady-state detachment predicts that it depends strongly on the surface tension of the melt and the advancing contact angle with the ampoule wall. Detached solidification is more likely when the contact angle for the melt on the ampoule wall is high, i.e. non-wetting. It has been claimed that impurities increase the contact angle. The objective of the current project is to determine the influence of residual gases on the surface tension and contact angle of molten semiconductors on typical ampoule materials. We are focusing on determining the influence of oxygen on the contact angle of molten InSb on clean silica ('quartz'), including the advancing and retreating contact angles in addition to the usual equilibrium contact angle. We have created a gas flow system that allows us to control the oxygen partial pressure over a sessile drop of InSb on a horizontal quartz surface. The cell is slowly tilted while videotaping to reveal the contact angles on the two sides of the drop just prior to it rolling down the surface. Thus far, we have learned the following: (1) Molten InSb readily forms an oxide layer in the presence of the trace amounts of oxygen found in high purity argon; (2) This oxide contains a substantial amount of Ga, which presumably is a trace contaminant that is not detectable in the starting material; (3) The addition of 10% hydrogen to the argon gas is sufficient to reduce the oxide and produce a clean drop; (4) An infrared filter must precede the video camera in order to produce a sharp image of the drop for later image analysis; (5) Tilting the surface on which the drop rests causes the two sides of the drop to display different contact angles, reflecting contact line sticking; (6) Vibration strongly accelerates the approach of the drop to its final shape on a horizontal surface by helping to overcome sticking of the contact line; (7) Oscillation of the drop surface due to vibration appears to increase as the surface is inclined from horizontal. Presumably, the angle at which the drop rolls down the surface is also reduced by vibration. This observation is particularly significant, as the meniscus must move along the ampoule wall during detached solidification.
An augmented Young-Laplace model of an evaporating meniscus in a micro-channel with high heat flux
High flux evaporations from a steady meniscus formed in a 2 micron channel is modeled using the augmented Young-Laplace equation. The heat flux is found to be a function of the long range van der Waals dispersion force which represents interfacial conditions between heptane and various substrates. Heat fluxes of (1.3-1.6) x 10(exp 6) W/m(exp 2) based on the width of the channel are obtained for heptane completely wetting the substrate at 100 C. Small channels are used to obtain these large fluxes. Even though the real contact angle is 0 deg, the apparent contact angle is found to vary between 24.8 deg and 25.6 deg. The apparent contact angle, which represents viscous losses near the contact line, has a large effect on the heat flow rate because of its effect on capillary suction and the area of the meniscus. The interfacial heat flux is modeled using kinetic theory for the evaporation rate. The superheated state depends on the temperature and the pressure of the liquid phase. The liquid pressure differs from the pressure of the vapor phase due to capillarity and long range van der Waals dispersion forces which are relevant in the ultra think film formed at the leading edge of the meniscus. Important pressure gradients in the thin film cause a substantial apparent contact angle for a complete wetting system. The temperature of the liquid is related to the evaporation rate and to the substrate temperature through the steady heat conduction equation. Conduction in the liquid phase is calculated using finite element analysis except in the vicinity of the thin film. A lubrication theory solution for the thin film is combined with the finite element analysis by the method of matched asymptotic expansions.
Low-Energy Ion Scattering Intensities from Supported Nanoparticles: The Spherical Cap Model
Supported nanoparticles are of great importance to many technologies like fuel processing and chemical synthesis using catalysts and electrocatalysts, energy storage and generation using fuel cells and batteries, electrochemistry, magnetic information storage, and more. Low-energy ion scattering spectroscopy (LEIS) with noble gas ions like He+ is a powerful tool for the characterization of nanoparticles dispersed across flat support surfaces due to its ability to probe the elemental composition in the topmost atomic layer of a surface, providing quantitative information regarding the size and number density of nanoparticles. In this work, we present a derivation of the LEIS intensities expected from nanoparticles and the support material as a function of the average particle size, their number per unit area, and their contact angle with the support when modeled as spherical caps of the nanoparticle material dispersed over the surface of a flat support. The model assumes that the ion intensities are determined only by the physical blocking of linear ion trajectories and independent of the tilt angle of the local surface relative to the incident and scattered ion directions, an assumption we support by quantitative modeling of published data which tested tilt-angle effects. The model is a generalization to arbitrary contact angles of the hemispherical cap model, which assumes 90° contact angle and has been widely used to model spectroscopic signals in LEIS (and also in Auger and photoelectron spectroscopies) during nanoparticle growth. Here, this new model quantitatively reveals how LEIS signals are sensitive not only to the diameter and number density of the nanoparticle but also to their contact angle (or height/diameter ratio). With the use of additional data (e.g., from microscopy or adsorption microcalorimetry), the model presented here will enable more accurate determination of the average size, shape, and number density of supported nanoparticles based on LEIS intensity measurements.
Modulating Interactions between Molten Polystyrene and Porous Solids Using Atomic Layer Deposition
Understanding and modulating the interactions between molten polymers and porous solids is important for numerous processes and phenomena including catalytic conversion of polymers and fabrication of nanocomposites and nanostructured materials. Although changing the surface composition of pores would enable modulation of interactions between polymer and nanoporous solids, it is challenging to achieve such a control without inducing significant changes to the size and structure of nanopores. In this work, we demonstrate that the interactions between molten polystyrene (PS) and disordered packings of SiO 2 nanoparticles (NPs) can be modulated by changing the surface composition of the NPs using atomic layer deposition (ALD). A disordered packing of silica NPs is modified with varying surface coverages of TiO 2 , WO 3 and CaCO 3 , with coverages estimated by the mass gain and the refractive index change of NP packings. Based on the time required to fully infiltrate these ALD-modified NP packings via capillarity, the contact angles for PS on different surfaces prepared via ALD are determined. The contact angle gradually changes from that of pure SiO 2 to that of the fully covered surfaces. The contact angles for PS on SiO 2 , TiO 2 , WO 3 and CaCO 3 are found to be 20°, 62°, 70° and 10°, respectively. Interestingly, the contact angles and interfacial energies between PS and the ALD-modified surfaces do not correlate strongly with the water contact angle of these surfaces; thus, caution must be exercised in predicting how a polymer would wet or interact with porous solids solely based on their hydrophilicity. Furthermore, the method presented in this work can be extended to study the interactions between a wide range of polymers and surfaces in porous media, which will have important implications for designing new catalytic materials for polymer upcycling reactions as well as novel NP-polymer composite films and membranes with enhanced mechanical and transport properties.
Calorimetric Energies and Chemical Potentials of Metal Atoms in Catalytic Nanoparticles on Oxide and Carbon Supports: Improved Size Dependencies and Adhesion Energies
The chemical potential of metal atoms, μM, in supported metal nanoparticles is an important descriptor related to both the catalytic activity and the stability of the nanoparticles. Here, we derive an expression relating μM to the radius of the particle’s contact area with the support and the adhesion energy at the metal/support interface (E adh ) that assumes the particles have the shape of spherical caps but of arbitrary contact angle with the support (θ c ) and includes an empirical correction for the increase in metal surface energy and adhesion energy with decreasing radius of curvature. We then show that, at any assumed contact angle, we can simultaneously fit previously reported measurements of both calorimetric μ M (from heats of metal vapor adsorption during nanoparticle growth by vapor deposition) versus metal coverage data and the He + low-energy ion scattering (LEIS) intensities for the metal and/or support versus metal coverage (using our recently developed spherical cap model for quantitative LEIS intensities), to determine the particle size versus coverage and E adh . Only one choice of contact angle gives a pair of values for contact angle and E adh , which is consistent with the Young–Dupré equation for the equilibrium shape of a spherical particle. At this equilibrium shape, we then applied this spherical cap model (SCM) to reanalyze microcalorimetric metal chemical potentials and LEIS signals versus coverage data for nine metal/support combinations that were previously analyzed by assuming that the particles had the shape of hemispherical caps, i.e., with a contact angle of 90°. We show that this revised approach gives close agreement with the calorimetric and LEIS data; the best-fit contact angles vary from 64 to 84°, correcting the earlier assumption of 90°. Furthermore, these results provide significant accuracy improvements in particle size versus coverage, metal chemical potential versus size and coverage, metal/support adhesion energies and contact angles for Cu, Ag and Au on CeO 2 (111), Ni on MgO(100), Ag on Fe 3 O 4 (111) and TiO 2 (100), and Ag, Ni and Pd on Ni-supported graphene. This revised approach is much more broadly applicable than the earlier hemispherical cap model (HCM).
Capillary Driven Flows Along Differentially Wetted Interior Corners
Closed-form analytic solutions useful for the design of capillary flows in a variety of containers possessing interior corners were recently collected and reviewed. Low-g drop tower and aircraft experiments performed at NASA to date show excellent agreement between theory and experiment for perfectly wetting fluids. The analytical expressions are general in terms of contact angle, but do not account for variations in contact angle between the various surfaces within the system. Such conditions may be desirable for capillary containment or to compute the behavior of capillary corner flows in containers consisting of different materials with widely varying wetting characteristics. A simple coordinate rotation is employed to recast the governing system of equations for flows in containers with interior corners with differing contact angles on the faces of the corner. The result is that a large number of capillary driven corner flows may be predicted with only slightly modified geometric functions dependent on corner angle and the two (or more) contact angles of the system. A numerical solution is employed to verify the new problem formulation. The benchmarked computations support the use of the existing theoretical approach to geometries with variable wettability. Simple experiments to confirm the theoretical findings are recommended. Favorable agreement between such experiments and the present theory may argue well for the extension of the analytic results to predict fluid performance in future large length scale capillary fluid systems for spacecraft as well as for small scale capillary systems on Earth.
Activity-induced migration of viscous droplets on a solid substrate
Active matter exploits motion to induce changes in shape and conformation via external input. Here, in this paper, we establish theoretically that viscous liquid droplets containing magnetic nanoparticles with frozen-in magnetic moments, sitting on a solid substrate and surrounded by an ambient gas phase, can deform and migrate under the influence of a magnetic torque. The effect arises because the collective rotation of the magnetic nanoparticles at the liquid–gas interface tilts the droplet away from a symmetric configuration, breaks the reflection symmetry with respect to the centre axis, and leads to a left–right asymmetry of the contact angles. A sufficiently strong magnetic torque leads the contact angles to overcome hysteresis effects leading the droplet to migrate. We develop a general framework to explain how symmetry-breaking affects droplet migration. Thus previous results of droplet spreading and migration can be recovered as special cases. Such droplets can be employed as agents in active surfaces and can move against gravity, chemical and thermal gradients, providing a mechanism that could be utilized by both industry and medicine.