Static and dynamic behavior of the liquid- vapor interface during weightlessness
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LIQUID-VAPOR INTERFACE↗
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In Situ Monitoring the Nucleation and Growth of Nanoscale CaCO 3 at the Oil–Water Interface
Interfaces can actively control the nucleation kinetics, orientations, and polymorphs of calcium carbonate (CaCO 3 ). Prior studies have revealed that CaCO 3 formation can be affected by the interplay between chemical functional moieties on solid–liquid or air–liquid interfaces as well as CaCO 3 ’s precursors and facets. Yet little is known about the roles of a liquid–liquid interface, specifically an oil–liquid interface, in directing CaCO 3 mineralization which are common in natural and engineered systems. Here, in this study, by using in situ X-ray scattering techniques to locate a meniscus formed between water and a representative oil, isooctane, we successfully monitored CaCO 3 formation at the pliable isooctane–water interface and systematically investigated the pivotal roles of the interface in the formation of CaCO 3 (i.e., particle size, its spatial distribution with respect to the interface, and its mineral phase). Different from bulk solution, ∼5 nm CaCO 3 nanoparticles form at the isooctane–water interface. They stably exist for a long time (36 h), which can result from interface-stabilized dehydrated prenucleation clusters of CaCO 3 . There is a clear tendency for enhanced amounts and faster crystallization of CaCO 3 at locations closer to isooctane, which is attributed to a higher pH and an easier dehydration environment created by the interface and oil. Our study provides insights into CaCO 3 nucleation at an oil–water interface, which can deepen our understanding of pliable interfaces interacting with CaCO 3 and benefit mineral scaling control during energy-related subsurface operation.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Nonequilibrium study of the intrinsic free-energy profile across a liquid-vapour interface
We calculate an atomistically detailed free-energy profile across a heterogeneous system using a nonequilibrium approach. The path-integral formulation of Crooks fluctuation theorem is used in conjunction with the intrinsic sampling method to calculate the free-energy profile for the liquid-vapour interface of the Lennard-Jones fluid. Free-energy barriers are found corresponding to the atomic layering in the liquid phase as well as a barrier associated with the presence of an adsorbed layer as revealed by the intrinsic density profile. Our findings are in agreement with profiles calculated using Widom’s potential distribution theorem applied to both the average and the intrinsic profiles as well as the literature values for the excess chemical potential.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
An atomistic model for the thermal resistance of a liquid–solid interface
The thermal resistance associated with the interface between a solid and a liquid is analysed from an atomistic point of view. Partial evaluation of the associated Green–Kubo integral elucidates the various factors governing heat transport across the interface and leads to a quantitative model for the thermal resistance in terms of atomistic-level system parameters. The model is validated using molecular dynamics simulations.
Mechanics↗
Possible fossil H2O liquid-ice interfaces in the Martian crust
The extensive chaotic and fretted terrains in the equatorial regions of Mars are explained on the basis of the vertical distribution of H2O liquid and ice which once existed in the crust. This account assumes that below the permafrost containing water ice, there was a second zone in which liquid water resided for at least a time. Diagenetic alteration and cementation characterized the material in the subpermafrost zone; above, pristine fragmented material with various ice concentrations was found. Later, the ice-laden zone was stripped away by a number of erosional processes, exposing the former ice-liquid water interface.
Soderblom, L. A.↗
First-order wetting transition at a liquid-vapor interface
Evidence from reflectance and contact angle measurements is presented that three-phase mixtures of i-C3H7OH-C7F14 exhibit a first-order wetting phase transition at the liquid-vapor interface at 38 C. Equilibration phenomena support this interpretation. Ellipsometry was used to measure the apparent thickness of the intruding layer in the three-phase mixture. At temperatures slightly above the wetting temperature T(w), the intruding layer's thickness is several hundred angstroms and its variation with temperature is extremely weak. Below T(w), three-phase contact can occur between the vapor and both the upper and lower liquid phases; one of the angles which characterizes this contact has a very simple temperature dependence. The thickness of the intruding layer, monitored as the solutions approached equilibrium, is found to depend quite weakly on the height spanned by the upper liquid phase in the vicinity of a first-order wetting transition.
Schmidt, J. W.↗
Molecular Threading: Mechanical Extraction, Stretching and Placement of DNA Molecules from a Liquid-Air Interface
We present “molecular threading”, a surface independent tip-based method for stretching and depositing single and double-stranded DNA molecules. DNA is stretched into air at a liquid-air interface, and can be subsequently deposited onto a dry substrate isolated from solution. The design of an apparatus used for molecular threading is presented, and fluorescence and electron microscopies are used to characterize the angular distribution, straightness, and reproducibility of stretched DNA deposited in arrays onto elastomeric surfaces and thin membranes. Molecular threading demonstrates high straightness and uniformity over length scales from nanometers to micrometers, and represents an alternative to existing DNA deposition and linearization methods. These results point towards scalable and high-throughput precision manipulation of single-molecule polymers.
59 BASIC BIOLOGICAL SCIENCES↗
Enhanced electro-osmosis in propylene carbonate salt solutions
Properties of solid–liquid interfaces and surface charge characteristics mediate ionic and molecular transport through porous systems, affecting many processes such as separations. Herein, we report experiments designed to probe the electrochemical properties of solid–liquid interfaces using a model system of a single polyethylene terephthalate (PET) pore in contact with aqueous and propylene carbonate solutions of LiClO 4 . First, the existence and polarity of surface charges were inferred from current–voltage curves recorded when a pore was placed in contact with a LiClO4 concentration gradient. Second, the electro-osmotic transport of uncharged polystyrene particles through the PET pore provided information on the polarity and the magnitude of the pore walls’ zeta potential. Our experiments show that the PET pores become effectively positively charged when in contact with LiClO 4 solutions in propylene carbonate, even though in aqueous LiClO 4 , the same pores are negatively charged. Additionally, the electro-osmotic velocity of the particles revealed a significantly higher magnitude of the positive zeta potential of the pores in propylene carbonate compared to the magnitude of the negative zeta potential in water. The presented methods of probing the properties of solid–liquid interfaces are expected to be applicable to a wide variety of solid and liquid systems.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Flight 1 technical report for experiment 74-37 contained polycrystalline solidification in low-G
A .005 M solution of fluorescein in cyclohexanol was directionally solidified in a standard 10 x 10 x 45mm UV silica cuvette, using a bottom thermoelectric chilling device. Progress of the experiment was monitored by time lapse photography. During flight (SPAR I) the camera malfunctioned and only one quarter of the expected data were collected. Comparison of flight and ground specimens indicated that: (1) The dark green layer observed ahead of the solid-liquid interface which is most likely the solute-enriched zone, appears to be wider in the flight specimen; (2) Parasitic nucleation ahead of the solid-liquid interface in the flight sample led to an irregularly shaped interface, smaller grain size, equiaxed grain morphology and a larger average macroscopic growth rate; (3) The formation of equiaxed grains ahead of the solid-liquid interface in the flight specimen may be attributed to ordered islands within the liquid, which survived remelting because of the low degree of superheating (approximately equal to 1.5 C), did not settle because of reduced gravity and acted as nuclei during cooling.
Papaziak, J. M.↗
Matching time and spatial scales of rapid solidification: Dynamic TEM experiments coupled to CALPHAD-informed phase-field simulations
A combination of dynamic transmission electron microscopy (DTEM) experiments and CALPHAD-informed phase-field simulations was used to study rapid solidification in Cu–Ni thin-film alloys. Experiments—conducted in the DTEM—consisted of in situ laser melting and determination of the solidification kinetics by monitoring the solid–liquid interface and the overall microstructure evolution (time-resolved measurements) during the solidification process. Modelling of the Cu–Ni alloy microstructure evolution was based on a phase-field model that included realistic Gibbs energies and diffusion coefficients from the CALPHAD framework (thermodynamic and mobility databases). DTEM and post mortem experiments highlighted the formation of microsegregation-free columnar grains with interface velocities varying from ~0.1 to ~0.6 m s –1 . After an 'incubation' time, the velocity of the planar solid–liquid interface accelerated until solidification was complete. In addition, a decrease of the temperature gradient induced a decrease in the interface velocity. The modelling strategy permitted the simulation (in 1D and 2D) of the solidification process from the initially diffusion-controlled to the nearly partitionless regimes. Lastly, results of DTEM experiments and phase-field simulations (grain morphology, solute distribution, and solid–liquid interface velocity) were consistent at similar time (μs) and spatial scales (μm).
36 MATERIALS SCIENCE↗
Molecular beam scattering from flat jets of liquid dodecane and water
Abstract Molecular beam experiments in which gas molecules are scattered from liquids provide detailed, microscopic perspectives on the gas–liquid interface. Extending these methods to volatile liquids while maintaining the ability to measure product energy and angular distributions presents a significant challenge. The incorporation of flat liquid jets into molecular beam scattering experiments in our laboratory has allowed us to demonstrate their utility in uncovering dynamics in this complex chemical environment. Here, we summarize recent work on the evaporation and scattering of Ne, CD 4 , ND 3 , and D 2 O from a dodecane flat liquid jet and present first results on the evaporation and scattering of Ar from a cold salty water jet. In the evaporation experiments, Maxwell–Boltzmann flux distributions with a cos θ angular distribution are observed. Scattering experiments reveal both impulsive scattering (IS) and trapping followed by thermal desorption (TD). Super‐specular scattering is observed for all four species scattered from dodecane and is attributed to anisotropic momentum transfer to the liquid surface. In the IS channel, rotational excitation of the polyatomic scatterers is a significant energy sink, and these species accommodate more readily on the dodecane surface compared to Ne. Our preliminary results on cold salty water jets suggest that Ar atoms undergo some vapor‐phase collisions when evaporating from the liquid surface. Initial scattering experiments characterize the mechanisms of Ar interacting with an aqueous jet, allowing for comparison to dodecane systems. Key Points Molecular beam scattering from flat liquid jets is a powerful technique to elucidate mechanistic detail at the gas–liquid interface. Previous dodecane scattering experiments have uncovered angularly‐resolved thermal desorption fractions and energy transfer at the interface for several small molecule scatterers. Preliminary results on scattering from cold salty water reveal mechanisms of interaction between argon and an aqueous jet.
Yang, Walt↗
Validation of Ullage Collapse Due to Violent Lateral Slosh
Understanding the coupling between thermodynamics and propellant sloshing is important for cryogenic upper stages, especially during the lift-off phase and in missions including multiple engine restarts, as the fluid dynamic condition of the propellant is mainly influenced by various flight maneuvers. This paper describes the development and validation of a Volume of Fluid (VOF)-based CFD solver, Loci/STREAM-VOF, to the ullage collapse under violent later slosh conditions. Loci/STREAM-VOF is shown to be able to capture detailed slosh dynamics, including slosh frequency, non-linear slosh damping, and violent surface breakup due to forced acceleration. The comparison of surface shape and small drops formed during large amplitude slosh with experimental imagery shows excellent agreement throughout the sloshing period. Comparison of temperature histories in the ullage, at the gas-liquid interface, and inside liquid with the experiment conducted at JAXA also show very good agreement. The simulation points to a stratified temperature field inside the liquid near the interface, critical to the ullage pressure after the collapse. The predicted pressure collapse matches well with the experimental value due to sloshing. Parametric sensitivity studies suggest that high-fidelity Loci/STREM-VOF simulations can play an essential role in predicting the actual thermodynamics of ullage collapse when following the recommended simulation methodology.
H Q Yang↗
Disruption of an Aligned Dendritic Network by Bubbles During Re-Melting in a Microgravity Environment
The quiescent Microgravity environment can be quite dynamic. Thermocapillary flow about "large" static bubbles on the order of 1mm in diameter was easily observed by following smaller tracer bubbles. The bubble induced flow was seen to disrupt a large dendritic array, effectively distributing free branches about the solid-liquid interface. "Small" dynamic bubbles were observed to travel at fast velocities through the mushy zone with the implication of bringing/detaching/redistributing dendrite arm fragments at the solid-liquid interface. Large and small bubbles effectively re-orient/re-distribute dendrite branches/arms/fragments at the solid liquid interface. Subsequent initiation of controlled directional solidification results in growth of dendrites having random orientations which significantly compromises the desired science.
Grugel, Richard N.↗
Bubble formation and growth - Study of the boundary conditions at a liquid-vapor interface through irreversible thermodynamics Final report, Feb. 1966 - Feb. 1967
Irreversible thermodynamics of liquid-vapor phase change process
PHASE CHANGE↗
Processing eutectics in space
Experimental work is reported which was directed toward obtaining interface shape control while a numerical thermal analysis program was being made operational. An experimental system was developed in which the solid-liquid interface in a directionally solidified aluminum-nickel eutectic could be made either concave to the melt or convex to the melt. This experimental system provides control over the solid-liquid interface shape and can be used to study the effect of such control on the microstructure. The SINDA thermal analysis program, obtained from Marshall Space Flight Center, was used to evaluate experimental directional solidification systems for the aluminum-nickel and the aluminum-copper eutectics. This program was applied to a three-dimensional ingot, and was used to calculate the thermal profiles in axisymmetric heat flow. The results show that solid-liquid interface shape control can be attained with physically realizable thermal configurations and the magnitudes of the required thermal inputs were indicated.
Douglas, F. C.↗
Active colloidal particles at fluid-fluid interfaces
Here this review explores the intersection between two important fields of colloid and interface science – that of active colloidal particles and of (passive) particles at fluid-fluid interfaces. The former uses energy input at the particle level to propel particle motions and direct dynamic assemblies. The latter relies on the spontaneous adsorption of particles at fluid interfaces to modify the interfacial energy, rheology, and permeability of biphasic materials. Here, we address two key questions that connect these otherwise distinct fields of study. How do liquid interfaces influence the dynamics of active or driven colloidal particles? How can particle activity influence the dynamics of liquid interfaces? These questions motivate the pursuit of active particle surfactants that move and organize at fluid interfaces to perform useful functions such as enhancing mass transport or modulating interfacial properties. Drawing examples from the literature, we discuss how fluid interfaces can provide a unique environment for the study of active colloids, how surface tension can be harnessed to propel particle motions, and how capillary interactions can be activated to achieve dynamically tunable emulsions and foams. We highlight opportunities for the future study and application of active particles at liquid interfaces.
42 ENGINEERING↗
Preface to “From Coadsorption and Catalysis at Solid Surfaces to Liquid–Solid Interfaces in Theory and Experiment, Published in Honor of Professor Robert K. Grasselli, Irsee IX Symposium Kloster Irsee, Germany 16–19 June 2022 (Irsee IX)”
The 9th Irsee Symposium entitled “From Coadsorption and Catalysis at Solid Surfaces to Liquid–Solid Interfaces in Theory and Experiment”, sponsored by the Robert Karl Grasselli Foundation, took place at its traditional venue, the Schwäbisches Bildungszentrum in Irsee, Germany, on 16–19 June 2022. In the Irsee Symposium, selected experts gather every few years to discuss recent progress, challenges, new directions, and frontiers in catalysis. Furthermore, after the moratorium imposed on us by Covid-19, all the participants especially enjoyed the lively meeting and face-to-face interactions.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Role of adsorption in liquid lubrication
Changes at solid-liquid interfaces caused by adsorption from solution are discussed paying attention to the following aspects: (1) stability of adsorbed films and the structure of metal-additive-film-liquid interface and effect of adsorbate orientation. (2) chemical versus physical adsorption, (3) heat of adsorption, (4) adsorption of additives, (5) activated adsorption, effect of activating adsorbates, (6) displacement phenomena at solid-liquid interfaces, (7) competition of antiwear additives, their solvents, and water, (8) effect of adsorption on the orientation of liquid in the interfacial region, and (9) relation between the chemical nature of solid surfaces and their interaction with liquid lubricants. The relevance of the above adsorption phenomena to lubrication is discussed, referring where possible to specific examples.
Groszek, A. J.↗