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An improved direct liquid-feed fuel cell having a solid membrane electrolyte for electrochemical reactions of an organic fuel. Improvements in interfacing of the catalyst layer and the membrane and activating catalyst materials are disclosed.
A method was evaluated to measure the liquid-gas and the liquid-slush interfaces in two-phase cryogen systems using optical means. This method makes use of the attenuation of a directed light beam caused by the difference in the index of refraction between the solid particles and the surrounding liquid. Preliminary experimental results obtained in slush nitrogen are shown. The possibility of extending this technique to include a measure of solid fraction is also discussed.
Karma and Rapped recently developed a new sharp interface asymptotic analysis of the phase-field equations that is especially appropriate for modeling dendritic growth at low undercoolings. Their approach relieves a stringent restriction on the interface thickness that applies in the conventional asymptotic analysis, and has the added advantage that interfacial kinetic effects can also be eliminated. However, their analysis focussed on the case of equal thermal conductivities in the solid and liquid phases; when applied to a standard phase-field model with unequal conductivities, anomalous terms arise in the limiting forms of the boundary conditions for the interfacial temperature that are not present in conventional sharp-interface solidification models, as discussed further by Almgren. In this paper we apply their asymptotic methodology to a generalized phase-field model which is derived using a thermodynamically consistent approach that is based on independent entropy and internal energy gradient functionals that include double wells in both the entropy and internal energy densities. The additional degrees of freedom associated with the generalized phased-field equations can be chosen to eliminate the anomalous terms that arise for unequal conductivities.
In eutectic growth, as the solid phases grow they reject atoms to the liquid. This results in a variation of melt composition along the solid/liquid interface. In the past, mass transfer in eutectic solidification, in the absence of convection, was considered to be governed only by the diffusion induced by compositional gradients. However, mass transfer can also be generated by a temperature gradient. This is called thermotransport, thermomigration, thermal diffusion or the Soret effect. A theoretical model of the influence of the Soret effect on the growth of eutectic alloys is presented. A differential equation describing the compositional field near the interface during unidirectional solidification of a binary eutectic alloy was formulated by including the contributions of both compositional and thermal gradients in the liquid. A steady-state solution of the differential equation was obtained by applying appropriate boundary conditions and accounting for heat flow in the melt. Following that, the average interfacial composition was converted to a variation of undercooling at the interface, and consequently to microstructural parameters. The results obtained show that thermotransport can, under certain circumstances, be a parameter of paramount importance.
Magnetorheological (MR) suspensions are composed of colloidal particles which acquire dipole moments when subjected to an external magnetic field. At sufficient field strengths and concentrations, the dipolar particles rapidly aggregate to form long chains. Subsequent lateral cross-linking of the dipolar chains is responsible for a rapid liquid-to-solid-like rheological transition. The unique, magnetically-activated rheological properties of MR suspensions make them ideal for interfacing mechanical systems to electronic controls. Additionally, the ability to experimentally probe colloidal suspensions interacting through tunable anisotropic potentials is of fundamental interest. Our current experimental work has focused on understanding the fluctuations of dipolar chains. It has been proposed by Halsey and Toor (HT) that the strong Landau-Peierls thermal fluctuations of dipolar chains could be responsible for long-range attractions between chains. Such interactions will govern the long-time relaxation of MR suspensions. We have synthesized monodisperse neutrally buoyant MR suspensions by density matching stabilized ferrofluid emulsion droplets with D2O. This allows us to probe the dynamics of the dipolar chains using light scattering without gravitational, interfacial, and polydispersity effects to resolve the short-wavelength dynamics of the dipolar chains. We used diffusing wave spectroscopy to measure these dynamics. The particle displacements at short times that show an independence to the field strength, but at long times exhibit a constrained, sub-diffusive motion that slows as the dipole strength is increased. The experiments are in good qualitative agreement with Brownian dynamics simulations of dipolar chains. Although there have been several important and detailed studies of the structure and interactions in MR suspensions, there has not been conclusive evidence that supports or contradicts the HT model prediction that long-range interactions exist between fluctuating chains of dipolar particles. Resolving this issue would contribute greatly to the understanding of these interesting and important materials. We have begun to test the predictions of the HT model by both examining the dynamics of individual chains and by measuring the forces between dipolar chains directly to accurately and quantitatively assess the interactions that they experience. To do so, we employ optical trapping techniques and video-microscopy to manipulate and observe our samples on the microscopic level. With these techniques, it is possible to observe chains that are fluctuating freely in three-dimensions, independent of interfacial effects. More importantly, we are able to controllably observe the interactions of two chains at various separations to measure the force-distance profile. The techniques also allow us to study the mechanical properties of individual chains and chain clusters. Our work to this point has focused on reversibly-formed dipolar chains due to field induced dipoles where the combination of this chaining, the dipolar forces, and the hydrodynamic interactions that dictate the rheology of the suspensions. One can envision, however, many situations where optical, electronic, or rheological behavior may be optimized with magneto-responsive anisotropic particles. Chains of polarizable particles may have the best properties as they can coil and flex in the absence of a field and stiffen and orient when a field is applied. We have recently demonstrated a synthesis of stable, permanent paramagnetic chains by both covalently and physically linking paramagnetic colloidal particles. The method employed allows us to create monodisperse chains of controlled length. We observed the stability, field-alignment, and rigidity of this new class of materials. The chains may exhibit unique rheological properties in an applied magnetic field over isotropic suspensions of paramagnetic particles. They are also useful rheological models as bead-spring systems. These chains form the basis for our current experiments with optical traps.
In earlier investigations, Marangoni effects were observed to be the dominant mechanism of boiling transport in 2-propanol/water mixtures under reduced gravity conditions. In this investigation we have examined the mechanisms of binary mixture boiling by exploring the transport near a single bubble generated in a binary mixture between a heated surface and cold surface. The temperature field created in the liquid around the bubble produces vaporization over the portion of its interface near the heated surface and condensation over portions of its interface near the cold surface. Experiments were conducted using different mixtures of water and 2-propanol under 1g conditions and under reduced gravity conditions aboard the KC135 aircraft. Since 2-propanol is more volatile than water, there is a lower concentration of 2-propanol near the hot surface and a higher concentration of 2-propanol near the cold plate relative to the bulk quantity. This difference in interface concentration gives rise to strong Marangoni effects that move liquid toward the hot plate in the near bubble region for 2-propanol and water mixtures. In the experiments in this study, the pressure of the test system was maintained at about 5 kPa to achieve the full spectrum of boiling behavior (nucleate boiling, critical heat flux and film boiling) at low temperature and heat flux levels. Heat transfer data and visual documentation of the bubble shape were extracted from the experimental results. In the 1-g experiments at moderate to high heat flux levels, the bubble was observed to grow into a mushroom shape with a larger top portion near the cold plate due to the buoyancy effect. The shape of the bubble was somewhat affected by the cold plate subcooling and the superheat of the heated surface. At low superheat levels for the heated surface, several active nucleation sites were observed, and the vapor stems from them merged to form a larger bubble. The generation rate of vapor is moderate in this regime and the bubble shape is cylindrical in appearance. In some instances, the bubble interface appeared to oscillate. At higher applied heat flux levels, the top of the bubble became larger, apparently to provide more condensing interface area adjacent to the cold plate. Increasing the applied heat flux ultimately led to dry-out of the heated surface, with conditions just prior to dryout corresponding to the maximum heat flux (CHF). A more stable bubble was observed when the system attained the minimum heat flux (for film boiling). In this regime, most of the surface under the bottom of the bubble was dry with nucleate boiling sometimes occuring around the contact perimeter of the bubble at heated surface. Different variations (e.g. gap between two plates, molar concentration of the liquid mixture) of the experiments were examined to determine parametric effects on the boiling process and to determine the best conditions for the KC135 reduced gravity tests. Variation of the gap was found to have a minor impact on the CHF. However, reducing the gap between the hot and cold surface was observed to significantly reduce the minimum heat flux for fixed molar concentration of 2-propanol. In the reduced gravity experiments aboard the KC135 aircraft, the bubble formed in the 6.4 mm gap was generally cylindrical or barrel shaped and it increased its extent laterally as the surface superheat increased. In reduced gravity experiments, dryout of the heated surface under the bubble was observed to occur at a lower superheated temperature than for 1g conditions. Observed features of the boiling process and heat transfer data under reduced gravity will be discussed in detail. The results of the reduced gravity experiments will also be compared to those obtained in comparable 1g experiments. In tandem with the experiments we are also developing a computational model of the transport in the liquid surrounding the bubble during the boiling process. The computational model uses a level set method to model motion of the interface. It will incorporate a macroscale treatment of the transport in the liquid gap between the surfaces and a microscale treatment of transport in the regions between the bubble interface and the solid surfaces. The features of the model will be described in detail. Future research directions suggested by the results to date will also be discussed.
An improved direct liquid-feed fuel cell having a solid membrane electrolyte for electrochemical reactions of an organic fuel. Catalyst utilization and catalyst/membrane interface improvements are disclosed. Specifically, the catalyst layer is applied directly onto the membrane electrolyte.
Ionic liquids are versatile electrolytes whose properties at electrified interfaces have the potential to enable technologies such as supercapacitors and Li-metal battery anodes. At electrified carbon surfaces, ionic liquids form an electric double layer that stores energy and provides the foundation for supercapacitors. At electrified lithium surfaces, ionic liquids decompose to form a solid electrolyte interphase that has the potential to stabilize Li-metal anodes in rechargable batteries. The behavior of two ionic liquids of technological importance, [pyr14][TFSI] and [EMIM][BF4], are examined at these electrified interfaces through molecular dynamics and ab initio techniques.
Ionic liquids are versatile electrolytes whose properties at electrified interfaces have the potential to enable technologies such as supercapacitors and Li-metal battery anodes. At electrified carbon surfaces, ionic liquids form an electric double layer that stores energy and provides the foundation for supercapacitors. At electrified lithium surfaces, ionic liquids decompose to form a solid electrolyte interphase that has the potential to stabilize Li-metal anodes in rechargable batteries. The behavior of two ionic liquids of technological importance, [pyr14][TFSI] and [EMIM][BF4], are examined at these electrified interfaces through molecular dynamics and ab initio techniques.
Ionic liquids are versatile electrolytes whose properties at electrified interfaces have the potential to enable technologies such as supercapacitors and Li-metal battery anodes. At electrified carbon surfaces, ionic liquids form an electric double layer that stores energy and provides the foundation for supercapacitors. At electrified lithium surfaces, ionic liquids decompose to form a solid electrolyte interphase that has the potential to stabilize Li-metal anodes in rechargable batteries. The behavior of two ionic liquids of technological importance, [pyr14][TFSI] and [EMIM][BF4], are examined at these electrified interfaces through molecular dynamics and ab initio techniques.
The objectives of this work are to develop growth techniques and theory leading to improved bulk growth of semiconductor single crystals. Ground based experiments will be complemented by experiments carried out in the low-g environment provided by the space shuttle. Analytical studies and laboratory investigations are being conducted to better define the causes of crystalline defects and inhomogeneities. The compound semiconductor lead-tin-telluride is being used as the modeling material. Theoretical techniques are being developed to predict the thermal and solutal fields which are present during bulk growth from a melt. Techniques for measuring the thermophysical properties of semiconductors at high temperatures have been developed. During the past year electrochemical etching techniques have been developed for delineation of inhomogeneous regions in crystals. Thermal diffusivity measurements have been completed for the solid and liquid phases of PbTe and PbSnTe. Preliminary results have been obtained on the effects on crystal morphology of gravity, interface shape and interaction between the melt and the container.
There is a need to acquire autonomously cryogenic hydrocarbon liquid sample from remote planetary locations such as the lakes of Titan for instruments such as mass spectrometers. There are several problems that had to be solved relative to collecting the right amount of cryogenic liquid sample into a warmer spacecraft, such as not allowing the sample to boil off or fractionate too early; controlling the intermediate and final pressures within carefully designed volumes; designing for various particulates and viscosities; designing to thermal, mass, and power-limited spacecraft interfaces; and reducing risk. Prior art inlets for similar instruments in spaceflight were designed primarily for atmospheric gas sampling and are not useful for this front-end application. These cryogenic liquid sample acquisition system designs for remote space applications allow for remote, autonomous, controlled sample collections of a range of challenging cryogenic sample types. The design can control the size of the sample, prevent fractionation, control pressures at various stages, and allow for various liquid sample levels. It is capable of collecting repeated samples autonomously in difficult lowtemperature conditions often found in planetary missions. It is capable of collecting samples for use by instruments from difficult sample types such as cryogenic hydrocarbon (methane, ethane, and propane) mixtures with solid particulates such as found on Titan. The design with a warm actuated valve is compatible with various spacecraft thermal and structural interfaces. The design uses controlled volumes, heaters, inlet and vent tubes, a cryogenic valve seat, inlet screens, temperature and cryogenic liquid sensors, seals, and vents to accomplish its task.
Satellite observations of denitrification and ice clouds in the Arctic lower stratosphere in February 1997 are used with Lagrangian microphysical box model calculations to evaluate nucleation mechanisms of solid polar stratospheric cloud (PSC) particles. The occurrences of ice clouds are not correlated in time and space with the locations of back trajectories of denitrified air masses, indicating that ice particle surfaces are not always a prerequisite for the formation of solid PSCs that lead to denitrification. In contrast, the model calculations incorporating a pseudoheterogeneous freezing process occurring at the vapor-liquid interface can quantitatively explain most of the observed denitrification when the nucleation activation free energy for nitric acid dihydrate formation is raised by only approx.10% relative to the current published values. Once nucleated, the conversion of nitric acid dihydrate to the stable trihydrate phase brings the computed levels of denitrification closer to the measurements. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0320 Atmospheric Composition and Sb~lctureC: loud physics and chemistry; 0340 Atmospheric Composition and Structure: Middle atmosphere-composition and chemistry
Stommel et al. (1956) have first described an instability, known as thermosolutal convection, thermohaline convection, or double-diffusive convection. This instability may occur in the case of a fluid in a gravitational field with two diffusing components present. The present study is concerned with the effect of sidewalls on flow in the fingering regime in the absence of applied horizontal gradients. The work was motivated by numerical results obtained on the basis of a simulation of thermosolutal convection occurring during the unidirectional solidification of a binary alloy. In this case, the unperturbed solute field in the liquid ahead of the solidifying planar interface has an exponential vertical profile because of the rejection or preferential incorporation of solute by the solid phase.
A transient moving contact line is investigated experimentally. The dynamic interface shape between 20 and 800 microns from the contact line is compared with theory. A novel experiment is devised, in which the contact line is set into motion by electrically altering the solid-liquid surface tension gamma(sub SL). The contact line motion simulates that of spontaneous wetting along a vertical plate with a maximum capillary number Ca approx. = 4 x 10(exp -2). The images of the dynamic meniscus are analyzed as a funtion of Ca. For comparison, the steady-state hydrodynamic equation based on the creeping flow model in a wedge geometry and the three-region uniform perturbation expansion of Cox (1986) is adopted. The interface shape is well depicted by the uniform solutions for Ca <= 10(exp -3). However, for Ca > 10(exp -3), the uniform solution over-predicts the viscous bending. This over-prediction can be accounted for by modifying the slip coefficient within the intermediate solution. With this correction, the measured interface shape is seen to match the theoretical prediction for all capillary numbers. The amount of slip needed to fit the measurements does not scale with the capillary number.
Numerical and analytical solutions are presented for the temperature and concentration distributions during the solidification of a binary liquid alloy slab. The slab is taken to be of a finite depth but infinite in the horizontal direction. The solidification process is started by withdrawing a fixed amount of heat from the lower surface of the slab. The upper surface of the slab is subjected to both radiation and convective conditions. The solution gives the concentration and temperature profiles and the interface position as a function of time. Due to the smallness of the mass diffusion coefficient in the solid, the numerical solution method breaks down whenever the ratio of the diffusivities in the solid and the liquid falls below a certain value. An analytical method is developed which gives accurate solution for any value of the diffusivity ratio.
The present invention relates generally to the field of thermal transfer and, more specifically, to a direct-interface, fusible heat sink for non-venting, regenerable, and self-contained thermal regulation. A quick connect coupling includes a male and a female portion. The female portion is frozen in a container of solid-phase coolant fluid, i.e., water, so that passages in the housing are blocked by ice initially. The ice is melted by direct interface with liquid coolant fluid delivered from the male portion. The present invention has advantages in that the phase change material remains sealed at all times, including during regeneration. Also, it uses quick-disconnect couplings that allow the phase change material to completely fill the container and is easily handled in microgravity without spills, leakage, or handling of phase change material.
Fluid behavior in a low-g environment is controlled primarily by surface tension forces. Certain fluid and system characteristics determine the magnitude of these forces for both a free liquid surface and liquid in contact with a solid. These characteristics, including surface tension, wettability or contact angle, system geometry, and the relationships governing their interaction, are discussed. Various aspects of fluid behavior in a low-g environment are then presented. This includes the formation of static interface shapes, oscillation and rotation of drops, coalescence, the formation of foams, tendency for cavitation, and diffusion in liquids which were observed during the Skylab fluid mechanics science demonstrations. Liquid reorientation and capillary pumping to establish equilibrium configurations for various system geometries, observed during various free-fall (drop-tower) low-g tests, are also presented. Several passive low-g fluid storage and transfer systems are discussed. These systems use surface tension forces to control the liquid/vapor interface and provide gas-free liquid transfer and liquid-free vapor venting.