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Surface rheology and interface stability

Mondy, L.A.; Brooks, Carlton F.; Grillet, Anne M.; Moffat, Harry K.; Koehler, Timothy P.; Yaklin, Melissa A.; Cote, Raymond O.; Castaneda, Jaime N.

We have developed a mature laboratory at Sandia to measure interfacial rheology, using a combination of home-built, commercially available, and customized commercial tools. An Interfacial Shear Rheometer (KSV ISR-400) was modified and the software improved to increase sensitivity and reliability. Another shear rheometer, a TA Instruments AR-G2, was equipped with a du Nouey ring, bicone geometry, and a double wall ring. These interfacial attachments were compared to each other and to the ISR. The best results with the AR-G2 were obtained with the du Nouey ring. A Micro-Interfacial Rheometer (MIR) was developed in house to obtain the much higher sensitivity given by a smaller probe. However, it was found to be difficult to apply this technique for highly elastic surfaces. Interfaces also exhibit dilatational rheology when the interface changes area, such as occurs when bubbles grow or shrink. To measure this rheological response we developed a Surface Dilatational Rheometer (SDR), in which changes in surface tension with surface area are measured during the oscillation of the volume of a pendant drop or bubble. All instruments were tested with various surfactant solutions to determine the limitations of each. In addition, foaming capability and foam stability were tested and compared with the rheology data. It was found that there was no clear correlation of surface rheology with foaming/defoaming with different types of surfactants, but, within a family of surfactants, rheology could predict the foam stability. Diffusion of surfactants to the interface and the behavior of polyelectrolytes were two subjects studied with the new equipment. Finally, surface rheological terms were added to a finite element Navier-Stokes solver and preliminary testing of the code completed. Recommendations for improved implementation were given. When completed we plan to use the computations to better interpret the experimental data and account for the effects of the underlying bulk fluid.

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Investigation of interfacial rheology & foam stability

Grillet, Anne M.; Koehler, Timothy P.; Reichert, Matthew D.; Yaklin, Melissa A.; Brooks, Carlton F.; Mondy, L.A.; Castaneda, Jaime N.; Cote, Raymond O.

The rheology at gas-liquid interfaces strongly influences the stability and dynamics of foams and emulsions. Several experimental techniques are employed to characterize the rheology at liquid-gas interfaces with an emphasis on the non-Newtonian behavior of surfactant-laden interfaces. The focus is to relate the interfacial rheology to the foamability and foam stability of various aqueous systems. An interfacial stress rheometer (ISR) is used to measure the steady and dynamic rheology by applying an external magnetic field to actuate a magnetic needle suspended at the interface. Results are compared with those from a double wall ring attachment to a rotational rheometer (TA Instruments AR-G2). Micro-interfacial rheology (MIR) is also performed using optical tweezers to manipulate suspended microparticle probes at the interface to investigate the steady and dynamic rheology. Additionally, a surface dilatational rheometer (SDR) is used to periodically oscillate the volume of a pendant drop or buoyant bubble. Applying the Young-Laplace equation to the drop shape, a time-dependent surface tension can be calculated and used to determine the effective dilatational viscosity of an interface. Using the ISR, double wall ring, SDR, and MIR, a wide range of sensitivity in surface forces (fN to nN) can be explored as each experimental method has different sensitivities. Measurements will be compared to foam stability.

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Experiments for foam model development and validation

Mondy, L.A.; Gorby, Allen D.; Cote, Raymond O.; Castaneda, Jaime N.; Thompson, Kyle R.; Rao, Rekha R.; Moffat, Harry K.; Kraynik, Andrew M.; Russick, Edward M.; Adolf, Douglas B.; Grillet, Anne M.; Brotherton, Christopher M.; Bourdon, Christopher B.

A series of experiments has been performed to allow observation of the foaming process and the collection of temperature, rise rate, and microstructural data. Microfocus video is used in conjunction with particle image velocimetry (PIV) to elucidate the boundary condition at the wall. Rheology, reaction kinetics and density measurements complement the flow visualization. X-ray computed tomography (CT) is used to examine the cured foams to determine density gradients. These data provide input to a continuum level finite element model of the blowing process.

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Wetting and free surface flow modeling for potting and encapsulation

Adolf, Douglas B.; Castaneda, Jaime N.; Kraynik, Andrew M.; Noble, David R.; Sun, Amy C.; Cote, Raymond O.; Grillet, Anne M.; Notz, Patrick N.; Brooks, Carlton F.; Givler, R.C.; Hopkins, Matthew M.; Mondy, L.A.; Rao, Rekha R.

As part of an effort to reduce costs and improve quality control in encapsulation and potting processes the Technology Initiative Project ''Defect Free Manufacturing and Assembly'' has completed a computational modeling study of flows representative of those seen in these processes. Flow solutions are obtained using a coupled, finite-element-based, numerical method based on the GOMA/ARIA suite of Sandia flow solvers. The evolution of the free surface is solved with an advanced level set algorithm. This approach incorporates novel methods for representing surface tension and wetting forces that affect the evolution of the free surface. In addition, two commercially available codes, ProCAST and MOLDFLOW, are also used on geometries representing encapsulation processes at the Kansas City Plant. Visual observations of the flow in several geometries are recorded in the laboratory and compared to the models. Wetting properties for the materials in these experiments are measured using a unique flowthrough goniometer.

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Modeling injection molding of net-shape active ceramic components

Rao, Rekha R.; Brooks, Carlton F.; Cote, Raymond O.; Castaneda, Jaime N.; Mondy, L.A.; Noble, David R.; Hopkins, Matthew M.; Notz, Patrick N.; Halbleib, Laura L.; Yang, Pin Y.; Burns, George B.; Grillet, Anne M.

To reduce costs and hazardous wastes associated with the production of lead-based active ceramic components, an injection molding process is being investigated to replace the current machining process. Here, lead zirconate titanate (PZT) ceramic particles are suspended in a thermoplastic resin and are injected into a mold and allowed to cool. The part is then bisque fired and sintered to complete the densification process. To help design this new process we use a finite element model to describe the injection molding of the ceramic paste. Flow solutions are obtained using a coupled, finite-element based, Newton-Raphson numerical method based on the GOMA/ARIA suite of Sandia flow solvers. The evolution of the free surface is solved with an advanced level set algorithm. This approach incorporates novel methods for representing surface tension and wetting forces that affect the evolution of the free surface. Thermal, rheological, and wetting properties of the PZT paste are measured for use as input to the model. The viscosity of the PZT is highly dependent both on temperature and shear rate. One challenge in modeling the injection process is coming up with appropriate constitutive equations that capture relevant phenomenology without being too computationally complex. For this reason we model the material as a Carreau fluid and a WLF temperature dependence. Two-dimensional (2D) modeling is performed to explore the effects of the shear in isothermal conditions. Results indicate that very low viscosity regions exist near walls and that these results look similar in terms of meniscus shape and fill times to a simple Newtonian constitutive equation at the shear-thinned viscosity for the paste. These results allow us to pick a representative viscosity to use in fully three-dimensional (3D) simulation, which because of numerical complexities are restricted to using a Newtonian constitutive equation. Further 2D modeling at nonisothermal conditions shows that the choice of representative Newtonian viscosity is dependent on the amount of heating of the initially room temperature mold. An early 3D transient model shows that the initial design of the distributor is sub-optimal. However, these simulations take several months to run on 4 processors of an HP workstation using a preconditioner/solver combination of ILUT/GMRES with fill factors of 3 and PSPG stabilization. Therefore, several modifications to the distributor geometry and orientations of the vents and molds have been investigated using much faster 3D steady-state simulations. The pressure distribution for these steady-state calculations is examined for three different distributor designs to see if this can indicate which geometry has the superior design. The second modification, with a longer distributor, is shown to have flatter, more monotonic isobars perpendicular to the flow direction indicating a better filling process. The effects of the distributor modifications, as well as effects of the mold orientation, have also been examined with laboratory experiments in which the flow of a viscous Newtonian oil entering transparent molds is recorded visually. Here, the flow front is flatter and voids are reduced for the second geometry compared to the original geometry. A horizontal orientation, as opposed to the planned vertical orientation, results in fewer voids. Recently, the Navier-Stokes equations have been stabilized with the Dohrman-Bochev PSPP stabilization method, allowing us to calculate transient 3D simulations with computational times on the order of days instead of months. Validation simulations are performed and compared to the experiments. Many of the trends of the experiments are captured by the level set modeling, though quantitative agreement is lacking mainly due to the high value of the gas phase viscosity necessary for numerical stability, though physically unrealistic. More correct trends are predicted for the vertical model than the horizontal model, which is serendipitous as the actual mold is held in a vertical geometry. The full, transient mold filling calculations indicate that the flow front is flatter and voids may be reduced for the second geometry compared to the original geometry. The validated model is used to predict mold filling for the actual process with the material properties for the PZT paste, the original distributor geometry, and the mold in a vertical orientation. This calculation shows that voids may be trapped at the four corners of the mold opposite the distributor.

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An experimental investigation of the effect of walls on gas-liquid flows through fixed particle

Proceedings of the American Society of Mechanical Engineers Fluids Engineering Division Summer Conference

Cooper, Marcia A.; Cote, Raymond O.; O'Hern, Timothy J.; Torczynski, J.R.; Evans, Lindsey R.; Cross, William M.

The effect of particle diameter on downward co-current gas-liquid flow through a fixed bed of particles confined within a cylindrical column is investigated. Several hydrodynamic regimes that depend strongly on the properties of the gas stream, the liquid stream, and the packed particle bed are known to exist within these systems. This experimental study focuses on characterizing the effect of wall confinement on these hydrodynamic regimes as the diameter d of the spherical particles becomes comparable to the column diameter D (or D/d becomes order-unity). The packed bed consists of polished, solid, spherical, monodisperse particles (beads) with mean diameter in the range of 0.64-2.54 cm. These diameters yield D/d values between 15 and 3.75, so this range overlaps and extends the previously investigated range for two-phase flow. Measurements of the pressure drop across the bed and across the pulses are obtained for varying gas and liquid flow rates. Copyright © 2005 by ASME.

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Mold-filling experiments for validation of modeling encapsulation. Part 1, "wine glass" mold

Mondy, L.A.; Grillet, Anne M.; Cote, Raymond O.; Castaneda, Jaime N.

The C6 project 'Encapsulation Processes' has been designed to obtain experimental measurements for discovery of phenomena critical to improving these processes, as well as data required in the verification and validation plan (Rao et al. 2001) for model validation of flow in progressively complex geometries. We have observed and recorded the flow of clear, Newtonian liquids and opaque, rheologically complex suspensions in two mold geometries. The first geometry is a simple wineglass geometry in a cylinder and is reported here in Part 1. The results in a more realistic encapsulation geometry are reported in Part 2.

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Investigation of oil injection into brine for the Strategic Petroleum Reserve : hydrodynamics and mixing experiments with SPR liquids

O'Hern, Timothy J.; Torczynski, J.R.; Cote, Raymond O.; Castaneda, Jaime N.

An experimental program was conducted to study a proposed approach for oil reintroduction in the Strategic Petroleum Reserve (SPR). The goal was to assess whether useful oil is rendered unusable through formation of a stable oil-brine emulsion during reintroduction of degassed oil into the brine layer in storage caverns. An earlier report (O'Hern et al., 2003) documented the first stage of the program, in which simulant liquids were used to characterize the buoyant plume that is produced when a jet of crude oil is injected downward into brine. This report documents the final two test series. In the first, the plume hydrodynamics experiments were completed using SPR oil, brine, and sludge. In the second, oil reinjection into brine was run for approximately 6 hours, and sampling of oil, sludge, and brine was performed over the next 3 months so that the long-term effects of oil-sludge mixing could be assessed. For both series, the experiment consisted of a large transparent vessel that is a scale model of the proposed oil-injection process at the SPR. For the plume hydrodynamics experiments, an oil layer was floated on top of a brine layer in the first test series and on top of a sludge layer residing above the brine in the second test series. The oil was injected downward through a tube into the brine at a prescribed depth below the oil-brine or sludge-brine interface. Flow rates were determined by scaling to match the ratio of buoyancy to momentum between the experiment and the SPR. Initially, the momentum of the flow produces a downward jet of oil below the tube end. Subsequently, the oil breaks up into droplets due to shear forces, buoyancy dominates the flow, and a plume of oil droplets rises to the interface. The interface was deflected upward by the impinging oil-brine plume. Videos of this flow were recorded for scaled flow rates that bracket the equivalent pumping rates in an SPR cavern during injection of degassed oil. Image-processing analyses were performed to quantify the penetration depth and width of the oil jet. The measured penetration depths were shallow, as predicted by penetration-depth models, in agreement with the assumption that the flow is buoyancy-dominated, rather than momentum-dominated. The turbulent penetration depth model overpredicted the measured values. Both the oil-brine and oil-sludge-brine systems produced plumes with hydrodynamic characteristics similar to the simulant liquids previously examined, except that the penetration depth was 5-10% longer for the crude oil. An unexpected observation was that centimeter-size oil 'bubbles' (thin oil shells completely filled with brine) were produced in large quantities during oil injection. The mixing experiments also used layers of oil, sludge, and brine from the SPR. Oil was injected at a scaled flow rate corresponding to the nominal SPR oil injection rates. Injection was performed for about 6 hours and was stopped when it was evident that brine was being ingested by the oil withdrawal pump. Sampling probes located throughout the oil, sludge, and brine layers were used to withdraw samples before, during, and after the run. The data show that strong mixing caused the water content in the oil layer to increase sharply during oil injection but that the water content in the oil dropped back to less than 0.5% within 16 hours after injection was terminated. On the other hand, the sediment content in the oil indicated that the sludge and oil appeared to be well mixed. The sediment settled slowly but the oil had not returned to the baseline, as-received, sediment values after approximately 2200 hours (3 months). Ash content analysis indicated that the sediment measured during oil analysis was primarily organic.

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Investigation of oil injection into brine for the strategic petroleum reserve : hydrodynamics experiments with simulant liquids

Torczynski, J.R.; Torczynski, J.R.; O'Hern, Timothy J.; Barney, Jeremy B.; Castaneda, Jaime N.; Cote, Raymond O.

An experimental program is being conducted to study a proposed approach for oil reintroduction in the Strategic Petroleum Reserve (SPR). The goal is to assess whether useful oil is rendered unusable through formation of a stable oil-brine emulsion during reintroduction of degassed oil into the brine layer in storage caverns. This report documents the first stage of the program, in which simulant liquids are used to characterize the buoyant plume that is produced when a jet of crude oil is injected downward from a tube into brine. The experiment consists of a large transparent vessel that is a scale model of the proposed oil injection process at the SPR. An oil layer is floated on top of a brine layer. Silicon oil (Dow Corning 200{reg_sign} Fluid, 5 cSt) is used as the simulant for crude oil to allow visualization of the flow and to avoid flammability and related concerns. Sodium nitrate solution is used as the simulant for brine because it is not corrosive and it can match the density ratio between brine and crude oil. The oil is injected downward through a tube into the brine at a prescribed depth below the oil-brine interface. Flow rates are determined by scaling to match the ratio of buoyancy to momentum between the experiment and the SPR. Initially, the momentum of the flow produces a downward jet of oil below the tube end. Subsequently, the oil breaks up into droplets due to shear forces, buoyancy dominates the flow, and a plume of oil droplets rises to the interface. The interface is deflected upward by the impinging oil-brine plume. Two different diameter injection tubes were used (1/2-inch and 1-inch OD) to vary the scaling. Use of the 1-inch injection tube also assured that turbulent pipe flow was achieved, which was questionable for lower flow rates in the 1/2-inch tube. In addition, a 1/2-inch J-tube was used to direct the buoyant jet upwards rather than downwards to determine whether flow redirection could substantially reduce the oil-plume size and the oil-droplet residence time in the brine. Reductions of these quantities would inhibit emulsion formation by limiting the contact between the oil and the brine. Videos of this flow were recorded for scaled flow rates that bracket the equivalent pumping rates in an SPR cavern. Image-processing analyses were performed to quantify the penetration depth of the oil jet, the width of the jet, and the deflection of the interface. The measured penetration depths are shallow, as predicted by penetration-depth models, in agreement with the assumption that the flow is buoyancy-dominated, rather than momentum-dominated. The turbulent penetration depth model provided a good estimate of the measured values for the 1-inch injection tube but overpredicted the penetration depth for the 1/2-inch injection tube. Adding a virtual origin term would improve the prediction for the 1/2-inch tube for low to nominal injection flow rates but could not capture the rollover seen at high injection flow rates. As expected, the J-tube yielded a much narrower plume because the flow was directed upward, unlike the downward-oriented straight-tube cases where the plume had to reverse direction, leading to a much wider effective plume area. Larger surface deflections were caused by the narrower plume emitted from the J-tube. Although velocity was not measured in these experiments, the video data showed that the J-tube plume was clearly faster than those emitted from the downward-oriented tubes. These results indicate that oil injection tube modifications could inhibit emulsion formation by reducing the amount of contact (both time and area) between the oil and the brine. Future studies will employ crude oil, saturated brine, and interfacial solids (sludge) from actual SPR caverns.

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25 Results
25 Results