Publications

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We examine several methods to create a sheet of magnesium oxide (MgO) macroporous ceramic material via tape casting. These methods include the approach pioneered by Akartuna et al.1 in which an oil/water emulsion is stabilized by surface-modified metal oxide particles at the droplet interfaces. Upon drying, a scaffold of the self-assembled particles is strong enough to be removed from the substrate material and sintered. We find that this method can be used with MgO particles surface modified by short amphiphilic molecules. This approach is compared with two more traditional methods to induce structure into a green ceramic: 1) creation of an MgO ceramic slip with added pore formers, and 2) sponge impregnation of a reticulated foam with the MgO slip. Green and sintered samples made using each method are hardness tested and results compared for several densities of the final ceramics. Optical and SEM images of the materials are shown.

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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When a fluid jet impinges on a solid substrate, a variety of behaviors may occur around the impact region. One example is mounding, where the fluid enters the impact region faster than it can flow away, forming a mound of fluid above the main surface. For some operating conditions, this mound can destabilize and buckle, entraining air in the mound. Other behaviors include submerging flow, where the jet impinges into an otherwise steady pool of liquid, entraining a thin air layer as it enters the pool. This impact region is one of very high shear rates and as such, complex fluids behave very differently than do Newtonian fluids. In this work, we attempt to characterize this range of behavior for Newtonian and non-Newtonian fluids using dimensionless parameters. We model the fluid as a modified Bingham-Carreau-Yasuda fluid, which exhibits the full range of pseudoplastic flow properties throughout the impact region. Additionally, we study viscoelastic effects through the use of the Giesekus model. Both 2-D and 3-D numerical simulations are performed using a variety of finite element method techniques for tracking the jet interface, including Arbitrary Lagrangian Eulerian (ALE), diffuse level sets, and a conformal decomposition finite element method (CDFEM). The presence of shear-thinning characteristics drastically reduces unstable mounding behavior, yet can lead to air entrainment through the submerging flow regime. We construct an operating map to understand for what flow parameters mounding and submerging flows will occur, and how the fluid rheology affects these behaviors. This study has many implications in high-speed industrial bottle filling applications.

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In this presentation we examine the accuracy and performance of a suite of discrete-element-modeling approaches to predicting equilibrium and dynamic rheological properties of polystyrene suspensions. What distinguishes each approach presented is the methodology of handling the solvent hydrodynamics. Specifically, we compare stochastic rotation dynamics (SRD), fast lubrication dynamics (FLD) and dissipative particle dynamics (DPD). Method-to-method comparisons are made as well as comparisons with experimental data. Quantities examined are equilibrium structure properties (e.g. pair-distribution function), equilibrium dynamic properties (e.g. short- and long-time diffusivities), and dynamic response (e.g. steady shear viscosity). In all approaches we deploy the DLVO potential for colloid-colloid interactions. Comparisons are made over a range of volume fractions and salt concentrations. Our results reveal the utility of such methods for long-time diffusivity prediction can be dubious in certain ranges of volume fraction, and other discoveries regarding the best formulation to use in predicting rheological response.

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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