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Interfacial Region Thermophysics and Intrinsic Stability of Thin Free Liquid Films

Abstract

The film rupture process that dictates merging of adjacent bubbles is particularly important in nucleate boiling heat transfer, bubbly two-phase flow in small tubes, and the mechanisms that dictate the Leidenfrost transition. To understand the mechanisms of bubble merging in nano-structured boiling surfaces and in nanotubes, it is useful to explore film stability and onset of rupture at the molecular level. This dissertation reports the results of such an investigation combining three strategies that includes a new formulation of capillarity theory for free liquid films, molecular dynamics (MD) simulations using similar interaction potentials and bubble merging experiments. Two forms of our molecular film capillarity theory are developed here: one for non-polar fluids based on a Lennard-Jones interaction potential, and a second specifically for water using a modified treatment of the SPC/E interaction potential that accounts for water dipole interactions. The capillarity theory provides theoretical relationships among parameters that govern film structure and thermophysical behavior, while the companion MD simulations allow more detailed molecular level exploration of the film thermophysics. Results obtained with theoretical models and MD simulation studies indicate that the wave instability and the lack of thermodynamics intrinsic stability can lead to rupture of the liquid film, as its thickness decreases below a critical value. It is further predicted that wave instability predominates as an onset of rupture mechanism for liquid films of macroscopic extent, but for free liquid films with nanoscale lateral extent (in, for example, nanostructured boiling surfaces), lack of core stability is more likely to be the mechanism. For electrolyte aqueous solutions, theoretical models and MD simulation studies suggest that dissolved salts tend to alter the surface tension at liquid vapor interfaces and affect the stability of the free liquid film between adjacent bubbles. Bubble merging experiments are designed and carried out for various electrolyte aqueous solutions. The interaction of pairs of bubbles injected into solution with different dissolved salt concentrations is studied experimentally to determine the probability of merging from statistics for ensembles of bubble pairs. The results of these experiments indicate that for some types of salts, very low dissolved salt concentrations can strongly reduce the tendency of adjacent bubbles to merge, implying that the presence of the dissolved salt in such cases strongly enhances the stability of the free liquid film between adjacent bubbles. The trends are compared to predictions of free liquid film stability by wave instability theory and MD simulations.

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