The wetting of ceramic surfaces by aluminum alloys has been reexamined using a chemical system where interfacial reactions and oxide film effects could be isolated. The system Al–Mg–O was chosen since it is technologically important and high-purity, well-characterized materials are readily available. Magnesium alloyed with the aluminum sessile drop and silicon picked up from the experimental apparatus cause an initial reduction in contact angle by altering the protective nature of the oxide film formed on the sessile drop. Evidence of spreading is observed as an intermediate process in the reactive sessile drop pairs. Reaction products formed between the Al–Mg alloys and sapphire (Al2O3), spinel (MgAl2O4), or periclase (MgO) can be interpreted with predicted phase equilibria and the measured loss of magnesium from the sessile drop. Only the rate of the periclase alloy interaction was rapid enough to result in a continuous product layer after 24 h at 800 °C. The volatilization of all of the magnesium from the sessile drop resulted in the formation of a true Al–Al2O3 interface. The contact angle for a true Al–Al2O3 interface is 88 ± 5 deg at 800 °C. The liquid-solid interfacial energy is 1688 ergs/cm2.

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Sessile drop studies of molten aluminum on single-crystal sapphire substrates were conducted to investigate the effects of atmosphere on contact angle, substrate reactions, and interfacial crystal growth. Unlike previous investigations performed briefly in a vacuum environment in a temperature range within 600°C of the aluminum melting point, these experiments were conducted at higher temperatures (1200" to 1600°C) and at 1-atm total pressure over longer experimental times to more closely approach equilibrium conditions. A continuously flowing buffered gas system utilizing high-purity metered mixtures of hydrogen and helium in combination with a thoria ceramic electrolyte sensor were employed to achieve variations of the oxygen partial pressure from to atm while continuously maintaining the total pressure at 1 atm. At constant temperature, it was found that neither the oxygen partial pressure nor the crystallographic orientation of the sapphire substrate had a significant effect on the observed contact angles. A continuous decrease of acute contact angles and a single reaction ring characterized the 8-h experiments without the alternating spreading and contracting behavior repeatedly reported in the literature. This phenomenon can be attributed to the lower rate of metal evaporation and interfacial reaction a t the higher total gas pressure and yet extremely low oxygen partial pressure of these experiments. Profilometric analysis of sapphire substrates subsequent to the removal of the quenched sessile drops indicates a reduction in metal-solid interaction due to the closer approach to equilibrium than in previous studies. An epitaxial orientation with respect to the substrate was observed in a-alumina crystallite formation at the metal-ceramic interface. Experimental evidence suggests that it was formed by a nucleation and growth process during the cooling period. [

The spreading kinetics of molten aluminum on ceramic surfaces bearing reactive coatings has been studied through the direct observation of sessile drops, either formed in situ or emplaced at temperature. Analysis of videotapes permitted the assessment of the rate of advance of rapidly spreading droplets. Experimental conditions in this study were chosen to avoid the severe retarding effect of the aluminum oxide film which is typically encountered in aluminum wetting experiments. A variety of reactive coating systems were examined (B, Cu, Ni, Ti, and Ti + B), and the effect of coating amount was assessed. Based upon the experiments of this study, the main effect of the coatings is to drive spreading due to strong exothermic interfacial reactions. The intensity of the interfacial reaction causes the change in free energy per unit area of interface to dominate the rate of movement of the triple line.