ABSTRACT
Gallium-based liquid metals (LM) have surface tension an order of magnitude higher than water and break up into micro-droplets when mixed with other liquids. In contrast, silicone oil readily mixes into LM foams to create oil-in-LM emulsions with oil inclusions. Previously, the LM was foamed through rapid mixing in air for an extended duration (over 2 hours). This process first results in the internalization of oxide flakes that form at the air-liquid interface. Once a critical fraction of these randomly shaped solid flakes is reached, air bubbles internalize into the LM to create foams that can internalize secondary liquids. Here, we introduce an alternative oil-in-LM emulsion fabrication method that relies on the prior addition of SiO2 micro-particles into the LM before mixing it with the silicone oil. This particle-assisted emulsion formation process provides a higher control over the composition of the LM-particle mixture before oil addition, which we employ to systematically study the impact of particle characteristics and content on the emulsions' composition and properties. We demonstrate that the solid particle size (0.8 µm to 5 µm) and volume fraction (1% to 10%) have a negligible impact on the internalization of the oil inclusions. The inclusions are mostly spherical with diameters of 20 to 100 µm diameter and are internalized by forming new, rather than filling old, geometrical features. We also study the impact of the particle characteristics on the two key properties related to the functional application of the LM emulsions in the thermal management of microelectronics. In particular, we measure the impact of particles and silicone oil on the emulsion's thermal conductivity and its ability to prevent deleterious gallium-induced corrosion and embrittlement of contacting metal substrates. .
ABSTRACT
Gallium-based liquid metals (LMs) combine metallic properties with the deformability of a liquid, which makes them promising candidates for a variety of applications. To broaden the range of physical and chemical properties, a variety of solid additives have been incorporated into the LMs in the literature. In contrast, only a handful of secondary fluids have been incorporated into LMs to create foams (gas-in-LM) or emulsions (liquid-in-LM). LM foams readily form through mixing of LM in air, facilitated by the formation of a native oxide on the LM. In contrast, LM breaks up into microdroplets when mixed with a secondary liquid such as silicone oil. Stable silicone oil-in-LM emulsions form only during mixing of the oil with LM foam. In this work, we investigate the fundamental mechanism underlying this process. We describe two possible microscale mechanisms for emulsion formation: (1) oil replacing air in the foam or (2) oil creating additional features in the foam. The associated foam-to-emulsion density difference demonstrates that emulsions predominantly form through the addition of oxide-covered silicone oil capsules to the LM foam. We demonstrate this through density and surface wettability measurements and multiscale imaging of LM foam mixed with varied silicone oil contents in air or nitrogen environments. We also demonstrate the presence of a continuous silicone oil film on the emulsion surface and that this oil film prevents the embrittlement of contacting aluminum.
ABSTRACT
Gallium based liquid metals (LM) have prospective biomedical, stretchable electronics, soft robotics, and energy storage applications, and are being widely adopted as thermal interface materials. The danger of gallium corroding most metals used in microelectronics requires the cumbersome addition of "barrier" layers or LM break-up into droplets within an inert matrix such as silicone oil. Such LM-in-oil emulsions are stabilized by native oxide on the droplets but have decreased thermal performance. Here we show that mixing of the silicone oil into an LM-air foam yields emulsions with inverted phases. We investigate the stability of these oil-in-LM emulsions through a range of processing times and oil viscosities, and characterize the impact of these parameters on the materials' structure and thermal property relationships. We demonstrate that the emulsion with 40 vol% of 10 cSt silicone oil provides a unique thermal management material with a 10 W m-1 K-1 thermal conductivity and an exterior lubricant thin film that completely prevents corrosion of contacting aluminum.
