Recent large-scale computer simulations suggest that it may be possible to create a new class of soft solids, called 'bijels', by stabilizing and arresting the bicontinuous interface in a binary liquid demixing via spinodal decomposition using particles that are neutrally wetted by both liquids. The interfacial layer of particles is expected to be semi-permeable; hence, if realized, these new materials would have many potential applications, for example, as micro-reaction media. However, the creation of bijels in the laboratory faces serious obstacles. In general, fast quench rates are necessary to bypass nucleation, so that only samples with limited thickness can be produced, which destroys the three-dimensionality of the putative bicontinuous network. Moreover, even a small degree of unequal wettability of the particles by the two liquids can lead to ill-characterized, 'lumpy' interfacial layers and therefore irreproducible material properties. Here, we report a reproducible protocol for creating three-dimensional samples of bijel in which the interfaces are stabilized by essentially a single layer of particles. We demonstrate how to tune the mean interfacial separation in these bijels, and show that mechanically, they indeed behave as soft solids. These characteristics and their tunability will be of great value for microfluidic applications.
The liquid-liquid phase separation of a binary solvent can be arrested by colloidal particles trapped at the interface [K. Stratford, Science 309, 2198 (2005)]. We show experimentally that the colloidal network so formed can remain stable after fully remixing the liquids, creating a new type of gel in which colloids in a single-phase solvent have locally planar coordination. We argue that this structure is likely maintained by primary-minimum Derjaguin-Landau-Verweg-Overbeek bonding of our charged colloids, created under strong compression by capillary forces. We present simulation evidence that the combination of a short-ranged attraction with a repulsive barrier can strongly stabilize such locally planar gels.
Abstract. Colloidal particles with appropriate wetting properties can become very strongly trapped at an interface between two immiscible fluids. We have harnessed this phenomenon to create a new class of soft materials with intriguing and potentially useful characteristics. The material is known as a bijel: bicontinuous interfacially-jammed emulsion gel. It is a colloid-stabilized emulsion with fluid-bicontinuous domains. The potential to create these gels was first predicted using computer simulations. Experimentally we use mixtures of water and 2,6-lutidine at the composition for which the system undergoes a critical demixing transition on warming. Colloidal silica, with appropriate surface chemistry, is dispersed while the system is in the single-fluid phase; the composite sample is then slowly warmed well beyond the critical temperature. The liquids phase separate via spinodal decomposition and the particles become swept up on the newly created interfaces. As the domains coarsen the interfacial area decreases and the particles eventually become jammed together. The resulting structures have a significant yield stress and are stable for many months. Here we begin to explore the complex wetting properties of fluorescently-tagged silica surfaces in water-lutidine mixtures, showing how they can be tuned to allow bijel creation. Additionally we demonstrate how the particle properties change with time while they are immersed in the solvents.
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