Observation of isotropic-isotropic demixing in colloidal platelet-sphere mixtures

Mixtures of colloids with different sizes and shapes are ubiquitous in nature and industry. The possible existence of isotropic-isotropic (I1-I2) demixing of platelets and spheres remains an open question. Here we present direct experimental evidence of I1-I2 demixing using platelets with a very small thickness-to-diameter ratio mixed with silica spheres at the size ratio q = R(sphere)/R(disk) = 0.0901 ± 0.0004. The platelets cause the isotropic-to-nematic phase transition at a very low volume fraction because of their highly anisometric shape. The presence of silica spheres in the suspension accelerates the phase transition and packs the nematic phase more densely via depletion interaction. Increasing the sphere volume fraction to 0.0014, a tri-phase region emerges. This direct observation of I1-I2 demixing seems to validate the free-volume scaled particle theory and indicates the need for refinement of the fundamental measure density functional theory.