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Phase segregation triggered by selective evaporation can emerge in multicomponent systems, leading to complex physicochemical hydrodynamics. Recently, Li et al. (Phys. Rev. Lett., vol. 120, 2018, 224501) and Kim & Stone (J. Fluid Mech., vol. 850, 2018, pp. 769–783) reported a segregative behaviour (i.e. demixing) in an evaporating binary droplet. In this work, by means of experiments and theoretical analysis, we investigate the flow dynamics after the occurrence of the phase segregation. As example, we take the 1,2-hexanediol–water binary droplet system. First, we reveal experimentally the overall physicochemical hydrodynamics of the evaporation process, including the segregative behaviour and the resulting flow structure close to the substrate. By quantifying the evolution of the radial flow, we identify three successive life stages of the evaporation process. At Stage I, a radially outward flow is observed, driven by the Marangoni effect. At the transition to Stage II, the radial flow reverses partially, starting from the contact line. This flow breaks the axial symmetry and remarkably is driven by the segregation itself. Finally at Stage III, the flow decays as the evaporation ceases gradually. At this stage, the segregation has grown to the entire droplet, and the flow is again controlled by the Marangoni effect. The resulting Marangoni flow homogenizes the distribution of the entrapped volatile water over the whole droplet.
A liquid–gas interface (LGI) on submerged microstructure surfaces has the potential to achieve large slip velocities, which is significant for underwater applications such as drag reduction. However, surfactants adsorbing on the LGI can cause surface tension gradient against the mainstream, which weakens the flow near the LGI and severely limits drag reduction. The mechanism of the effect of surfactants on two-dimensional flows has already been proposed, while the effect of surfactants on the three-dimensional flow near the LGI is still not clear. In our study, we specifically design an experimental system to directly observe a three-dimensional backflow at the LGI. The formation as well as the behaviour of the backflow are demonstrated to be significantly influenced by the surfactant. Combining experimental measurements, theoretical analyses and numerical simulations, we reveal the underlying mechanism of the backflow, which is a competition between the mainstream and the Marangoni flows generated by the interfacial concentration gradients of surfactant simultaneously in streamwise and spanwise directions, reflecting the three-dimensional feature of the backflow. In addition, a kinematic similarity is obtained to characterize the backflow. The current work provides a model system for investigating the three-dimensional backflow at the LGI with surfactants, which is significant for practical applications such as drag reduction and superhydrophobicity.
The Greek aperitif Ouzo is not only famous for its specific anise-flavoured taste, but also for its ability to turn from a transparent miscible liquid to a milky-white coloured emulsion when water is added. Recently, it has been shown that this so-called Ouzo effect, i.e. the spontaneous emulsification of oil microdroplets, can also be triggered by the preferential evaporation of ethanol in an evaporating sessile Ouzo drop, leading to an amazingly rich drying process with multiple phase transitions (Tan et al., Proc. Natl Acad. Sci. USA, vol. 113 (31), 2016, pp. 8642–8647). Due to the enhanced evaporation near the contact line, the nucleation of oil droplets starts at the rim which results in an oil ring encircling the drop. Furthermore, the oil droplets are advected through the Ouzo drop by a fast solutal Marangoni flow. In this article, we investigate the evaporation of mixture droplets in more detail, by successively increasing the mixture complexity from pure water over a binary water–ethanol mixture to the ternary Ouzo mixture (water, ethanol and anise oil). In particular, axisymmetric and full three-dimensional finite element method simulations have been performed on these droplets to discuss thermal effects and the complicated flow in the droplet driven by an interplay of preferential evaporation, evaporative cooling and solutal and thermal Marangoni flow. By using image analysis techniques and micro-particle-image-velocimetry measurements, we are able to compare the numerically predicted volume evolutions and velocity fields with experimental data. The Ouzo droplet is furthermore investigated by confocal microscopy. It is shown that the oil ring predominantly emerges due to coalescence.
The dissolution of a single droplet, containing a mixture of oils, in water is experimentally studied. The oils in the droplet varied in terms of their solubility in water and their hydrophobicity. We demonstrate that the polarity of the droplet constituents strongly influences the dissolution dynamics. A binary-component droplet, containing two polar components (one soluble the other insoluble) exhibits a retarded dissolution as compared to a droplet containing only the soluble component. We argue that in this case the mixture in the droplet can be assumed homogeneous, leading to a smaller effective contact area of the soluble liquid in the droplet with the bulk water, and thus delayed dissolution. On the other hand, it is shown that this is not the case when a polar, soluble component is mixed with an insoluble non-polar component, in which case segregation between the different liquids inside the droplet occurs, leading to Marangoni flows and superspreading of the droplet. The segregation is confirmed by volumetric measurements and by the use of a solvatochromic dye in combination with confocal microscopy, which clearly showed that during dissolution local concentration differences inside the droplet developed.
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