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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.
For a small sessile or pendant droplet it is generally assumed that gravity does not play any role once the Bond number is small. This is even assumed for evaporating binary sessile or pendant droplets, in which convective flows can be driven due to selective evaporation of one component and the resulting concentration and thus surface tension differences at the air–liquid interface. However, recent studies have shown that in such droplets gravity indeed can play a role and that natural convection can be the dominant driving mechanism for the flow inside evaporating binary droplets (Edwards et al., Phys. Rev. Lett., vol. 121, 2018, 184501; Li et al., Phys. Rev. Lett., vol. 122, 2019, 114501). In this study, we derive and validate a quasi-stationary model for the flow inside evaporating binary sessile and pendant droplets, which successfully allows one to predict the prevalence and the intriguing interaction of Rayleigh and/or Marangoni convection on the basis of a phase diagram for the flow field expressed in terms of the Rayleigh and Marangoni numbers.
The evaporation of multicomponent droplets is relevant to various applications but challenging to study due to the complex physicochemical dynamics. Recently, Li etal. (Phys. Rev. Lett., vol. 120, 2018, 224501) reported evaporation-triggered segregation in 1,2-hexanediol–water binary droplets. In this present work, we added 0.5 wt % silicone oil to the 1,2-hexanediol–water binary solution. This minute silicone oil concentration dramatically modifies the evaporation process, as it triggers an early extraction of the 1,2-hexanediol from the mixture. Surprisingly, we observe that the segregation of 1,2-hexanediol forms plumes, rising up from the rim of the sessile droplet towards the apex during droplet evaporation. By orientating the droplet upside down, i.e. by studying a pendent droplet, the absence of the plumes indicates that the flow structure is induced by buoyancy, which drives a Rayleigh–Taylor instability (i.e. driven by density differences and gravitational acceleration). From micro particle image velocimetry measurement, we further prove that the segregation of the non-volatile component (1,2-hexanediol) hinders the evaporation near the contact line, which leads to a suppression of the Marangoni flow in this region. Hence, on long time scales, gravitational effects, rather than Marangoni flows, play the dominant role in the flow structure. We compare the measurement of the evaporation rate with the diffusion model of Popov (Phys. Rev., vol. 71, 2005, 036313), coupled with Raoult's law and the activity coefficient. This comparison indeed confirms that the silicone-oil-triggered segregation of the non-volatile 1,2-hexanediol significantly delays the evaporation. With an extended diffusion model, in which the influence of the segregation has been implemented, the evaporation can be well described.
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