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The ability to transfer microdroplets between fluid phases offers numerous advantages in various fields, enabling better control, manipulation, and utilization of small volumes of fluids in pharmaceutical formulations, microfluidics, and lab-on-a-chip devices, single-cell analysis or droplet-based techniques for nanomaterial synthesis. This study focuses on the stability and morphology of a sessile oil microdroplet at the four-phase contact line of solid-water-oil-air during the droplet transfer from underwater to air. We observed a distinct transition in microdroplet dynamics, characterized by a shift from a scenario dominated by Marangoni forces to one dominated by capillary forces. In the regime dominated by Marangoni forces, the oil microdroplets spread in response to the contact between the water-air interface and the water-oil interface and the emergence of an oil concentration gradient along the water-air interface. The spreading distance along the four-phase contact line follows a power law relationship of $t^{3/4}$, reflecting the balance between Marangoni forces and viscous forces. On the other hand, in the capillarity-dominated regime, the oil microdroplets remain stable at the contact line and after being transferred into the air. We identify the crossover between these two regimes in the parameter space defined by three factors: the approaching velocity of the solid-water-air contact line ($v_{cl}$), the radius of the oil microdroplet ($r_o$), and the radius of the water drop ($r_w$). Furthermore, we demonstrate how to use the four-phase contact line for shaping oil microdroplets using a full liquid process by the contact line lithography. The findings in this study may be also applied to materials synthesis where nanoparticles, microspheres, or nanocapsules are produced by microdroplet-based techniques., Comment: 6 figures

Over the past decade, there has been a growing interest in the study of multicomponent drops. These drops exhibit unique phenomena, as the interplay between hydrodynamics and the evolving physicochemical properties of the mixture gives rise to distinct and often unregulated behaviors. Of particular interest is the complex dynamic behavior of the drop contact line, which can display self-lubrication effect. The presence of a slipping contact line in self-lubricating multicomponent drops can suppress the coffee-stain effect, conferring valuable technological applications. This review will explain the current understanding of the self-lubrication effect of drops, and cover an analysis of fundamental concepts and recent advances in colloidal assembly. The potential applications of self-lubricating drops across different fields will also be highlighted.

Accurate detection and analysis of traces of persistent organic pollutants in water is important in many areas, including environmental monitoring and food quality control, due to their long environmental stability and potential bioaccumulation. While conventional analysis of organic pollutants requires expensive equipment, surface enhanced Raman spectroscopy (SERS) has demonstrated great potential for accurate detection of these contaminants. However, SERS analytical difficulties, such as spectral preprocessing, denoising, and substrate-based spectral variation, have hindered widespread use of the technique. Here, we demonstrate an approach for predicting the concentration of sample pollutants from messy, unprocessed Raman data using machine learning. Frequency domain transform methods, including the Fourier and Walsh Hadamard transforms, are applied to sets of Raman spectra of three model micropollutants in water (rhodamine 6G, chlorpyrifos, and triclosan), which are then used to train machine learning algorithms. Using standard machine learning models, the concentration of sample pollutants are predicted with more than 80 percent cross-validation accuracy from raw Raman data. cross-validation accuracy of 85 percent was achieved using deep learning for a moderately sized dataset (100 spectra), and 70 to 80 percent cross-validation accuracy was achieved even for very small datasets (50 spectra). Additionally, standard models were shown to accurately identify characteristic peaks via analysis of their importance scores. The approach shown here has the potential to be applied to facilitate accurate detection and analysis of persistent organic pollutants by surface-enhanced Raman spectroscopy.

Pipeline transportation is a vital method for conveying crushed oil sand ores and tailings in the oil sands industry. This study focuses on enhancing economic benefits by exploring the separation of valuable bitumen residues from coarse sand tailings within hydrotransport pipelines. Employing three-dimensional transient Eulerian-Eulerian computational fluid dynamics (CFD) simulations coupled with a population balance model (PBM), we examine the aggregation and breakage of bitumen droplets under various flow conditions. The CFD-PBM model's accuracy is validated against field measurements of velocity profiles and pressure drops. Our findings reveal that higher slurry velocities lead to intensified particle-bitumen interactions, resulting in reduced aggregated bitumen droplet sizes at the pipeline's core. Additionally, variations in bitumen fraction cause shifts in the distribution of coarse particles along the pipe's vertical axis, with increased aggregation and larger droplets in the upper region. Notably, we demonstrate that smaller bubbles promote a more uniform distribution of bitumen compared to larger bubbles. These insights provide valuable knowledge for optimizing bitumen recovery processes, facilitating the integration of pipeline dynamics with downstream separation and extraction units., Comment: 14

Preconcentration of the target compound is a critical step that ensures the accuracy of the subsequent chemical analysis. In this work, we present a straightforward yet effective liquid-liquid extraction approach based on surface nanodroplets (i.e., nanoextraction) for offline analysis of highly diluted sample solutions. The extraction and sample collection were streamlined in a 3-m microcapillary tube. The concentration of the target analyte in surface nanodroplets was significantly increased compared to the concentration in the sample solution, reaching several orders of magnitudes. A limit of detection (LOD) was decreased by a factor of $\sim 10^3$ for an organic model compound in Fourier-transform infrared spectroscopy (FTIR) measurements and $\sim 10^5$ for a model fluorescent dye in fluorescence detection. The quantitative analysis of the organic compound was also achieved in a wide concentration region from $10^{-3}$ M to $10^{-4}$ M. The total volume of surface nanodroplets can be manipulated to further enhance extraction efficiency, according to the principle that governs droplet formation by solvent exchange. Additionally, our method exhibited significantly improved sensitivity compared to traditional dispersive liquid-liquid microextraction (DLLME). The LOD of the fluorescent dye and the organic model compound obtained with DLLME was 3 orders of magnitude and 20 times higher than the LOD achieved through nanoextraction approach. The nanoextraction developed in this work can be applied to preconcentrate multi-compounds from river water samples, without clear interference from each other. This can further extend its applicability for the detection and quantification of target analytes in complex aqueous samples by common analytical instruments.

Evaporation of multi-component liquid mixtures in confined geometries, such as capillaries, is crucial in applications such as microfluidics, two-phase cooling devices, and inkjet printing. Predicting the behaviour of such systems becomes challenging because evaporation triggers complex spatio-temporal changes in the composition of the mixture. These changes in composition, in turn, affect evaporation. In the present work, we study the evaporation of aqueous glycerol solutions contained as a liquid column in a capillary tube. Experiments and direct numerical simulations show three evaporation regimes characterised by different temporal evolutions of the normalised mass transfer rate (or Sherwood number, $Sh$), namely $Sh (\tilde{t}) = 1$, $Sh \sim 1/\sqrt{\tilde{t}}$, and $Sh \sim \exp\left(-\tilde{t}\right)$. Here $\tilde{t}$ is a normalised time. We present a simplistic analytical model which shows that the evaporation dynamics can be expressed by the classical relation $Sh = \exp \left( \tilde{t} \right) \mathrm{erfc} \left( \sqrt{\tilde{t}}\right)$. For small and medium $\tilde{t}$, this expression results in the first and second of the three observed scaling regimes, respectively. This analytical model is formulated in the limit of pure diffusion and when the penetration depth $\delta(t)$ of the diffusion front is much smaller than the length $L(t)$ of the liquid column. When $\delta \approx L$, finite length effects lead to $Sh \sim \exp\left(-\tilde{t}\right)$, i.e. the third regime. Finally, we extend our analytical model to incorporate the effect of advection and determine the conditions under which this effect is important. Our results provide fundamental insight into the physics of selective evaporation from a multi-component liquid column.

As the most complex and heaviest component in bitumen, asphaltene precipitation induced by solvent dilution is important in oil sands extraction to remove solids and water from bitumen froth through dilution by paraffinic solvents. This review will compare asphaltene precipitation to dilution-induced solvent shifting in aqueous systems via the ouzo effect. We attempt to highlight similarities and differences in the evolution of nanodroplets and effects from solvent mixing conditions and point out mutual experimental techniques and modeling approaches for the research of both asphaltene precipitation and nanodroplet formation. The review will start from basic concepts in both asphaltene precipitation and the ouzo effect, then move on to the effects of solvent mixing on asphaltene precipitation in bulk. After that, we will introduce advances in microfluidic systems combined with cutting-edge experimental and simulation tools for asphaltene precipitation induced under controlled mixing with solvents and a droplet formation. Such comparison will inspire more in-depth understanding and control of asphaltene precipitation and the ouzo effect in aqueous systems., Comment: 32 Pages, 12 Figures

This work demonstrates an original and ultrasensitive approach for surface-enhanced Raman spectroscopy (SERS) detection based on evaporation of self-lubricating drops containing silver supraparticles. The developed method detects an extremely low concentration of analyte that is enriched and concentrated on sensitive SERS sites of the compact supraparticles formed from drop evaporation. A low limit of detection of 10^-16 M is achieved for a model hydrophobic compound rhodamine 6G (R6G). The quantitative analysis of R6G concentration is obtained from 10^-5 to 10^-11 M. In addition, for a model micro-pollutant in water triclosan, the detection limit of 10^-6 M is achieved by using microliter sample solutions. The intensity of SERS detection in this approach is robust to the dispersity of the nanoparticles in the drop but became stronger after a longer drying time. The ultrasensitive detection mechanism is the sequential process of concentration, extraction, and absorption of the analyte during evaporation of self-lubrication drop and hot spot generation for intensification of SERS signals. This novel approach for sample preparation in ultrasensitive SERS detection can be applied to the detection of chemical and biological signatures in areas such as environment monitoring, food safety, and biomedical diagnostics., Comment: 25 Pages, 12 Figures

Bitumen residues in the oil sand tailings can be a threat to the environment that separating them from tailings before disposal is crucial. However, low bitumen concentration in the tailings slurry and the complex transport characteristics of the four-phase mixture make the process difficult. This study establishes an Eulerian-Eulerian CFD model for an industrial-scale oil sand tailings pipeline. A comprehensive sensitivity analysis was conducted on the selection of carrier-solid and solid-bitumen drag models. The combination of small and large particle sizes (i.e., 75 & 700 um) and bitumen droplet size (i.e., 400 um) provided good agreement with field data in velocity profiles and pressure drop. The validated model was subsequently extended to investigate the influence of the secondary phase (i.e., bitumen droplets and bubbles) on flow characteristics in a tailing pipeline. The investigation covered a range of bitumen droplet size (100-400 um), bitumen fraction (0.0025-0.1), bubble size (5-1000 um), and bubble fraction (0.0025-0.3) and their influences on the velocity, solids, and bitumen distribution are revealed. For an optimum bubble size of 500 um, a maximum recovery of 59% from the top 50 % and 83 % from the top 75 % of the pipe cross-section was obtained. The present study demonstrates the preferential distribution of bitumen and provides valuable insight on bitumen recovery from an industrial-scale tailings pipeline., Comment: 51, 14 figures

Switchable hydrophilicity solvents (SHSs) are solvents defined by their ability to switch from their hydrophobic form to a hydrophilic form when put in contact with an acidic trigger such as $CO_2$. As a consequence, SHSs qualify as promising alternatives to volatile organic compounds during the industrial solvent extraction processes, as greener and inexpensive methods can be applied to separate and recover SHSs. Furthermore, because of their less volatile nature, SHSs are less flammable and so increase the safety of a larger-scale extraction process. In this work, we study the dynamics and in-drop phase separation during the dissolution process of a drop composed of SHS and polymer, triggered by an acid in the surrounding aqueous environment. From 70 different experimental conditions, we found a scaling relationship between the drop dissolution time and initial volume with an overall scaling coefficient $\sim$ 0.53. We quantitatively assessed and found a shorter dissolution time related with a decrease in pH of the aqueous phase or an increase in initial polymer concentration in the drop. Examining the internal state of the drop during the dissolution revealed an in-drop phase separation behavior, resulting in a porous morphology of the final polymer particle. Our experimental results provide a microscopic view of the SHS dissolution process from droplets, and findings may help design SHS extraction processes for particle formation from emulsions., Comment: 15 pages, 8 figures

Liquid-liquid extraction based on surface nanodroplets, namely nanoextraction, can continuously extract and enrich target analytes from the flow of a sample solution. This sample preconcentration technique is easy to operate in a continuous flow system with low organic solvent consumption and a high enrichment factor. In this review, the evolution from single drop microextraction to advanced nanoextraction will be briefly introduced. Also, the formation principle and key features of surface nanodroplets will be summarized. Further, the major findings of nanoextraction combined with in-droplet chemistry toward sensitive and quantitative detection will be discussed. Finally, we will give our perspectives on the future trend of nanoextraction., Comment: 9 pages, 5 figures, review article

Solvent exchange is a controlled process for dilution-induced phase separation. This work utilizes the solvent exchange method to reveal the effect of the mixing dynamics on the asphaltene precipitation process under 20 different mixing conditions using a model system of n-heptane and asphaltene in toluene. The external mixing between the asphaltene solution and the paraffinic solvent is strictly controlled. We employed a high-spatial-resolution total internal reflection fluorescence microscope to detect asphaltene precipitates with a resolution up to 200 nm. A multiphysics model is used to simulate the evolution of the oversaturation pulse in the solvent exchange process. Based on the simulation results, we predicted the effect of the flow rate, dimension, the orientation of the microfluidic chamber, and temperature on the surface coverage and size distribution of asphaltene precipitates. The model predictions of all factors corroborate with the experimental observations. Local concentration of the solvent and shear forces are found to be the two main reasons for the change of asphaltene precipitation caused by mixing dynamics. However, the influence of thermodynamics is more critical than the mixing dynamics as temperature changes. Through a combination of experimental and simulation studies, this work illuminates the significance of the transportation process for the final morphology of asphaltene precipitates and provides an in-depth insight into the mechanism of mixing dynamics on the asphaltene precipitation. A smart mixing may be to boost new phase formation without excessive solvent consumption., Comment: 34 pages, 13 figures

Understanding the flow behavior of complex concentrated slurries is of tremendous importance for industrial waste management. In this study, the transport of three-phase oil sands tailings in a horizontal pipeline is simulated via the mixture multiphase model coupled with the kinetic theory of granular flow. The solid particles and bitumen droplets are conveyed via a non-Newtonian carrier fluid in a turbulent regime inside an industrial-scale pipeline. The simulation results showed exceptional agreement with the field data, with errors of <3.5% for velocity distribution and <15% for the pressure drop. A systematic parametric investigation was performed for a wide range of flow conditions, showing that the majority of bitumen droplets reside at the top region of the pipe. Our findings may help design an effective process for the separation of bitumen residues during pipeline transport., Comment: 49 pages, 20 figures

The transport and aggregation of particles in suspensions is an important process in many physicochemical and industrial processes. In this work, we study the transport of particles in an evaporating binary droplet. Surprisingly, the accumulation of particles occurs not only at the contact line (due to the coffee-stain effect) or at the solid substrate (due to sedimentation), but also at a particular radial position near the liquid-air interface, forming a "ring", which we term as the Marangoni ring. The formation of this ring is primarily attributed to the solutal Marangoni flow triggered by the evaporation dynamics of the water-glycerol droplet. Experiments and simulations show fair agreement in the volume evolution and the general structure of the solutal Marangoni flow, that is, the Marangoni vortex. Experiments show that the location of the Marangoni ring is strongly correlated with the Marangoni vortex. However, finite element numerical simulations fail to describe the particle distribution seen in the experiments. Interestingly, the particles not only accumulate to form the Marangoni ring but also assemble as colloidal crystals close to the liquid-air interface, yielding iridescence. The formation of the colloidal crystals in the experiments is strong evidence that non-hydrodynamic interactions, which are not represented in the simulations, also play a significant role in our system.

Asphaltene precipitation is a crucial phase separation phenomenon in the oil industry, especially in paraffinic froth treatment to extract bitumen from oil sands ores. This work reveals the formation of particles at 0.2 to 0.4 um in radius, defined as a primary sub-micron particle (PSMP), which is ubiquitous from diffusive mixing between asphaltene solution and any of 23 types of precipitants examined in our experiments. The yield and quantity of asphaltene particles are affected not only by the Hildebrand solubility parameter of the precipitants but also by the diffusion coefficients of the asphaltene solution and the precipitant. The Population Balance Model (PBM) with the Hildebrand solubility parameter has been used to model particle size distribution. Good agreement has been achieved between numerical predictions and the experimental data. It indicates that the colloid theory can describe the size distribution of PSMP and larger aggregates. Therefore, this study provides new insight into the mechanism for the dependence of yield and size distribution of the precipitated asphaltene particles on the composition of precipitants and adding inhibitors. Controlling of asphaltene yield and size distribution may be applied to the process of hydrocarbon separation or asphaltene precipitation prevention., Comment: Preprint submitted to Fuel

The global need for clean water requires sustainable technology for purifying contaminated water. Highly efficient solar-driven photodegradation is a sustainable strategy for wastewater treatment. In this work, we demonstrate that the photodegradation efficiency of micropollutants in water can be improved by ~2-24 times by leveraging polymeric microlenses (MLs). These microlenses (MLs) are fabricated from the in-situ polymerization of surface nanodroplets. We found that photodegradation efficiency ({\eta}) in water correlates approximately linearly with the sum of the intensity from all focal points of MLs, although no difference in the photodegradation pathway is detected from the chemical analysis of the byproducts. With the same overall power over a given surface area, {\eta} is doubled by using ordered arrays, compared to heterogeneous MLs on an unpatterned substrate. Higher {\eta} from ML arrays may be attributed to a coupled effect from the focal points on the same plane that creates high local concentrations of active species to further speed up the rate of photodegradation. As a proof-of-concept for ML-enhanced water treatment, MLs were formed on the inner wall of glass bottles that were used as containers for water to be treated. Three representative micropollutants (norfloxacin, sulfadiazine, and sulfamethoxazole) in the bottles functionalized by MLs were photodegraded by 30% to 170% faster than in normal bottles. Our findings suggest that the ML-enhanced photodegradation may lead to a highly efficient solar water purification approach without a large solar collector size. Such an approach may be particularly suitable for portable transparent bottles in remote regions., Comment: Preprint for ACS ES&T Water

Chemical reactions in small droplets are extensively explored to accelerate the discovery of new materials, increase efficiency and specificity in catalytic biphasic conversion and in high throughput analytics. In this work, we investigate the local rate of gas-evolution reaction within femtoliter droplets immobilized on a solid surface. The growth rate of hydrogen microbubbles (> 500 nm in radius) produced from the reaction was measured online by high-resolution confocal microscopic images. The growth rate of bubbles was faster in smaller droplets, and of bubbles near the three-phase boundary in the same droplet. The results were consistent for both pure and binary reacting droplets and on substrates of different wettability. Our theoretical analysis based on diffusion, chemical reaction, and bubble growth in a steady state predicted that the concentration of the reactant diffusing from the surrounding depended on the droplet size and the bubble location inside the droplet, in good agreement with experimental results. Our results reveal that the reaction rate may be spatially non-uniform in the reacting microdroplets. The findings may have implications for formulating chemical properties and uses of these droplets.

In this work, we unravel the role of surface properties of colloidal particles on the formation of supraparticles (clusters of colloidal particles) in a colloidal Ouzo droplet. Self-lubricating colloidal Ouzo droplets are an efficient and simple approach to form supraparticles, overcoming the challenge of the coffee stain effect in situ. Supraparticles are an efficient route to high-performance materials in various fields, from catalysis to carriers for therapeutics. Yet, the role of the surface of colloidal particles in the formation of supraparticles using Ouzo droplets remains unknown. Therefore, we used silica particles as a model system and compared sterically stabilized versus electrostatically stabilized silica particles - positively and negatively charged. Additionally, we studied the effect of hydration. Hydrated negatively charged silica particles and sterically stabilized silica particles form supraparticles. Conversely, dehydrated negatively charged silica particles and positively charged amine-coated particles form flat film-like deposits. Notably, the assembly process is different for all the four types of particles. The surface modifications alter (a) the contact line motion of the Ouzo droplet and (b) the particle-oil and particle-substrate interactions. These alterations modify the particle accumulation at the various interfaces, which ultimately determines the shape of the final deposit. Thus, by modulating the surface properties of the colloidal particles, we can tune the shape of the final deposit, from a spheroidal supraparticle to a flat deposit. In the future, this approach can be used to tailor the supraparticles for applications such as optics and catalysis, where the shape affects the functionality., Comment: 38 pages, 9 figures

The dissolution or growth of a droplet in a host liquid is an important part for processes like chemical extraction, chromatography or emulsification. In this work we look at the dissolution of a pair of vertically aligned droplets immersed in water, both experimentally and with numerical simulations. The liquids used for the droplets are long chain alcohols with a low but finite solubility in water and a significantly lower density than that of the host liquid. Therefore, a solutal plume is formed above of the bottom droplet and natural convection dominates the dissolution process. We monitor the volume of the droplets and the velocity field around them over time. When the liquids of the two droplets are the same, our previously found scaling laws for the Sherwood and Reynolds numbers as functions of the Rayleigh number (Dietrich et al., 2016, J. Fluid Mech.) can be applied to the lower droplet. However, remarkably, when the liquid of the top droplet is different than that of the bottom droplet the volume as function of time becomes non-monotonic, and an oscillatory Marangoni flow at the top droplet is observed. We identify the competition between solutal Marangoni flow and density driven convection as the origin of the oscillation, and numerically model the process., Comment: 29 pages, 8 figures

The removal of microbubbles from substrates is crucial for the efficiency of many catalytic and electrochemical gas evolution reactions in liquids. The current work investigates the coalescence and detachment of bubbles generated from catalytic decomposition of hydrogen peroxide. Self-propelled detachment, induced by the coalescence of two bubbles, is observed at sizes much smaller than those determined by buoyancy. Upon coalescence, the released surface energy is partly dissipated by the bubble oscillations, working against viscous drag. The remaining energy is converted to the kinetic energy of the out-of-plane jumping motion of the merged bubble. The critical ratio of the parent bubble sizes for the jumping to occur is theoretically derived from an energy balance argument and found to be in agreement with the experimental results. The present results provide both physical insight for the bubble interactions and practical strategies for applications in chemical engineering and renewable energy technologies like electrolysis.

The sensitive and reliable in-droplet chemical analysis benefits from the enhanced partition of an analyte into the droplets. This work, we will show that chemical reactions in surface nanodroplets can shift the partition of analytes from a highly diluted solution to the droplets. Seven types of organic acids with partition coefficients (LgP) ranging from -0.7 to 1.87 are used as model analytes dissolved in an oil solution that are extracted from the flow into aqueous nanodroplets immobilized on a substrate. The timescale of integrated extraction and reaction in droplets was represented by the decoloration time of the droplets. Our results show that the effective distribution coefficient of the analyte can be decreased by 3 to 11 times of the distribution coefficient of the analyte in the bulk liquids. The principle behind the significantly shifted partition is proposed to be enhanced the transfer of the analyte across the droplet surface. The chemical reaction in the droplets enhances the partition of the analyte from a highly diluted solution. Our results show that the interfacial behavior of the analyte may be advantageous as it may improve extraction and partition. Such enhanced extraction may be leveraged for sensitive chemical detection using reactive droplets.

Compartmentalizing reagents within small droplets is promising for highly efficient conversion and simplified procedures in many biphasic chemical reactions. In this work, surface nanodroplets (i.e., less than 100 nm in their maximal height) were employed to quantitatively understand the size effect on the chemical reaction rate of droplets. In our systems, a surface-active reactant in pure or binary nanodroplets reacted with the reactant in the bulk flow. Meanwhile, the product was removed from the droplet surface. The shrinkage rate of the nanodroplets was characterized by analyzing the lateral size as a function of time, where the droplet size was solely determined by chemical reaction rate at a given flow condition for the transport of the reactant and the product. We found that the overall kinetics increases rapidly with the decrease of droplets lateral radius R, as dR/dt ~ R^(-2). The faster increase in the concentration of the product in smaller droplets contributes to accelerating reaction kinetics. The enhancement of reaction rates from small droplet sizes was further confirmed when a non-reactive compound presented inside the droplets without reducing the concentrations of the reactant and the product on the droplet surface. The results of our study improve the understanding of chemical kinetics with droplets. Our findings highlight the effectiveness of small droplets for the design and control of enhanced chemical reactions in a broad range of applications.

How liquid transport occurs in confined spaces is relevant to many industrial and lab-scale processes, ranging from enhanced oil recovery to drug delivery systems. In this work, we investigate propelling microdroplets that form from liquid-liquid phase separation in a quasi-2D chamber, focusing on the direction and speed of microdroplets in response to local composition gradients. The confined ternary solution in our experiments comprises a model oil, a good solvent (ethanol) and a poor solvent (water). Depending on the initial solution composition, water-rich or oil-rich microdroplets, form and move spontaneously as the ternary solution mixes with and is displaced by water diffusing from a deep side channel. Microdroplet movement is followed in situ using high-speed bright-field imaging or fluorescence imaging when the solution is doped with a dye. Local ethanol composition gradients are estimated from the variation of fluorescence intensity in the local continuous liquid surrounding the mobile microdroplets. From phase separation of the ternary solution with high oil concentration, mobile oil-rich microdroplets form in a water-rich zone, accompanying the formation of water-rich microdroplets in an oil-rich zone. The fast movement of oil-rich microdroplets induces directional flow transport that mobilizes water-rich microdroplets close to the water-rich zone. The average microdroplet speed increases with the initial oil concentration in the ternary solution. The fastest speed of oil-rich microdroplets observed in our experiments is ~150 ${\mu}$m/s along the surface of a hydrophobic wall. The presence of a sharp ethanol composition gradient is the primary driving force for the fast movement of oil-rich microdroplets in confinement. Our results demonstrate the potential of enhancing liquid transport in confinement through composition gradients arising from phase separation., Comment: This is the authors' submitted version of the manuscript to Energy & Fuels

Interfacial stability is important for many processes involving heat and mass transfer across two immiscible phases. When this transfer takes place in the form of evaporation of a binary solution with one component being more volatile than the other, gradients in surface tension can arise. These gradients can ultimately destabilise the liquid-gas interface. In the present work, we study the evaporation of an ethanol-water solution, for which ethanol has a larger volatility. The solution is contained in a horizontal Hele-Shaw cell which is open from one end to allow for evaporation into air. A Marangoni instability is then triggered at the liquid-air interface. We study the temporal evolution of this instability by observing the effects that it has on the bulk of the liquid. More specifically, the growth of convective cells is visualized with confocal microscopy and the velocity field close to the interface is measured with micro-particle-image-velocimetry. The results of numerical simulations based on quasi 2D equations satisfactorily compare with the experimental observations, even without consideration of evaporative cooling, although this cooling can play an extra role in experiments. Furthermore, a linear stability analysis applied to a simplified version of the quasi 2D equations showed reasonably good agreement with the results from simulations at early times, when the instability has just been triggered and no coarsening has taken place. In particular, we find a critical Marangoni number below which a regime of stability is predicted., Comment: 32 pages, 11 figures, to be published in the Journal of Fluid Mechanics