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1. Diffusiophoresis: a novel transport mechanism - fundamentals, applications, and future opportunities

   https://doi.org/10.3389/fsens.2023.1322906  

   Ganguly, Arkava; Alessio, Benjamin M.; Gupta, Ankur (November 2023, Frontiers in Sensors)

   Diffusiophoresis involves the movement of colloidal-scale entities in response to concentration gradients of a solute. It is broadly categorized into two types: passive and active diffusiophoresis. In passive diffusiophoresis, external concentration gradients drive the motion, while in active diffusiophoresis, the colloidal entity itself assists in generating the gradients. In this perspective, we delve into the fundamental processes underlying passive and active diffusiophoresis and emphasize how prevalent both kinds of diffusiophoresis are in colloidal and natural systems. In particular, we highlight the colloidal focusing feature in passive diffusiophoresis and discuss how it underpins the variety of experimental observations and applications such as low-cost zetasizers, water filtration, and biological pattern formation. For active diffusiophoresis, we emphasize the dependence of particle trajectory on its shape and surface heterogeneity, and discuss how this dictates the applications such as drug delivery, removal of microplastics, and self-repairing materials. Finally, we offer insights and ideas regarding future opportunities in diffusiophoresis. 

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2. Effect of particle shape on stratification in drying films of binary colloidal mixtures

   https://doi.org/10.1063/5.0270685  

   Liu, Binghan; Grest, Gary S; Cheng, Shengfeng (July 2025, The Journal of Chemical Physics)

   The role of particle shape in evaporation-induced auto-stratification in polydisperse colloidal suspensions is explored with molecular dynamics simulations of mixtures of spheres and aspherical particles. A unified framework based on the competition between diffusion and diffusiophoresis is proposed to understand the effects of shape and size dispersity. In general, particles diffusing more slowly (e.g., larger particles) tend to accumulate more strongly at the evaporation front. However, larger particles have larger surface areas and therefore greater diffusiophoretic mobility. Hence, they are more likely to be driven away from the evaporation front via diffusiophoresis. For a rapidly dried bidisperse suspension containing small and large spheres, the competition leads to “small-on-top” stratification. Here, we employ a computational model in which the diffusion coefficient is inversely proportional to particle mass. For a mixture of spheres and aspherical particles with similar mass, the diffusion contrast is reduced, and the spheres are always enriched at the evaporation front as they have the smallest surface area for a given mass and, therefore, the lowest diffusiophoretic mobility. For a mixture of solid and hollow spheres that have the same outer radius and thus the same surface area, the diffusiophoretic contrast is suppressed, and the system is dominated by diffusion. Consequently, the solid spheres, which have a larger mass and diffuse more slowly, accumulate on top of the hollow spheres. Finally, for a mixture of thin disks and long rods that differ significantly in shape but have similar mass and surface area, both diffusion and diffusiophoresis contrasts are suppressed, and the mixture does not stratify. 

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3. Artificial chemotaxis under electrodiffusiophoresis

   https://doi.org/10.1016/j.jcis.2024.08.004  

   Silvera_Batista, Carlos A; Wang, Kun; Blake, Hannah; Nwosu-Madueke, Vivian; Marbach, Sophie (January 2025, Journal of Colloid and Interface Science)

   Hypothesis Through a large parameter space, electric fields can tune colloidal interactions and forces leading to diverse static and dynamical structures. So far, however, field-driven interactions have been limited to dipole-dipole and hydrodynamic contributions. Nonetheless, in this work, we propose that under the right conditions, electric fields can also induce interactions based on local chemical fields and diffusiophoretic flows. Experiments Herein, we present a strategy to generate and measure 3D chemical gradients under electric fields. In this approach, faradaic reactions at electrodes induce global pH gradients that drive long-range transport through electrodiffusiophoresis. Simultaneously, the electric field induces local pH gradients by driving the particle's double layer far from equilibrium. Findings As a result, while global pH gradients lead to 2D focusing away from electrodes, local pH gradients induce aggregation in the third dimension. Evidence points to a mechanism of interaction based on diffusiophoresis. Interparticle interactions display a strong dependence on surface chemistry, zeta potential and diameter of particles. Furthermore, pH gradients can be readily tuned by adjusting the voltage and frequency of the electric field. For large Péclet numbers, we observed a collective chemotactic-like collapse of particles. Remarkably, such collapse occurs without reactions at a particle's surface. By mixing particles with different sizes, we also demonstrate, through experiments and Brownian dynamics simulations, the emergence of non-reciprocal interactions, where small particles are more drawn towards large ones. 

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4. Diffusiophoresis in one-dimensional solute gradients

   https://doi.org/10.1039/c7sm01588g  

   Ault, Jesse T.; Warren, Patrick B.; Shin, Sangwoo; Stone, Howard A. (January 2017, Soft Matter)

   The diffusiophoretic motion of suspended colloidal particles under one-dimensional solute gradients is solved using numerical and analytical techniques. Similarity solutions are developed for the injection and withdrawal dynamics of particles into semi-infinite pores. Furthermore, a method of characteristics formulation of the diffusion-free particle transport model is presented and integrated to realize particle trajectories. Analytical solutions are presented for the limit of small particle diffusiophoretic mobility Γ p relative to the solute diffusivity D s for particle motions in both semi-infinite and finite domains. Results confirm the build up of local maxima and minima in the propagating particle front dynamics. The method of characteristics is shown to successfully predict particle motions and the position of the particle front, although it fails to accurately predict suspended particle concentrations in the vicinity of sharp gradients, such as at the particle front peak seen in some injection cases, where particle diffusion inevitably plays an important role. Results inform the design of applications in which the use of applied solute gradients can greatly enhance particle injection into and withdrawal from pores. 

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5. Diffusioosmosis-driven dispersion of colloids: a Taylor dispersion analysis with experimental validation

   https://doi.org/10.1017/jfm.2022.321  

   Alessio, Benjamin M.; Shim, Suin; Gupta, Ankur; Stone, Howard A. (July 2022, Journal of Fluid Mechanics)

   Diffusiophoresis refers to the movement of colloidal particles in the presence of a concentration gradient of a solute and enables directed motion of colloidal particles in geometries that are inaccessible, such as dead-end pores, without imposing an external field. Previous experimental reports on dead-end pore geometries show that, even in the absence of mean flow, colloidal particles moving through diffusiophoresis exhibit significant dispersion. Existing models of diffusiophoresis are not able to predict the dispersion and thus the comparison between the experiments and the models is largely qualitative. To address these quantitative differences between the experiments and models, we derive an effective one-dimensional equation, similar to a Taylor dispersion analysis, that accounts for the dispersion created by diffusioosmotic flow from the channel sidewalls. We derive the effective dispersion coefficient and validate our results by comparing them with direct numerical simulations. We also compare our model with experiments and obtain quantitative agreement for a wide range of colloidal particle sizes. Our analysis reveals two important conclusions. First, in the absence of mean flow, dispersion is driven by the flow created by diffusioosmotic wall slip such that spreading can be reduced by decreasing the channel wall diffusioosmotic mobility. Second, the model can explain the spreading of colloids in a dead-end pore for a wide range of particle sizes. We note that, while the analysis presented here focuses on a dead-end pore geometry with no mean flow, our theoretical framework is general and can be adapted to other geometries and other background flows. 

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