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Register a new userDrying paint: from micro-scale dynamics to mechanical instabilities
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Charged colloidal dispersions make up the basis of a broad range of industrial and commercial products, from paints to coatings and additives in cosmetics. During drying, an initially liquid dispersion of such particles is slowly concentrated into a solid, displaying a range of mechanical instabilities in response to highly variable internal pressures. Here we summarise the current appreciation of this process by pairing an advection-diffusion model of particle motion with a Poisson-Boltzmann cell model of inter-particle interactions, to predict the concentration gradients around a drying colloidal film. We then test these predictions with osmotic compression experiments on colloidal silica, and small-angle x-ray scattering experiments on silica dispersions drying in Hele-Shaw cells. Finally, we use the details of the microscopic physics at play in these dispersions to explore how two macroscopic mechanical instabilities -- shear-banding and fracture -- can be controlled.
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A quantitative understanding of the evaporative drying kinetics and nucleation rates of aqueous based aerosol droplets is important for a wide range of applications, from atmospheric aerosols to industrial processes such as spray drying. Here, we introduce a numerical model for interpreting measurements of the evaporation rate and phase change of drying free droplets made using a single particle approach. We explore the evaporation of aqueous sodium chloride and sodium nitrate solution droplets. Although the chloride salt is observed to reproducibly crystallise at all drying rates, the nitrate salt solution can lose virtually all of its water content without crystallising. The latter phenomenon has implications for our understanding of the competition between the drying rate and nucleation kinetics in these two systems. The nucleation model is used in combination with the measurements of crystallisation events to infer nucleation rates at varying equilibrium state points, showing that classical nucleation theory provides a good description of the crystallisation of the chloride salt but not the nitrate salt solution droplets. The reasons for this difference are considered.
Layers obtained by drying a colloidal dispersion of silica spheres are found to be a good benchmark to test the elastic behaviour of porous media, in the challenging case of high porosities and nano-sized microstructures. Classically used for these systems, Kendalls approach explicitely considers the effect of surface adhesive forces onto the contact area between the particles. This approach provides the Youngs modulus using a single adjustable parameter (the adhesion energy) but provides no further information on the tensorial nature and possible anisotropy of elasticity. On the other hand, homogenization approaches (e.g. rule of mixtures, Eshelby, Mori-Tanaka and self-consistent schemes), based on continuum mechanics and asymptotic analysis, provide the stiffness tensor from the knowledge of the porosity and the elastic constants of the beads. Herein, the self-consistent scheme accurately predicts both bulk and shear moduli, with no adjustable parameter, provided the porosity is less than 35%, for layers composed of particles as small as 15 nm in diameter. Conversely, Kendalls approach is found to predict the Youngs modulus over the full porosity range. Moreover, the adhesion energy in Kendalls model has to be adjusted to a value of the order of the fracture energy of the particle material. This suggests that sintering during drying leads to the formation of covalent siloxane bonds between the particles.
Viscoelastic fluids exhibit elastic instabilities in simple shear flow and flow through curved streamlines. Surprisingly, we found in a porous medium such fluids show strikingly different hydrodynamic instabilities depicted by very large sideways excursions and presence of fast and slow moving lanes which have not been reported before. Particle image velocimetry (PIV) measurements through a pillared microchannel, provide experimental evidence of such instabilities at very low Reynolds number (< 0.01). We observe a transition from a symmetric laminar to an asymmetric flow, which finally transforms to a nonlinear aperiodic flow with strong lateral movements. The instability is characterized by a rapid increase in spatial and temporal fluctuations of velocity components and pressure at a critical Deborah number (De). Our experiments reveal the presence of a fascinating interplay between pore space and fluid rheology.
We employ a novel fluid-particle model to study the shearing behavior of granular soils under different saturation levels, ranging from the dry material via the capillary bridge regime to higher saturation levels with percolating clusters. The full complexity of possible liquid morphologies is taken into account, implying the formation of isolated arbitrary-sized liquid clusters with individual Laplace pressures that evolve by liquid exchange via films on the grain surface. Liquid clusters can grow in size, shrink, merge and split, depending on local conditions, changes of accessible liquid and the pore space morphology determined by the granular phase. This phase is represented by a discrete particle model based on Contact Dynamics, where capillary forces exerted from a liquid phase add to the motion of spherical particles. We study the macroscopic response of the system due to an external compression force at various liquid contents with the help of triaxial shear tests. Additionally, the change in liquid cluster distributions during the compression due to the deformation of the pore space is evaluated close to the critical load.
We report on a new type of experiment that enables us to monitor spatially and temporally heterogeneous dynamic properties in complex fluids. Our approach is based on the analysis of near-field speckles produced by light diffusely reflected from the superficial volume of a strongly scattering medium. By periodic modulation of an incident speckle beam we obtain pixel-wise ensemble averages of the structure function coefficient, a measure of the dynamic activity. To illustrate the application of our approach we follow the different stages in the drying process of a colloidal thin film. We show that we can access ensemble averaged dynamic properties on length scales as small as ten micrometers over the full field of view.
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