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Register a new userTheory of Freezing Point Depression in Charged Porous Media
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Freezing in charged porous media can induce significant pressure and cause damage to tissues and functional materials. We formulate a thermodynamically consistent theory to model freezing phenomena inside charged heterogeneous porous space. Two regimes are distinguished: free ions in open pore space lead to negligible effects of freezing point depression and pressure. On the other hand, if nano-fluidic salt trapping happens, subsequent ice formation is suppressed due to the high concentration of ions in the electrolyte. In this case, our theory predicts that freezing starts at a significantly lower temperature compared to pure water. In 1D, as the temperature goes even lower, ice continuously grows, until the salt concentration reaches saturation, all ions precipitate to form salt crystals, and freezing completes. Enormous pressure can be generated if initial salt concentration is high before salt entrapment. We show modifications to the classical nucleation theory, due to the trapped salt ions. Interestingly, although the freezing process is enormously changed by trapped salts, our analysis shows that the Gibbs-Thompson equation on confined melting point shift is not affected by the presence of the electrolyte.
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A remarkable variety of organisms and wet materials are able to endure temperatures far below the freezing point of bulk water. Cryo-tolerance in biology is usually attributed to anti-freeze proteins, and yet massive supercooling ($< -40^circ$C) is also possible in porous media containing only simple aqueous electrolytes. For concrete pavements, the common wisdom is that freeze-thaw damage results from the expansion of water upon freezing, but this cannot explain the large pressures ($> 10$~MPa) required to damage concrete, the observed correlation between pavement damage and de-icing salts, or the damage of cement paste loaded with benzene (which contracts upon freezing). In this Letter, we propose a different mechanism -- nanofluidic salt trapping -- which can explain the observations, using simple mathematical models of dissolved ions confined to thin liquid films between growing ice and charged surfaces. Although trapped salt lowers the freezing point, ice nucleation in charged pores causes enormous disjoining pressures via the rejected ions, until their removal by precipitation or surface adsorption at a lower temperatures releases the pressure and allows complete freezing. The theory is able to predict the non-monotonic salt-concentration dependence of freeze-thaw damage in concreter and provides a general framework to understand the origins of cryo-tolerance.
Colloidal particles hold promise for mobilizing and removing trapped immiscible fluids from porous media, with implications for key energy and water applications. Most studies focus on accomplishing this goal using particles that can localize at the immiscible fluid interface. Therefore, researchers typically seek to optimize the surface activity of particles, as well as their ability to freely move through a pore space with minimal deposition onto the surrounding solid matrix. Here, we demonstrate that deposition can, surprisingly, promote mobilization of a trapped fluid from a porous medium without requiring any surface activity. Using confocal microscopy, we directly visualize both colloidal particles and trapped immiscible fluid within a transparent, three-dimensional (3D) porous medium. We find that as non-surface active particles deposit on the solid matrix, increasing amounts of trapped fluid become mobilized. We unravel the underlying physics by analyzing the extent of deposition, as well as the geometry of trapped fluid droplets, at the pore scale: deposition increases the viscous stresses on trapped droplets, overcoming the influence of capillarity that keeps them trapped. Given an initial distribution of trapped fluid, this analysis enables us to predict the extent of fluid mobilized through colloidal deposition. Taken together, our work reveals a new way by which colloids can be harnessed to mobilize trapped fluid from a porous medium.
The motion of active polymers in a porous medium is shown to depend critically on flexibilty, activity and degree of polymerization. For given Peclet number, we observe a transition from localisation to diffusion as the stiffness of the chains is increased. Whereas stiff chains move almost unhindered through the porous medium, flexible ones spiral and get stuck. Their motion can be accounted for by the model of a continuous time random walk with a renewal process corresponding to unspiraling. The waiting time distribution is shown to develop heavy tails for decreasing stiffness, resulting in subdiffusive and ultimately caged behaviour.
Porous media with hierarchical structures are commonly encountered in both natural and synthetic materials, e.g., fractured rock formations, porous electrodes and fibrous materials, which generally consist of two or more distinguishable levels of pore structure with different characteristic lengths. The multiphase flow behaviours in hierarchical porous media have remained elusive. In this study, we investigate the influences of hierarchical structures in porous media on the dynamics of immiscible fingering during fluid-fluid displacement. By conducting a series of numerical simulations, we found that the immiscible fingering can be suppressed due to the existence of secondary porous structures. To characterise the fingering dynamics in hierarchical porous media, a phase diagram is constructed by introducing a scaling parameter, i.e., the ratio of time scales considering the combined effect of characteristic pore sizes and wettability. The findings present in this work provide a basis for further research on the application of hierarchical porous media for controlling immiscible fingerings.
We study the conformational properties of charged polymers in a solvent in the presence of structural obstacles correlated according to a power law $sim x^{-a}$. We work within the continuous representation of a model of linear chain considered as a random sequence of charges $q_i=pm q_0$. Such a model captures the properties of polyampholytes -- heteropolymers comprising both positively and negatively charged monomers. We apply the direct polymer renormalization scheme and analyze the scaling behavior of charged polymers up to the first order of an $epsilon=6-d$, $delta=4-a$-expansion.
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