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The prediction of colloid transport in unsaturated porous media in the presence of large energy barrier is hampered by scant information of the proportional retention by straining and attractive interactions at surface energy minima. This study aims to fill this gap by performing saturated and unsaturated column experiments in which colloid pulses were added at various ionic strengths (ISs) from 0.1 to 50 mM. Subsequent flushing with deionized water released colloids held at the secondary minimum. Next, destruction of the column freed colloids held by straining. Colloids not recovered at the end of the experiment were quantified as retained at the primary minimum. Results showed that net colloid retention increased with IS and was independent of saturation degree under identical IS and Darcian velocity. Attachment rates were greater in unsaturated columns, despite an over 3-fold increase in pore water velocity relative to saturated columns, because additional retention at the readily available air-associated interfaces (e.g., the air–water–solid [AWS] interfaces) is highly efficient. Complementary visual data showed heavy retention at the AWS interfaces. Retention by secondary minima ranged between 8% and 46% as IS increased, and was greater for saturated conditions. Straining accounted for an average of 57% of the retained colloids with insignificant differences among the treatments. Finally, retention by primary minima ranged between 14% and 35% with increasing IS, and was greater for unsaturated conditions due to capillary pinning. [ABSTRACT FROM AUTHOR]

Naturally occurring polymers such as organic matter have been known to inhibit aggregation and promote mobility of suspensions in soil environments by imparting steric stability. This increase in mobility can significantly reduce the water filtering capacity of soils, thus jeopardizing a primary function of the vadose zone. Improvements to classic filtration theory have been made to account for the known decrease in attachment efficiency of electrostatically stabilized particles, and more recently, of sterically stabilized particles traveling through simple and saturated porous media. In the absence of an established unsaturated transport expression, and in the absence of applicable theoretical approaches for suspensions with asymmetric and nonindifferent electrolytes, this study presents an empirical correlation to predict attachment efficiency (a) for electrosterically stabilized suspensions in unsaturated systems in the presence of nonideal electrolytes. We show that existing models fall short in estimating polymer-coated colloid deposition in unsaturated media. This deficiency is expected given that the models were developed for saturated conditions where the mechanisms controlling colloid deposition are significantly different. A new correlation is derived from unsaturated transport data and direct characterization of microspheres coated with natural organic matter over a range of pH and CaCl2 concentrations. The improvements to existing transport models include the following: adjustment for a restricted liquid-phase in the medium, development of a quantitative term to account for unsaturated transport phenomena, and adjustments in the relative contribution of steric stability parameters based on direct measurements of the adsorbed polymer layer characteristics. Differences in model formulation for correlations designed for saturated systems and the newly proposed correlation for unsaturated systems are discussed, and the performance of the new model against a comprehensive set of experimental observations is evaluated. [ABSTRACT FROM AUTHOR]

Colloids play an important role in facilitating transport of adsorbed contaminants in soils. Recent studies showed that under saturated conditions colloid retention was a function of its concentration. It is unknown if this is the case under unsaturated conditions. In this study, the effect of colloid concentration on colloid retention was investigated in unsaturated columns by increasing concentrations of colloid influents with varying ionic strength. Colloid retention was observed in situ by bright field microscopy and quantified by measuring colloid breakthrough curves. In our unsaturated experiments, greater input concentrations resulted in increased colloid retention at ionic strength above 0.1 mM, but not in deionized water (i.e., 0 mM ionic strength). Bright field microscope images showed that colloid retention mainly occurred at the solid—water interface and wedge—shaped air—water—solid interfaces, whereas the retention at the grain—grain contacts was minor. Some colloids at the air—water—solid interfaces were rotating and oscillating and thus trapped. Computational hydrodynamic simulation confirmed that the wedge-shaped air—water—solid interface could form a "hydrodynamic trap" by retaining colloids in its low velocity vortices. Direct visualization also revealed that colloids once retained acted as new retention sites for other suspended colloids at ionic strength greater than 0.1 mM and thereby could explain the greater retention with increased input concentrations. Derjaguin—Landau—Verwey—Overbeek (DLVO) energy calculations support this concept. Finally, the results of unsaturated experiments were in agreement with limited saturated experiments under otherwise the same conditions. [ABSTRACT FROM AUTHOR]

Colloid deposition in granular media is relevant to numerous environmental problems. Classic filtration models assume a homogeneous pore space and largely ignore colloid aggregation. However, substantial evidence exists on the ubiquity of aggregation within porous media, suggesting that deposition is enhanced by it. This work studies the deposition process in relation to aggregate size and structure. We demonstrate that aggregation is induced at typical groundwater velocities by comparing the repulsive DLVO force between particle pairs to the hydrodynamic shear force opposing it. Column experiments imaged with high-resolution X-ray computed tomography are used to measure aggregate structure and describe their morphology probability distribution and spatial distribution. Aggregate volume and surface area are found to be power-law distributed, while Feret diameter is exponentially distributed with some flow rate dependencies caused by erosion and restructuring by the fluid shear. Furthermore, size and shape of aggregates are heterogeneous in depth, where a small number of large aggregates control the concentration versus depth profile shape. The range of aggregate fractal dimensions found (2.22-2.42) implies a high potential for restructuring or breaking during transport. Shear-induced aggregation is not currently considered in macroscopic models for particle filtration, yet is critical to consider in the processes that control deposition.

This study demonstrates that the pattern assembly and attachment strength of colloids in an evaporating sessile droplet resting on a smooth substrate can be controlled by adding nonionic solutes (surfactant) to the solution. As expected, increasing the surfactant concentration leads to a decrease in initial surface tension of the drop, σ(0). For the range of initial surface tensions investigated (39-72 mN m(-1)), three distinct deposition patterns were produced: amorphous stains (σ(0) = 63-72 mN m(-1)), coffee-ring stains (σ(0) = 48-53 mN m(-1)), and concentric rings (σ(0) = 39-45 mN m(-1)). A flow-displacement system was used to measure the attachment strength of the dried colloids. Characteristic drying regimes associated with the three unique pattern formations are attributed to abrupt transitions of contact line dynamics during evaporation. The first transition from slipping- to pinned-contact line was found to be a direct result of the competition between mechanical instability of the droplet and the friction generated by pinned colloids at the contact line. The second transition from pinned- to recurrent-stick-rip-slip-contact line was caused by repeated liquid film rupturing from evaporation-intensified surfactant concentration. Data from flow-displacement tests indicate that attachment strength of dried particles is strongest for amorphous stains (lowest surfactant concentration) and weakest for concentric rings (highest surfactant concentration). The mechanism behind these observations was ascribed to the formation and adsorption of micelles onto colloid and substrate surfaces as the droplet solution evaporates. The range of attachment forces observed between the colloids and the solid substrate were well captured by extended-DLVO interactions accounting for van der Waals attraction, electric double layer repulsion, and micelle-protrusion repulsion. Both empirical and theoretical results suggest that an increasingly dense layer of adsorbed micellar-protrusions on colloid and substrate surfaces acts as a physical barrier that hinders strong van der Waals attractive interactions at close proximity. Thereby, colloid stains dried at higher surfactant concentrations are more easily detached from the substrate when dislodging forces are applied than stains dried at lower surfactant concentrations.