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Thesis Title: Transport and Irreversible Retention of Hydrophobic Nanoparticles by Fluid-Fluid and Fluid-Solid Interfaces in Porous Media

Abstract:

Hydrophobic nanoparticle (NP) transport in porous media has implications for aquifer transport and retention of a wide range of contaminants that infiltrate water resources and threaten human health as well as aquatic environments. Comprehension of NP transport and interactions with hydrophobic surfaces and interfaces -given their ubiquity in porous aquifers- is essential for groundwater remediation from organic contaminants, toxic engineered NPs, and nanoplastics.

This research investigates the transport and attachment of hydrophobic NPs under varying physicochemical conditions in saturated and unsaturated porous media by integrating experimental observations across multiple scales, theoretical extended-DLVO predictions, and numerical modeling. A non-toxic, negatively-charged, hydrophobic model NP system synthesized from ethyl cellulose (EC), and exhaustively characterized for colloidal stability and interfacial interactions, was employed to systematically explore NP interactions with fluid-fluid and solid-fluid interfaces.

The upscaling capability of an advection-dispersion-retention continuum model was compared vis-à-vis a pore network model of irreversible NP attachment onto fluid interfaces in 3D columns packed with spherical glass beads, showing that the latter captures key pore-scale dynamics such as bypassed interfaces, slow-moving corner flows, and diffusion-dominated retention.

Transport experiments in 2D microfluidic pore networks confirm that the dynamics of NP retention in unsaturated porous media depend not only on the saturation of the non-wetting phase, but also on its connectivity and the accessibility of immobile fluid-fluid interfaces.