Spatio-Temporal Imaging of Instability and Transport of Pickering Nanodroplets in Porous Media

Featuring a large specific surface area with associated high reactivity, nanomaterials in various morphologies are ideal candidates for improved oil recovery (IOR), enhanced geothermal systems (EGS) and carbon capture utilization and storage (CCUS).  Encapsulation of solid nanomaterials within an oil-in-water (O/W) emulsion (i.e., Pickering emulsion) has been employed to prevent the aggregation and deposition of the nanomaterials in subsurface reservoirs in recent decades. Here, the dispersed phase droplets were decreased to nanoscale through a utilizable procedure. These nanodroplets were stabilized solely by polymer-coated magnetic iron oxide nanoparticles. Low-field NMR and X-ray CT were employed to constantly monitor the stability of Pickering nanoemulsions until phase separation. The polydisperse nanoemulsions are more easily separated due to the severely inhomogeneous chemical potentials of the emulsion droplets. Experimental and theoretical modeling results reveal that the Ostwald ripening is the main instability mechanism for nanoemulsions due to the very small droplets associated with a high surface area. The insolubility of long-chain hydrocarbons in water acts as a kinetic barrier to Ostwald ripening, making those nanoemulsions, both the Pickering and Classical (which is formed only by polymer) ones, inherently stable to Ostwald ripening.

The transport and retention of the Pickering nanodroplets in porous media is examined by X-ray CT imaging. Accordingly, in-situ transport of the nanoemulsions in a water-saturated sandpack was quantified spatiotemporally through X-ray CT. Effluents were collected and analyzed to further comprehend the nanoemulsion displacement and retention in porous media. Experimental results demonstrate that accumulation and retention of the nanodroplets in porous media are stimulated by ionic strength, nanodroplet size distribution, and nanoparticle wettability. Three transport modes in porous media (flow through with minimal retention, migration of accumulated nanodroplets, and retention of accumulated nanodroplets) can be achieved through carefully designing the nanoemulsion system.

These findings shed light on the fundamental understanding of the (nano-)colloidal dispersions transport in porous media and provide implications for IOR, EGS, and CCUS.