Thermo-Osmosis in Charged Nanochannels: Effects of Surface Charge and Ionic Strength

Thermo-osmosis refers to fluid migration due to the temperature gradient. The mechanistic understanding of thermo-osmosis in charged nano-porous media is still incomplete, while it is important for several environmental and energy applications, such as low-grade waste heat recovery, wastewater recovery, fuel cells, and nuclear waste storage. This paper presents results from a series of molecular dynamics simulations of thermo-osmosis in charged silica nanochannels that advance the understanding of the phenomenon. Simulations with pure water and water with dissolved NaCl are considered. First, the effect of surface charge on the sign and magnitude of the thermo-osmotic coefficient is quantified. This effect was found to be mainly linked to the structural modifications of an aqueous electrical double layer (EDL) caused by the nanoconfinement and surface charges. In addition, the results illustrate that the surface charges reduce the self-diffusivity and thermo-osmosis of interfacial liquid. The thermo-osmosis was found to change direction when the surface charge density exceeds -0.03C · m^-2. It was found that the thermo-osmotic flow and self-diffusivity increase with the concentration of NaCl. The fluxes of solvent and solute are decoupled by considering the Ludwig-Soret effect of NaCl ions to identify the main mechanisms controlling the behavior. In addition to the advance in microscopic quantification and mechanistic understanding of thermo-osmosis, the work provides approaches to investigate a broader category of coupled heat and mass transfer problems in nanoscale space.