Pressure Gradients Fail to Predict Diffusio-Osmosis

We present numerical simulations of diffusio-osmotic flow, i.e. the fluid flow generated by a concentration gradient along a solid-fluid interface. In our study, we compare a number of distinct approaches that have been proposed for computing such flows and compare them with a reference calculation based on direct, non-equilibrium Molecular Dynamics simulations. As alternatives, we consider schemes that compute diffusio-osmotic flow from the gradient of the chemical potentials of the constituent species and from the gradient of the component of the stress tensor parallel to the interface. We find that the approach based on treating chemical potential gradients as external forces acting on various species agrees with the direct simulations, thereby supporting the approach of Marbach et al. (J Chem Phys 146, 194701 (2017)). In contrast, an approach based on computing the gradients of the microscopic pressure tensor does not reproduce the direct non-equilibrium results.