Non-equilibrium molecular dynamics simulation study on permeation phenomena of LJ particles in slit-shaped membranes with periodic belt-like heterogeneous surfaces

In order to make clear the relationship between the pore structure and the diffusivity, we have carried out permeation simulations of pure gases through simple model membranes by using the external-field non-equilibrium molecular dynamics method. As the membrane, we model slit-shaped pores with periodic belt-like heterogeneous pore surfaces which are caused by the upheaval of surface atoms. Applying simulation results for membranes with several upheaval interval distances to Maxwell-Stefan (MS) theory, we calculate the effects of the molecular loading of permeating molecules in the pores on MS diffusivity (D_MS). In addition, the permeation potential barrier is estimated as the difference between the maximum and minimum permeation potential energies. The effect of the molecular loading on the permeation potential barrier and the D_MS are in inverse proportion. It is noted that, when the width of the adsorption area in the permeation direction is not common multiples of the molecular diameter, the permeation potential barrier decreases with the increase in the molecular loading. This is because the positive force against the permeation direction is caused to the permeating molecules by interactions with permeating molecules in the adsorpton area between adjacent upheavals. Therefore, we could suggest that the key factor for controlling diffusion property is the structural relationship between the adsorption area and the permeating molecules.