Bridging confined phase behavior of CH4-CO2 binary systems across scales

The Journal of Supercritical Fluids(2022)

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Phase behavior of confined fluids may deviate significantly from that of the bulk fluid due to the fluid–wall interactions being a significant portion of all intermolecular interactions under confinement. Despite recent advancements in understanding confined phase behavior of pure fluids, confined phase behavior of mixtures remains an understudied topic. In this work, we examine the confined phase behavior of a CH4-CO2 binary system by combining Monte Carlo (MC) simulations, a cubic equation of state (EoS), and the lattice Boltzmann method (LBM). First, the effects of confinement on density and phase distribution in nano-size pores are established using Gibbs Ensemble MC calculations, which produce precise results of liquid and vapor confined pressures and account for the modification of the phase change location. By comparing the phase envelopes of bulk and confined mixtures at a fixed temperature, it is observed that the phase envelopes shrink with reductions in pore size. Based on this observation, we extend a modified Peng–Robinson EoS, which was originally developed for pure fluids under confinement, to mixtures via van-der-Waals-type mixing rules and by accounting for shifts in the critical properties of confined CH4-CO2. The resulting phase envelopes are in good agreement with the MC data. In addition, a local density model is used in combination with the confined EoS to calculate adsorption isotherms of CH4-CO2 mixtures and to characterize the behavior of confined matter in nanopores. Finally, we incorporate this EoS in a multicomponent multiphase LBM that uses a pseudopotential model to represent intermolecular forces. This workflow utilizes multiscale simulation techniques to bridge the behavior of multicomponent systems across scales and to shed light on the confined phase behavior of CH4-CO2 binary systems.
Confined phase behavior,Carbon dioxide–methane mixtures,Molecular simulations,Equation of state,Lattice Boltzmann method
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