Journal of Chemical and Engineering Data, Vol.65, No.3, 1159-1171, 2020
Employing SAFT Coarse-Grained Force Fields for the Molecular Simulation of Thermodynamic and Transport Properties of CO2-n-Alkane Mixtures
We report an assessment of the predictive and correlative capability of the SAFT coarse-grained force field as applied to mixtures of CO2 with n-decane and n-hexadecane. We obtain the pure and cross-interaction parameters by matching simulations to experimental phase equilibrium behavior and transfer these parameters to predict shear viscosities. We apply both equilibrium (based on the Green-Kubo formulation) and nonequilibrium (based on the application of an external force to generate an explicit velocity field) algorithms. Single- and two-site models are explored for CO2, and while for volumetric properties both models provide good results, only the model that aligns with the molecular shape is found to be robust when describing highly asymmetric binary mixtures over wide ranges of temperature and pressure. While the models provide good quantitative predictions of viscosity, deviations among the algorithms and with experimental data are encountered for binary mixtures involving longer chain fluids, and in particular at high-pressure and low-temperature states.