Ab initio simulation of isotherms for gas mixtures in metal-organic frameworks

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A Lattice Gas Grand Canonical Monte Carlo simulation method (LGCMC) is designed and implemented for a lattice of adsorption sites in microporous media. The method will be used for the ab initio prediction of adsorption isotherms of (binary) gas mixtures in metal-organic frameworks with regard to the storage of energy carrying molecules (CH4), the separation of CO2 from CH4/CO2 mixtures, and for separation problems for mixtures including CO2, CO, CH4, N2 and, as impurity, H2O. The method relies on accurate (4 kJ/mol or better) quantum chemical calculations of free energies of adsorption for individual sites and of interaction energies between molecules at different sites. With the present ab initio LGCMC method it is possible to reassess the assumptions of the usually applied Ideal Adsorbed Solution Theory for gas mixtures.