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

设计并实现了一种格子气巨正则蒙特卡罗模拟方法（LGCMC），用于模拟微孔介质中的吸附位格。该方法将用于从头计算预测的（二元）气体混合物在金属有机框架的吸附等温线方面的能量携带分子（CH 4）的存储，从CH 4/CO 2混合物的分离CO2，和分离问题的混合物，包括CO 2，CO，CH 4，N2和，作为杂质，H2O。该方法依赖于准确的（4千焦/摩尔或更好）的量子化学计算的自由能的吸附为个别网站和分子之间的相互作用能在不同的网站。用目前的从头计算LGCMC方法，它是可能的重新评估的假设，通常应用的理想吸附溶液理论的气体混合物。

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.