The adsorption and separation capabilities of metal-organic frameworks (MOFs) for CO2 and CH4 gas mixtures were studied by grand canonical Monte Carlo (GCMC) simulations. Three sub-families (M-MOF-74, M-MIL-53 and [M(atz)(bdc)0.5]) (M=Mg, Co, Ni, Zn, Al, Cr) MOFs with different metal ligands were investigated. Simulation results showed that the CO2 adsorption capability of Mg-MOF-74 exceeded the others at high pressures; both amine functionalized [Zn(atz)(bdc)0.5] and [Co(atz)(bdc)0.5] MOFs had superior CO2 separation performance at low pressures. The radial distribution functions and the overlapping snapshots of CO2 adsorption showed that in each sub-family of MOFs, different metal ligands affected their CO2 adsorption configuration and resulted in their different adsorption and separation capabilities. This work could provide some guidance for the design and development of new high performance MOFs for CO2 and CH4 separation.%采用巨正则Monte Carlo法（GCMC），对CH4/CO2混合气体体系基于金属-有机骨架材料（MOFs）的吸附分离进行了模拟研究。吸附分离材料涉及3个系列（M-MOF-74、M-MIL-53和[M(atz)(bdc)0.5]）（M=Mg, Co, Ni, Zn, Al, Cr）不同金属配位的8种MOF材料。研究表明，Mg-MOF-74的CO2吸附性能在高压下优于其他材料；在低压时，拥有大量氨基官能团的[Zn(atz)(bdc)0.5]和[Co(atz)(bdc)0.5]材料有更高效的CO2分离性能。通过径向分布函数和CO2吸附构型快照重叠图进一步分析发现，各个系列材料不同金属配位对CO2吸附构型的影响造成了材料吸附分离性能有较大的不同。研究结果能够为实验上设计和开发新型高效CO2和CH4吸附分离MOFs材料提供启发。
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