3 years ago

Understanding the Effect of Ligands on C2H2 Storage and C2H2/CH4, C2H2/CO2 Separation in Metal–Organic Frameworks with Open Cu(II) Sites

Understanding the Effect of Ligands on C2H2 Storage and C2H2/CH4, C2H2/CO2 Separation in Metal–Organic Frameworks with Open Cu(II) Sites
Fan Li, Yuanyuan Cheng, Hao Zhou, Siyuan Yang, Youyong Li, Yujin Ji, Lifeng Ding
Safe and efficient storage and separation of acetylene pose a significant challenge in industry. In this study, we investigated 11 open Cu(II) site (OCS)-based metal–organic frameworks (MOFs) formed by various organic ligands for their C2H2 adsorption capacities and their C2H2/CO2, C2H2/CH4 separation performance using both grand canonical Monte Carlo (GCMC) simulations and density functional theory (DFT) calculations. Our simulations revealed that both OCSs and organic ligands of the MOFs play key roles in promoting C2H2 storage capacity and the separation of C2H2 over CH4 and CO2 under 2 bar. Judicious selection of organic ligands with suitable dimensions and functional sites, such as methyl group, Lewis basic nitrogen site, and fluorine group, can facilitate C2H2 adsorption in addition to OCS and help distinguish C2H2 from CH4 and CO2. Short ligands presented in the MOFs, such as MOF-505 which gives the highest volumetric C2H2 storage capacity under 2 bar, not only increase the density of OCSs but also create overlapped interaction regions for guest molecules. GCMC simulation results suggested that NOTT-106 had the second highest volumetric C2H2 storage capacity because of its methyl functionalized ligands. DFT calculations however suggested that the Lewis basic nitrogen functionalized ligand of ZJU-40 might have a stronger affinity with C2H2 than that of NOTT-106, which indicated that C2H2 storage capacity in ZJU-40 should be better than that in NOTT-106. In contrast, MOF-505, ZJU-40, and NOTT-108 showed excellent C2H2/CH4 separation performance as well as modest C2H2/CO2 separation capability.

Publisher URL: http://dx.doi.org/10.1021/acs.jpcc.7b08370

DOI: 10.1021/acs.jpcc.7b08370

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