Li Hengbo, Zhou Yunzhe, Chen Cheng, Li Yashuang, Liu Zheng, Wu Mingyan, Hong Maochun
College of Chemistry, Fuzhou University, Fuzhou 350108, China.
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
Inorg Chem. 2024 Nov 11;63(45):21548-21554. doi: 10.1021/acs.inorgchem.4c03735. Epub 2024 Oct 28.
Benefiting from highly tunable pore environments, some metal-organic frameworks (MOFs) have recently shown promising prospects in the separation of methanol-to-olefin (MTO) products (mainly CH and CH). However, the "trade-off" between gas storage capacity and selectivity always results in inefficient separation. In addition, poor stability of MOFs also limits practical separation applications. Herein, we have successfully assembled a layered Y-MOF () with bent diisophthalate ligands (HL), Y-O chains, and 2-fluorobenzoic acids. As expected, not only exhibits good chemical stability but also shows significant potential for CH/CH separation. For , the CH uptake at 298 K and 10 kPa is 63 cm/g, and the IAST selectivity of for CH/CH (V/V = 50/50) is calculated to be 20.5. To the best of our knowledge, both CH uptake and selectivity of surpass most porous materials. GCMC simulation indicates that the special supramolecular binding sites in have much stronger interactions with CH than CH molecules. More importantly, practical breakthrough experiments demonstrate that can effectively separate CH/CH (50/50) mixtures, thus obtaining high-purity CH and CH, respectively.
得益于高度可调节的孔环境，一些金属有机框架材料（MOFs）最近在甲醇制烯烃（MTO）产物（主要是CH₄和C₂H₄）的分离方面展现出了广阔的前景。然而，气体储存容量和选择性之间的“权衡”总是导致分离效率低下。此外，MOFs较差的稳定性也限制了其实际分离应用。在此，我们成功地组装了一种层状Y-MOF（），其含有弯曲的间苯二甲酸二酯配体（HL）、Y-O链和2-氟苯甲酸。正如预期的那样，不仅表现出良好的化学稳定性，而且在CH₄/C₂H₄分离方面也显示出巨大的潜力。对于，在298 K和10 kPa下的CH₄吸附量为63 cm³/g，对于CH₄/C₂H₄（V/V = 50/50）的IAST选择性经计算为20.5。据我们所知，的CH₄吸附量和选择性均超过了大多数多孔材料。GCMC模拟表明，中的特殊超分子结合位点与CH₄分子的相互作用比与C₂H₄分子的相互作用要强得多。更重要的是，实际突破实验表明能够有效地分离CH₄/C₂H₄（50/50）混合物，从而分别获得高纯度的CH₄和C₂H₄。
