The versatile chemistry of metal organic frameworks (MOFs) enables them for many applications involving the recognition and manipulation of molecules. Hierarchical MOF features not only bring in additional chemical properties, they also create mesoporosity that extends the pore size distribution of bulk MOF particles. In this work, we demonstrate heterometallic hierarchical MOF nanoparticles formed by intergrowth of pillared MOFs. Pillared MOF MI2(ndc)2(dabco) (MI=Co, Ni, Cu, Zn, ndc=naphthelenedicarboxylic acid, dabco=1,4-diazabicyclo[2.2.2]octane) nanoparticles were synthesized with various morphologies, on which MII2(ndc)2(dabco) (MII=Co, Ni, Cu, Zn) nanoparticles were intergrown. Several parameters related to the system were exploited to give a general strategy of intergrowth of pillared MOF nanoparticles, based on which all 12 pairs of heterometallic heteroepitaxial growths among Co, Ni, Cu and Zn were achieved. The intergrown particles preserved the structure, crystallinity, and morphology of their respective primary particles, while creating additional mesoporosity for gas adsorption. Adsorption of hydrocarbons (CH4, ethane, ethene, propane, and propene) at pressures up to 10 bar (absolute) was performed on the MOFs. The hierarchical MOFs have shown increased adsorption of hydrocarbons at low pressures, and IAST selectivity of propane/methane as high as 53 were observed (total pressure 1 bar, CH4 mole fraction: 0.8), suggesting the hierarchical materials can be used for adsorptive removal of natural gas liquids from crude natural gas.

Hierarchical MOFs nanoparticles from intergrowth and their applications in light hydrocarbon/methane separation

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.