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Postsynthetic Functionalization of Mg-MOF-74 with Tetraethylenepentamine: Structural Characterization and Enhanced CO2 Adsorption.

Postsynthetic functionalization of magnesium 2,5-dihydroxyterephthalate (Mg-MOF-74) with tetraethylenepentamine (TEPA) resulted in improved CO2 adsorption performance under dry and humid conditions. XPS, elemental analysis, and neutron powder diffraction studies indicated that TEPA was incorporated throughout the MOF particle, although it coordinated preferentially with the unsaturated metal sites located in the immediate proximity to the surface. Neutron and X-ray powder diffraction analyses showed that the MOF structure was preserved after amine incorporation, with slight changes in the lattice parameters. The adsorption capacity of the functionalized amino-Mg-MOF-74 (TEPA-MOF) for CO2 was as high as 26.9 wt % versus 23.4 wt % for the original MOF due to the extra binding sites provided by the multiunit amines. The degree of functionalization with the amines was found to be important in enhancing CO2 adsorption, as the optimal surface coverage improved performance and stability under both pure CO2 and CO2/H2O coadsorption, and with partially saturated surface coverage, optimal CO2 capacity could be achieved under both wet and dry conditions by a synergistic binding of CO2 to the amines as well as metal centers.