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Amides Do Not Always Work: Observation of Guest Binding in an Amide-Functionalized Porous Metal–Organic Framework

Benson, Oguarabau, da Silva, Ivan, Argent, Stephen P., Cabot, Rafel, Savage, Mathew, Godfrey, Harry G.W., Yan, Yong, Parker, Stewart F., Manuel, Pascal, Lennox, Matthew J., Mitra, Tamoghna, Easun, Timothy L., Lewis, William, Blake, Alexander J., Besley, Elena, Yang, Sihai, Schröder, Martin
Journal of the American Chemical Society 2016 v.138 no.45 pp. 14828-14831
adsorption, amides, carbon dioxide, geometry, porosity, spectroscopy
An amide-functionalized metal organic framework (MOF) material, MFM-136, shows a high CO₂ uptake of 12.6 mmol g–¹ at 20 bar and 298 K. MFM-136 is the first example of an acylamide pyrimidyl isophthalate MOF without open metal sites and, thus, provides a unique platform to study guest binding, particularly the role of free amides. Neutron diffraction reveals that, surprisingly, there is no direct binding between the adsorbed CO₂/CH₄ molecules and the pendant amide group in the pore. This observation has been confirmed unambiguously by inelastic neutron spectroscopy. This suggests that introduction of functional groups solely may not necessarily induce specific guest–host binding in porous materials, but it is a combination of pore size, geometry, and functional group that leads to enhanced gas adsorption properties.