Abstract
Understanding the mechanism of gas-sorbent interactions is of fundamental importance for the design of improved gas storage materials. Here we report the binding domains of carbon dioxide and acetylene in a tetra-amide functionalized metal-organic framework, MFM-188, at crystallographic resolution. Although exhibiting moderate porosity, desolvated MFM-188a exhibits exceptionally high carbon dioxide and acetylene adsorption uptakes with the latter (232 cm3 g−1 at 295 K and 1 bar) being the highest value observed for porous solids under these conditions to the best of our knowledge. Neutron diffraction and inelastic neutron scattering studies enable the direct observation of the role of amide groups in substrate binding, representing an example of probing gas-amide binding interactions by such experiments. This study reveals that the combination of polyamide groups, open metal sites, appropriate pore geometry and cooperative binding between guest molecules is responsible for the high uptakes of acetylene and carbon dioxide in MFM-188a.
Highlights
Understanding the mechanism of gas-sorbent interactions is of fundamental importance for the design of improved gas storage materials
A 3D plot summarising the relationship between BET surface area, density of ‘open metal sites (OMSs) þ functional groups’ in the structure, and uptake of C2H2 is shown in Fig. 3c for a number of the best metal-organic frameworks (MOFs) reported to date
MFM-188a displays a suitably high BET surface area and high density of binding sites owing to its framework topology and pore geometry, and shows a record high C2H2 uptake
Summary
Understanding the mechanism of gas-sorbent interactions is of fundamental importance for the design of improved gas storage materials. We report the binding domains of carbon dioxide and acetylene in a tetra-amide functionalized metal-organic framework, MFM-188, at crystallographic resolution. This study reveals that the combination of polyamide groups, open metal sites, appropriate pore geometry and cooperative binding between guest molecules is responsible for the high uptakes of acetylene and carbon dioxide in MFM-188a. The emergence of metal-organic frameworks (MOFs) as multifunctional materials results from the combination of their high porosity and precise design of pore functionality. 13) and D2, N2 and O2-loaded Cr-BTT14 (BTT3 À 1⁄4 1⁄4 1,3,5-benzenetristetrazolate) clearly conclude that OMSs are the primary binding domains for guest molecules This observation has been further evidenced by neutron spectroscopic experiments, which confirmed the large translational and/or rotational hindrance of bound guest molecules at OMSs15. Experimental observation of the precise role of amides in guest binding in MOFs is still largely lacking
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