Tailoring Porosity and Rotational Dynamics in a Series of Octacarboxylate Metal-Organic Frameworks
| Autor: | Timothy L. Easun, Daniil I. Kolokolov, Florian Moreau, Matthew J. Lennox, Harriott Nowell, Elena Besley, Dailly Anne M, Alexander G. Stepanov, Alexander J. Blake, William Lewis, Martin Schröder, Sihai Yang |
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| Jazyk: | angličtina |
| Rok vydání: | 2017 |
| Předmět: |
Multidisciplinary
Materials science Ligand Nanotechnology 02 engineering and technology Nuclear magnetic resonance spectroscopy 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences 0104 chemical sciences Chemical engineering Deuterium Physical Sciences Gravimetric analysis QD Metal-organic framework Elongation 0210 nano-technology Porosity Bar (unit) |
| Zdroj: | Moreau, F, Kolokolov, D I, Stepanov, A G, Easun, T L, Dailly, A, Lewis, W, Blake, A J, Nowell, H, Lennox, M, Besley, E, Yang, S & Schroder, M 2017, ' Tailoring Porosity and Rotational Dynamics in a Series of Octacarboxylate Metal-Organic Frameworks ', Proceedings of the National Academy of Sciences, vol. 114, no. 12, pp. 3056-3061 . https://doi.org/10.1073/pnas.1615172114 Moreau, F, Kolokolov, D I, Stepanov, A G, Easun, T L, Dailly, A, Lewis, W, Blake, A J, Nowell, H, Lennox, M J, Besley, E, Yang, S & Schröder, M 2017, ' Tailoring porosity and rotational dynamics in a series of octacarboxylate metal-organic frameworks ', Proceedings of the National Academy of Sciences of the United States of America, vol. 114, no. 12, pp. 3056-3061 . https://doi.org/10.1073/pnas.1615172114 |
| ISSN: | 0027-8424 |
| DOI: | 10.1073/pnas.1615172114 |
| Popis: | Modulation and precise control of porosity of metal-organic frameworks (MOFs) is of critical importance to their materials function. Here we report modulation of porosity for a series of isoreticular octacarboxylate MOFs, denoted MFM-180 to MFM-185, via a strategy of selective elongation of metal-organic cages. Owing to the high ligand connectivity, these MOFs do not show interpenetration, and are robust structures that have permanent porosity. Interestingly, activated MFM-185a shows a high Brunauer–Emmett–Teller (BET) surface area of 4,734 m2 g−1 for an octacarboxylate MOF. These MOFs show remarkable CH4 and CO2 adsorption properties, notably with simultaneously high gravimetric and volumetric deliverable CH4 capacities of 0.24 g g−1 and 163 vol/vol (298 K, 5–65 bar) recorded for MFM-185a due to selective elongation of tubular cages. The dynamics of molecular rotors in deuterated MFM-180a-d16 and MFM-181a-d16 were investigated by variable-temperature 2H solid-state NMR spectroscopy to reveal the reorientation mechanisms within these materials. Analysis of the flipping modes of the mobile phenyl groups, their rotational rates, and transition temperatures paves the way to controlling and understanding the role of molecular rotors through design of organic linkers within porous MOF materials. |
| Databáze: | OpenAIRE |
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