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Effect of partial linker fluorination and linker extension on structure and properties of the Al-MOF CAU-10
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Number of Authors: 4
2017 (English)In: Microporous and Mesoporous Materials, ISSN 1387-1811, E-ISSN 1873-3093, Vol. 249, 128-136 p.Article in journal (Refereed) Published
Abstract [en]

The systematic investigation of the solvothermal system Al3+/5-fluoroisophthalic acid (H(2)mBDC-5F)/isophthalic acid (H(2)mBDC)/DMF/H2O through a mixed-linker approach led to new mixed-linker CAU-10 derivatives containing 11, 28 and 44% of fluorinated linker molecules (denoted as CAU-10-H/F-11, CAU-10-H/F-28 and CAU-10-H/F-44, respectively), as determined by NMR spectroscopy. The crystal structure of CAU-10-H/F-28 was determined using the Rietveld method (space group 14(1)md, a = b = 21.3075(5), c = 10.7101(3) angstrom). The structure is built up by helical chains composed of cis corner-sharing AlO6 polyhedra. Each of these helices is interconnected to four adjacent helices with alternating rotational orientation through the carboxylate groups of mBDC(2-) linker molecules. Thus, accessible, square-shaped channels are formed. Sorption measurements revealed a high dependency of the adsorbed amount of gas on the degree of fluorination. With increasing fluorination, the total uptake decreases in N-2, H-2 and H2O sorption experiments and the hydrophobic character of the pores increases. In addition, an extended CAU-10 derivative, CAU-10-HTATB, was discovered using the tricarboxylic acid 4,4',4-s-triazine-2,4,6-triyl-tribenzoic acid (H(3)TATB) during the high-throughput investigation of the system Al3+/H(3)TATB/DMF/H2O. This new MOF, which was denoted CAU-10-HTATB, was thoroughly characterized using IR spectroscopy, thermogravimetric and elemental analysis, temperature dependent powder X-ray diffraction (PXRD) and sorption measurements. Although the compound is thermally stable up to 400 degrees C according to temperature-dependent PXRD measurements, it is not porous towards N2 molecules. The structure of CAU-10-HTATB could be also refined from PXRD data using the Rietveld method (space group l4(1)/a, a = b = 36.438 (1), c = 10.9373 (9) angstrom).

Place, publisher, year, edition, pages
2017. Vol. 249, 128-136 p.
Keyword [en]
Metal-organic frameworks, Aluminium, Powder X-ray diffraction, CAU-10, Water sorption
National Category
Chemical Sciences Nano Technology Materials Engineering
Identifiers
URN: urn:nbn:se:su:diva-145962DOI: 10.1016/j.micromeso.2017.04.054ISI: 000404315500016OAI: oai:DiVA.org:su-145962DiVA: diva2:1141798
Available from: 2017-09-15 Created: 2017-09-15 Last updated: 2017-09-15Bibliographically approved

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