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Enhancing the Water Stability of Al-MIL-101-NH2 via Postsynthetic Modification

Titelangaben

Wittmann, Thomas ; Siegel, Renée ; Reimer, Nele ; Milius, Wolfgang ; Stock, Norbert ; Senker, Jürgen:
Enhancing the Water Stability of Al-MIL-101-NH2 via Postsynthetic Modification.
In: Chemistry : a European Journal. Bd. 21 (2015) Heft 1 . - S. 314-323.
ISSN 1521-3765
DOI: https://doi.org/10.1002/chem.201404654

Volltext

Link zum Volltext (externe URL): Volltext

Abstract

The resistance of metal-organic frameworks towards water is a very critical issue concerning their practical use. Recently, it was shown for microporous MOFs that the water stability could be increased by introducing hydrophobic pendant groups. Here, we demonstrate a remarkable stabilisation of the mesoporous MOF Al-MIL-101-NH2 by post-synthetic modification with phenyl isocyanate. In this process 86% of the amino groups were converted into phenylurea units. As a consequence, the long-term stability of AlMIL-101-URPh in liquid water could be extended beyond a week. In water saturated atmospheres Al-MIL-101-URPh decomposed at least 12-times slower than the unfunctionalised analogue. To study the underlying processes both materials were characterised by Ar, N-2 and H2O sorption measurements, powder X-ray diffraction, thermogravimetric and chemical analysis as well as solid-state NMR and IR spectroscopy. Postsynthetic modification decreased the BET equivalent surface area from 3363 to 1555 m(2)g(-1) for Al-MIL-101URPh and reduced the mean diameters of the mesopores by 0.6 nm without degrading the structure significantly and reducing thermal stability. In spite of similar water uptake capacities, the relative humidity-dependent uptake of Al-MIL101-URPh is slowed and occurs at higher relative humidity values. In combination with H-1-Al-27 D-HMQC NMR spectroscopy experiments this favours a shielding mechanism of the Al clusters by the pendant phenyl groups and rules out pore blocking.

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Publikationsform: Artikel in einer Zeitschrift
Begutachteter Beitrag: Ja
Zusätzliche Informationen: ISI:000346735000033
Keywords: Hybrid materials; Metal-organic frameworks; Porosity; Postsynthetic modification; Water stability
Institutionen der Universität: Fakultäten > Fakultät für Biologie, Chemie und Geowissenschaften
Fakultäten > Fakultät für Biologie, Chemie und Geowissenschaften > Fachgruppe Chemie
Fakultäten > Fakultät für Biologie, Chemie und Geowissenschaften > Fachgruppe Chemie > Lehrstuhl Anorganische Chemie III
Fakultäten > Fakultät für Biologie, Chemie und Geowissenschaften > Fachgruppe Chemie > Lehrstuhl Anorganische Chemie III > Lehrstuhl Anorganische Chemie III - Univ.-Prof. Dr. Jürgen Senker
Fakultäten
Titel an der UBT entstanden: Ja
Themengebiete aus DDC: 500 Naturwissenschaften und Mathematik
500 Naturwissenschaften und Mathematik > 540 Chemie
Eingestellt am: 18 Mär 2021 08:18
Letzte Änderung: 07 Feb 2023 10:05
URI: https://eref.uni-bayreuth.de/id/eprint/64075