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Selective host-guest interactions in metal-organic frameworks via multiple hydrogen bond donor-acceptor recognition sites

Title data

Wittmann, T. ; Tschense, C. B. L. ; Zappe, L. ; Koschnick, C. ; Siegel, Renée ; Stäglich, Robert ; Lotsch, B. V. ; Senker, Jürgen:
Selective host-guest interactions in metal-organic frameworks via multiple hydrogen bond donor-acceptor recognition sites.
In: Journal of Materials Chemistry A. Vol. 7 (May 2019) Issue 17 . - pp. 10379-10388.
ISSN 2050-7496
DOI: https://doi.org/10.1039/c8ta12190g

Abstract in another language

Targeted recognition of medium sized molecules with mixed hydrogen bond units is essential for using porous materials for molecular separation, sensing and drug delivery. One promising way to achieve selectivity, is to make use of the key-and-lock principle guiding the design of hydrogen bond receptors matching the chemical signature of the target molecules. Among the class of porous materials metal-organic frameworks are particularly well suited for this purpose, as they allow for functionalizing the inner surfaces with various pending groups. Here we report the successful incorporation of 2-pyridyl urea (URPy) side groups with hydrogen bond donor-donor-acceptor (DDA) patterns into the framework MIL-101 with pores in the mesoporous range. Their influence on the sorption properties was investigated by competitive adsorption of 2-aminopyridine (2-AP) and 3-aminopyridine (3-AP) on MIL-101-URPy (Al, Cr) derivatives and comparison to the behaviour of a single donor function within MIL-101-NH2 (Al, Cr) derivatives. Grafting the coordinatively unsaturated sites at the inorganic building units (IBUs) with diethylamine, additionally allowed the adsorption at these sites to be suppressed and thus to focus on the hydrogen bond receptors. Compared to the single D sites the selectivity of 2-AP over 3-AP is enhanced by a factor of five for the DDA pending groups. Based on N-15 NMR spectroscopy and DFT calculations this observation is explained by forming double hydrogen bonds between the pyridyl urea groups and the 2-AP molecules, while 3-AP exhibits a single hydrogen bond only. At the D site of MIL-101-NH2 both 2-AP and 3-AP form single hydrogen bonds only.

Further data

Item Type: Article in a journal
Refereed: Yes
Additional notes: ISI:000472183200023
Institutions of the University: Faculties > Faculty of Biology, Chemistry and Earth Sciences
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Chair Anorganic Chemistry III
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Chair Anorganic Chemistry III > Chair Anorganic Chemistry III - Univ.-Prof. Dr. Jürgen Senker
Faculties
Result of work at the UBT: Yes
DDC Subjects: 500 Science
500 Science > 540 Chemistry
Date Deposited: 25 Sep 2019 09:20
Last Modified: 26 Sep 2019 06:28
URI: https://eref.uni-bayreuth.de/id/eprint/52430