NDLI: Elucidating Gating Effects for Hydrogen Sorption in MFU-4-Type Triazolate-Based Metal–Organic Frameworks Featuring Different Pore Sizes

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Elucidating Gating Effects for Hydrogen Sorption in MFU-4-Type Triazolate-Based Metal–Organic Frameworks Featuring Different Pore Sizes

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Hanss, Jan Denysenko, Dmytro Grzywa, Maciej Streppel, Barbara Tonigold, Markus Volkmer, Dirk Mugnaioli, Enrico Krkljus, Ivana Kolb, Ute Hirscher, Michael
Description	Author Affiliation: Denysenko D ( Institute of Physics, Chair of Solid State and Material Science, Augsburg University, Universitätsstrasse 1, 86135 Augsburg, Germany.)
Abstract	A highly porous member of isoreticular MFU-4-type frameworks, $[Zn_{5}Cl_{4}(BTDD)_{3}]$ (MFU-4l(arge)) $(H_{2}-BTDD=bis(1H-1,2,3-triazolo[4,5-b],[4′,5′-i])dibenzo[1,4]dioxin),$ has been synthesized using $ZnCl_{2}$ and $H_{2}-BTDD$ in N,N-dimethylformamide as a solvent. MFU-4l represents the first example of MFU-4-type frameworks featuring large pore apertures of 9.1 Å. Here, MFU-4l serves as a reference compound to evaluate the origin of unique and specific gas-sorption properties of MFU-4, reported previously. The latter framework features narrow-sized pores of 2.5 Å that allow passage of sufficiently small molecules only (such as hydrogen or water), whereas molecules with larger kinetic diameters (e.g., argon or nitrogen) are excluded from uptake. The crystal structure of MFU-4l has been solved ab initio by direct methods from 3D electron-diffraction data acquired from a single nanosized crystal through automated electron diffraction tomography (ADT) in combination with electron-beam precession. Independently, it has been solved using powder X-ray diffraction. Thermogravimetric analysis (TGA) and variable-temperature X-ray powder diffraction (XRPD) experiments carried out on MFU-4l indicate that it is stable up to 500 °C $(N_{2}$ atmosphere) and up to 350 °C in air. The framework adsorbs 4 wt % hydrogen at 20 bar and 77 K, which is twice the amount compared to MFU-4. The isosteric heat of adsorption starts for low surface coverage at $5 kJ mol^{−1}$ and decreases to $3.5 kJ mol^{−1}$ at higher $H_{2}$ uptake. In contrast, MFU-4 possesses a nearly constant isosteric heat of adsorption of ca. $7 kJ mol^{−1}$ over a wide range of surface coverage. Moreover, MFU-4 exhibits a $H_{2}$ desorption maximum at 71 K, which is the highest temperature ever measured for hydrogen physisorbed on metal–organic frameworks (MOFs).
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	6
Volume Number	17
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2011-02-07
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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