Interlinker Hydrogen Bonds Govern CO2 Adsorption
in a Series of Flexible 2D Diacylhydrazone/Isophthalate-Based MOFs:
Influence of Metal Center, Linker Substituent, and Activation Temperature
Posted on 2020-07-14 - 22:04
Four new layered flexible metal–organic
frameworks (MOFs)
containing a diacylhydrazone moiety, namely, guest-filled [Zn2(iso)2(tdih)2]n (1), [Zn2(NH2iso)2(tdih)2]n (2),
[Cd2(iso)2(tdih)2]n (3) and [Cd2(NH2iso)2(tdih)2]n (4) were synthesized using terephthalaldehyde di-isonicotinoylhydrazone
(tdih) as a linear ditopic linker as well as isophtalate
(iso) or 5-aminoisophthalate (NH2iso) as angular colinkers.
The MOFs with hexacoordinated cadmium centers feature two-dimensional
pore systems as compared to the MOFs with pentacoordinated zinc centers
showing either zero-dimensional or mixed zero-/one-dimensional voids,
as evidenced by single-crystal X-ray diffraction. In contrast to the
frameworks based on isophtalates which do not show any significant
gas uptakes, introduction of amino-substituted linker enables CO2 adsorption. Gently activated aminoisophthalate-based frameworks,
that is, guest-exchanged in methanol and heated to 100 °C, show
reversible gated CO2 adsorptions at 195 K, whereas the
increase of activation temperature to 150 °C or more leads to
one-step isotherms and lower adsorption capacities. X-ray diffraction
and IR spectroscopy reveal significant structural differences in interlayer
hydrogen bonding upon activation of materials at higher temperatures.
The work emphasizes the role of hydrogen bonds in crystal engineering
of layered materials and the importance of activation conditions in
such systems.
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Roztocki, Kornel; Szufla, Monika; Bon, Volodymyr; Senkovska, Irena; Kaskel, Stefan; Matoga, Dariusz (2020). Interlinker Hydrogen Bonds Govern CO2 Adsorption
in a Series of Flexible 2D Diacylhydrazone/Isophthalate-Based MOFs:
Influence of Metal Center, Linker Substituent, and Activation Temperature. ACS Publications. Collection. https://doi.org/10.1021/acs.inorgchem.0c01182