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Discovery and In Si...
Discovery and In Situ Crystallization Studies of Cerium-Based Metal–Organic Frameworks with V-Shaped Linker Molecules
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Gosch, Jonas (författare)
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Guiotto, Virginia (författare)
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Steinke, Felix (författare)
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- Svensson Grape, Erik, 1991- (författare)
- Stockholms universitet,Institutionen för material- och miljökemi (MMK)
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Atzori, Cesare (författare)
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Mertin, Kalle (författare)
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Otto, Tobias (författare)
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Ruser, Niklas (författare)
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Meier, Christoph (författare)
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Morelli Venturi, Diletta (författare)
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- Inge, A. Ken, 1984- (författare)
- Stockholms universitet,Institutionen för material- och miljökemi (MMK)
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Lomachenko, Kirill A. (författare)
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Crocellà, Valentina (författare)
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Stock, Norbert (författare)
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(creator_code:org_t)
- 2023
- 2023
- Engelska.
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Ingår i: Inorganic Chemistry. - 0020-1669 .- 1520-510X. ; 62:51, s. 20929-20939
- Relaterad länk:
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https://urn.kb.se/re...
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https://doi.org/10.1...
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Abstract
Ämnesord
Stäng
- We report the discovery and characterization of two porous Ce(III)-based metal–organic frameworks (MOFs) with the V-shaped linker molecules 4,4′-sulfonyldibenzoate (SDB2–) and 4,4′-(hexafluoroisopropylidene)bis(benzoate) (hfipbb2–). The compounds of framework composition [Ce2(H2O)(SDB)3] (1) and [Ce2(hfipbb)3] (2) were obtained by using a synthetic approach in acetonitrile that we recently established. Structure determination of 1 was accomplished from 3D electron diffraction (3D ED) data, while 2 could be refined against powder X-ray diffraction (PXRD) data using the crystal structure of an isostructural La-MOF as the starting model. Their framework structures consist of chain-like inorganic building units (IBUs) or hybrid-BUs that are interconnected by the V-shaped linker molecules to form framework structures with channel-type pores. The composition of both compounds was confirmed by PXRD, elemental analysis, as well as NMR and IR spectroscopy. Interestingly, despite the use of (NH4)2[CeIV(NO3)6] in the synthesis, cerium ions in both MOFs occur exclusively in the + III oxidation state as determined by X-ray absorption near edge structure (XANES) and X-ray photoelectron spectroscopy (XPS). Thermal analyses reveal remarkably high thermal stabilities of ≥400 °C for the MOFs. Initial N2 sorption measurements revealed the peculiar sorption behavior of 2 which prompted a deeper investigation by Ar and CO2 sorption experiments. The combination with nonlocal density functional theory (NL-DFT) calculations adds to the understanding of the nature of the different pore diameters in 2. An extensive quasi-simultaneous in situ XANES/XRD investigation was carried out to unveil the formation of Ce-MOFs during the solvothermal syntheses in acetonitrile. The crystallization of the two Ce(III)-MOFs presented herein as well as two previously reported Ce(IV)-MOFs, all obtained by a similar synthetic approach, were studied. While the XRD patterns show time-dependent MOF crystallization, the XANES data reveal the presence of Ce(III) intermediates and their subsequent conversion to the MOFs. The addition of acetic acid in combination with the V-shaped linker molecule was identified as the crucial factor for the formation of the crystalline Ce(III/IV)-MOFs.
Ämnesord
- NATURVETENSKAP -- Kemi -- Oorganisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Inorganic Chemistry (hsv//eng)
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Gosch, Jonas
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Guiotto, Virgini ...
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Steinke, Felix
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Svensson Grape, ...
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Atzori, Cesare
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Mertin, Kalle
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visa fler...
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Otto, Tobias
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Ruser, Niklas
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Meier, Christoph
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Morelli Venturi, ...
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Inge, A. Ken, 19 ...
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Lomachenko, Kiri ...
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Crocellà, Valent ...
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Stock, Norbert
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visa färre...
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Inorganic Chemis ...
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Stockholms universitet