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  Flexibility versus rigidity: what determines the stability of zeolite frameworks? A case study

Verheyen, E., Joos, L., Martineau, C., Dawson, C. J., Weidenthaler, C., Schmidt, W., et al. (2014). Flexibility versus rigidity: what determines the stability of zeolite frameworks? A case study. Materials Horizons, 1(6), 582-587. doi:10.1039/C4MH00127C.

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Verheyen, E.1, Autor
Joos, L.2, Autor
Martineau, C.3, Autor
Dawson, C. J.4, Autor
Weidenthaler, C.5, Autor           
Schmidt, W.6, Autor           
Yuan, R.1, Autor
Breynaert , E.1, Autor
van Speybroeck , V.2, Autor
Waroquier, M.2, Autor
Taulelle, F.1, 3, Autor
Treacy, M. M. J.4, Autor
Martens, J. A.1, Autor
Kirschhock, C. E. A.1, Autor
Affiliations:
1Centre for Surface Chemistry and Catalysis, KU Leuven, Kasteelpark Arenberg 23–box 2461, B-3001 Leuven, Belgium, ou_persistent22              
2Center for Molecular Modeling, Ghent University, B-9052 Zwijnaarde, Belgium , ou_persistent22              
3Tectospin, Institut Lavoisier de Versailles, UMR CNRS 8180 Université de Versailles St Quentin en Yvelines, 45 Avenue des Etats Unis, Versailles Cedex, France , ou_persistent22              
4Department of Physics, Arizona State University, P.O. Box 871504, Tempe, USA, ou_persistent22              
5Research Group Weidenthaler, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1950291              
6Research Group Schmidt, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445618              

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 Zusammenfassung: All silica COK-14/-COK-14 with OKO topology is the first case of a zeolite which reversibly transforms from a systematically interrupted to a fully connected state and back. Analysis of the opening/closing behavior allowed the study of entropy and framework flexibility as determinants for the stability of zeolite topologies, which, until now, has been experimentally inaccessible. Interconversion of the all-silica COK-14 zeolite with fully connected OKO topology and its -COK-14 variant with systematic framework interruption was investigated using high-temperature XRD, thermogravimetric analysis, 29 Si MAS NMR, nitrogen adsorption and a range of modelling techniques. Specific framework bonds in the OKO framework can be reversibly hydrolyzed and condensed. Structural silanols of the parent -COK-14, prepared by degermanation of the IM-12 zeolite, were condensed by heating at 923 K, and hydrolyzed again to the initial state by contacting the zeolite with warm water. Molecular modelling revealed an inversion of the relative stabilities for both variants depending on temperature and hydration. Condensation of the structural silanols in -COK-14 to COK-14 is entropy driven, mainly resulting from the release of water molecules. Framework reopening in the presence of water is spontaneous due to the high rigidity of the fully connected OKO framework. Isomorphous substitution was demonstrated as a viable option for stabilization of the fully connected OKO framework as this renders the closed framework flexible.

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Sprache(n): eng - English
 Datum: 2014-07-232014-08-192014-11-01
 Publikationsstatus: Erschienen
 Seiten: 6
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1039/C4MH00127C
 Art des Abschluß: -

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Titel: Materials Horizons
  Kurztitel : Mater. Horiz.
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: Cambridge : Royal Society of Chemistry
Seiten: - Band / Heft: 1 (6) Artikelnummer: - Start- / Endseite: 582 - 587 Identifikator: ISSN: 2051-6347
CoNE: https://pure.mpg.de/cone/journals/resource/2051-6347