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Aluminum Siting in Silicon‐Rich Zeolite Frameworks: A Combined High‐Resolution 27 Al NMR Spectroscopy and Quantum Mechanics / Molecular Mechanics Study of ZSM‐5

2007; Wiley; Volume: 46; Issue: 38 Linguagem: Inglês

10.1002/anie.200702628

1521-3773

Štěpán Sklenák, Jiřı́ Dědeček, Chengbin Li, Blanka Wichterlová, Vendula Gábová, Marek Sierka, Joachim Sauer,

Muon and positron interactions and applications

Angewandte Chemie International EditionVolume 46, Issue 38 p. 7286-7289 Communication Aluminum Siting in Silicon-Rich Zeolite Frameworks: A Combined High-Resolution 27Al NMR Spectroscopy and Quantum Mechanics / Molecular Mechanics Study of ZSM-5† Stepan Sklenak Dr., Stepan Sklenak Dr. [email protected] J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Dolejškova 3, 182 23 Prague, Czech Republic, Fax: (+420) 28658-2307Search for more papers by this authorJiří Dědeček Dr., Jiří Dědeček Dr. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Dolejškova 3, 182 23 Prague, Czech Republic, Fax: (+420) 28658-2307Search for more papers by this authorChengbin Li Dr., Chengbin Li Dr. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Dolejškova 3, 182 23 Prague, Czech Republic, Fax: (+420) 28658-2307Search for more papers by this authorBlanka Wichterlová Dr., Blanka Wichterlová Dr. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Dolejškova 3, 182 23 Prague, Czech Republic, Fax: (+420) 28658-2307Search for more papers by this authorVendula Gábová Dr., Vendula Gábová Dr. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Dolejškova 3, 182 23 Prague, Czech Republic, Fax: (+420) 28658-2307Search for more papers by this authorMarek Sierka Dr., Marek Sierka Dr. Humboldt-Universität zu Berlin, Institut für Chemie, Unter den Linden 6, 10099 Berlin, Germany, Fax: (+49) 30-2093-7136Search for more papers by this authorJoachim Sauer Prof., Joachim Sauer Prof. [email protected] Humboldt-Universität zu Berlin, Institut für Chemie, Unter den Linden 6, 10099 Berlin, Germany, Fax: (+49) 30-2093-7136Search for more papers by this author Stepan Sklenak Dr., Stepan Sklenak Dr. [email protected] J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Dolejškova 3, 182 23 Prague, Czech Republic, Fax: (+420) 28658-2307Search for more papers by this authorJiří Dědeček Dr., Jiří Dědeček Dr. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Dolejškova 3, 182 23 Prague, Czech Republic, Fax: (+420) 28658-2307Search for more papers by this authorChengbin Li Dr., Chengbin Li Dr. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Dolejškova 3, 182 23 Prague, Czech Republic, Fax: (+420) 28658-2307Search for more papers by this authorBlanka Wichterlová Dr., Blanka Wichterlová Dr. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Dolejškova 3, 182 23 Prague, Czech Republic, Fax: (+420) 28658-2307Search for more papers by this authorVendula Gábová Dr., Vendula Gábová Dr. J. Heyrovský Institute of Physical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Dolejškova 3, 182 23 Prague, Czech Republic, Fax: (+420) 28658-2307Search for more papers by this authorMarek Sierka Dr., Marek Sierka Dr. Humboldt-Universität zu Berlin, Institut für Chemie, Unter den Linden 6, 10099 Berlin, Germany, Fax: (+49) 30-2093-7136Search for more papers by this authorJoachim Sauer Prof., Joachim Sauer Prof. [email protected] Humboldt-Universität zu Berlin, Institut für Chemie, Unter den Linden 6, 10099 Berlin, Germany, Fax: (+49) 30-2093-7136Search for more papers by this author First published: 17 September 2007 https://doi.org/10.1002/anie.200702628Citations: 212 † Supported by the Academy of Sciences of the Czech Republic (project no. 1ET400400413), the Grant Agencies of the Czech Republic (project no. 203/06/1449), and of the Academy of Sciences of the Czech Republic (project no. IAA4040308), by the German Research Foundation (DFG) and the Funds of the German Chemical Industry (FCI). We thank Prof. Peter F. Rogl of the University of Vienna, Austria for helpful discussions on crystallography questions. Read the full textAboutPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShare Give accessShare full text accessShare full-text accessPlease review our Terms and Conditions of Use and check box below to share full-text version of article.I have read and accept the Wiley Online Library Terms and Conditions of UseShareable LinkUse the link below to share a full-text version of this article with your friends and colleagues. Learn more.Copy URL Share a linkShare onEmailFacebookTwitterLinkedInRedditWechat Graphical Abstract Finding Al: The distribution of catalytically active sites over crystallographic positions in zeolites is not random but controlled by synthesis. For differently synthesized ZSM-5 samples, distinct 27Al resonances have been identified by NMR spectroscopy. Shift calculations by DFT show that the observed resonances belong to Al in different crystallographic sites (see picture). Supporting Information Supporting information for this article is available on the WWW under http://www.wiley-vch.de/contents/jc_2002/2007/z702628_s.pdf or from the author. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article. References 1C. A. Fyfe, G. C. Gobbi, J. Klinowski, J. M. Thomas, S. Ramdas, Nature 1982, 296, 530–533. 2L. B. Alemany, Appl. Magn. Reson. 1993, 4, 179–201. 3P. Sarv, C. Fernandez, J. P. Amoureux, K. Keskinen, J. Phys. Chem. 1996, 100, 19223–19226. 4O. H. Han, C. S. Kim, S. B. Hong, Angew. Chem. 2002, 114, 487–490; . Chem. Int. 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B 1999, 103, 1462–1476. 26This is in agreement with the result of Sarv et al.[3] who reported a tiny difference (0–0.2 ppm) between the F1 values of the resonances for Na- and Ca-ZSM-5. 27V. Moravetski, J. R. Hill, U. Eichler, A. K. Cheetham, J. Sauer, J. Am. Chem. Soc. 1996, 118, 13015–13020. 28K. Wolinski, J. F. Hinton, P. Pulay, J. Am. Chem. Soc. 1990, 112, 8251–8260. 29M. J. Frisch, et al. Gaussian 03, Revision C.02, Gaussian, Inc., Wallingford CT, 2004. See the Supporting Information for a list of all authors. 30S. Sklenak, J. Dědeček, C. Li, B. Jansang, unpublished results. 31E. Lippmaa, A. Samoson, M. Magi, J. Am. Chem. Soc. 1986, 108, 1730–1735. 32Moreover, the correlation between chemical shift and bond angle seems to be of limited validity for high-silica zeolites, as the data in Table S3 and Figure S1 of the Supporting Information indicate; see also reference [13]. Citing Literature Volume46, Issue38September 24, 2007Pages 7286-7289 ReferencesRelatedInformation