NMR Signatures of the Active Sites in Sn-β Zeolite†
Patrick Wolf
Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
Department of Chemistry & Department of Chemical and Biological Engineering, University of Wisconsin - Madison, 1101 University Avenue, Madison, WI 53706 (USA)
These authors contributed equally to this work.
Search for more papers by this authorMaxence Valla
Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
These authors contributed equally to this work.
Search for more papers by this authorDr. Aaron J. Rossini
Centre de RMN à Très Hauts Champs, Institut de Sciences Analytiques, Université de Lyon (CNRS/ENS Lyon/UCB Lyon 1), 69100 Villeurbanne (France)
These authors contributed equally to this work.
Search for more papers by this authorDr. Aleix Comas-Vives
Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
These authors contributed equally to this work.
Search for more papers by this authorDr. Francisco Núñez-Zarur
Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
These authors contributed equally to this work.
Search for more papers by this authorProf. Dr. Bernard Malaman
Institut Jean Lamour-CNRS-UMR 7198, Université de Lorraine, Faculté des Sciences, BP 70239, 54506 Vandoeuvre-les-Nancy (France)
Search for more papers by this authorDr. Anne Lesage
Centre de RMN à Très Hauts Champs, Institut de Sciences Analytiques, Université de Lyon (CNRS/ENS Lyon/UCB Lyon 1), 69100 Villeurbanne (France)
Search for more papers by this authorProf. Dr. Lyndon Emsley
Centre de RMN à Très Hauts Champs, Institut de Sciences Analytiques, Université de Lyon (CNRS/ENS Lyon/UCB Lyon 1), 69100 Villeurbanne (France)
Search for more papers by this authorCorresponding Author
Prof. Dr. Christophe Copéret
Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
Christophe Copéret, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
Ive Hermans, Department of Chemistry & Department of Chemical and Biological Engineering, University of Wisconsin - Madison, 1101 University Avenue, Madison, WI 53706 (USA)
Search for more papers by this authorCorresponding Author
Prof. Dr. Ive Hermans
Department of Chemistry & Department of Chemical and Biological Engineering, University of Wisconsin - Madison, 1101 University Avenue, Madison, WI 53706 (USA)
Christophe Copéret, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
Ive Hermans, Department of Chemistry & Department of Chemical and Biological Engineering, University of Wisconsin - Madison, 1101 University Avenue, Madison, WI 53706 (USA)
Search for more papers by this authorPatrick Wolf
Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
Department of Chemistry & Department of Chemical and Biological Engineering, University of Wisconsin - Madison, 1101 University Avenue, Madison, WI 53706 (USA)
These authors contributed equally to this work.
Search for more papers by this authorMaxence Valla
Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
These authors contributed equally to this work.
Search for more papers by this authorDr. Aaron J. Rossini
Centre de RMN à Très Hauts Champs, Institut de Sciences Analytiques, Université de Lyon (CNRS/ENS Lyon/UCB Lyon 1), 69100 Villeurbanne (France)
These authors contributed equally to this work.
Search for more papers by this authorDr. Aleix Comas-Vives
Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
These authors contributed equally to this work.
Search for more papers by this authorDr. Francisco Núñez-Zarur
Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
These authors contributed equally to this work.
Search for more papers by this authorProf. Dr. Bernard Malaman
Institut Jean Lamour-CNRS-UMR 7198, Université de Lorraine, Faculté des Sciences, BP 70239, 54506 Vandoeuvre-les-Nancy (France)
Search for more papers by this authorDr. Anne Lesage
Centre de RMN à Très Hauts Champs, Institut de Sciences Analytiques, Université de Lyon (CNRS/ENS Lyon/UCB Lyon 1), 69100 Villeurbanne (France)
Search for more papers by this authorProf. Dr. Lyndon Emsley
Centre de RMN à Très Hauts Champs, Institut de Sciences Analytiques, Université de Lyon (CNRS/ENS Lyon/UCB Lyon 1), 69100 Villeurbanne (France)
Search for more papers by this authorCorresponding Author
Prof. Dr. Christophe Copéret
Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
Christophe Copéret, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
Ive Hermans, Department of Chemistry & Department of Chemical and Biological Engineering, University of Wisconsin - Madison, 1101 University Avenue, Madison, WI 53706 (USA)
Search for more papers by this authorCorresponding Author
Prof. Dr. Ive Hermans
Department of Chemistry & Department of Chemical and Biological Engineering, University of Wisconsin - Madison, 1101 University Avenue, Madison, WI 53706 (USA)
Christophe Copéret, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir Prelog Weg 2, 8093 Zurich (Switzerland)
Ive Hermans, Department of Chemistry & Department of Chemical and Biological Engineering, University of Wisconsin - Madison, 1101 University Avenue, Madison, WI 53706 (USA)
Search for more papers by this authorWe acknowledge SNF Grants No. 200021_143600 and 200021_146661, Ambizione project PZ00P2_148059, EQUIPEX contract ANR-10-EQPX-47-01, and ERC Advanced Grant No. 320860 for funding.
Abstract
Dynamic nuclear polarization surface enhanced NMR (DNP-SENS), Mössbauer spectroscopy, and computational chemistry were combined to obtain structural information on the active-site speciation in Sn-β zeolite. This approach unambiguously shows the presence of framework SnIV-active sites in an octahedral environment, which probably correspond to so-called open and closed sites, respectively (namely, tin bound to three or four siloxy groups of the zeolite framework).
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References
- 1
- 1aF. Cavani, J. H. Teles, ChemSusChem 2009, 2, 508–534;
- 1bB. Notari, Adv. Catal. 1996, 41, 253–334;
- 1cS. Bordiga, A. Damin, F. Bonino, C. Lamberti, Surface and Interfacial Organometallic Chemistry and Catalysis, Vol. 16 (Eds.: ), Springer, Berlin, 2005, pp. 37–68.
10.1007/b138073 Google Scholar
- 2
- 2aY. Román-Leshkov, M. Davis, ACS Catal. 2011, 1, 1566–1580;
- 2bR. Lobo, AIChE J. 2008, 54, 1402–1409;
- 2cM. Dusselier, P. Van Wouwe, A. Dewaele, E. Makshina, B. F. Sels, Energy Environ. Sci. 2013, 6, 1415–1442.
- 3
- 3aM. S. Holm, S. Saravanamurugan, E. Taarning, Science 2010, 328, 602–603;
- 3bY. Román-Leshkov, M. Moliner, J. A. Labinger, M. E. Davis, Angew. Chem. 2010, 122, 9138–9141;
10.1002/ange.201004689 Google ScholarAngew. Chem. Int. Ed. 2010, 49, 8954–8957;
- 3cM. Moliner, Y. Román-Leshkov, M. E. Davis, Proc. Natl. Acad. Sci. USA 2010, 107, 6164–6168;
- 3dW. R. Gunther, Y. Wang, Y. Ji, V. K. Michaelis, S. T. Hunt, R. G. Griffin, Y. Román-Leshkov, Nat. Commun. 2012, 3, 1109–1116.
- 4
- 4aA. Corma, L. Nemeth, M. Renz, S. Valencia, Nature 2001, 412, 423–425;
- 4bA. Corma, V. Fornés, S. Iborra, M. Mifsud, M. Renz, J. Catal. 2004, 221, 67–76;
- 4cM. Renz, T. Blasco, A. Corma, V. Fornés, R. Jensen, L. Nemeth, Chem. Eur. J. 2002, 8, 4708–4717.
10.1002/1521-3765(20021018)8:20<4708::AID-CHEM4708>3.0.CO;2-U CAS PubMed Web of Science® Google Scholar
- 5A. Corma, M. Renz, Chem. Commun. 2004, 550–551.
- 6
- 6aA. Corma, M. E. Domine, L. Nemeth, S. Valencia, J. Am. Chem. Soc. 2002, 124, 3194–3195;
- 6bM. Boronat, A. Corma, M. Renz, J. Phys. Chem. B 2006, 110, 21168–21174;
- 6cA. Corma, M. E. Domine, S. Valencia, J. Catal. 2003, 215, 294–304.
- 7
- 7aC. Hammond, S. Conrad, I. Hermans, Angew. Chem. 2012, 124, 11906–11909; Angew. Chem. Int. Ed. 2012, 51, 11736–11739;
- 7bP. Wolf, C. Hammond, S. Conrad, I. Hermans, Dalton Trans. 2014, 43, 4514–4519;
- 7cJ. Dijkmans, D. Gabriëls, M. Dusselier, F. de Clippel, P. Vanelderen, K. Houthoofd, A. Malfliet, Y. Pontikes, B. F. Sels, Green Chem. 2013, 15, 2777–2785;
- 7dP. Li, G. Liu, H. Wu, Y. Liu, J. Jiang, P. Wu, J. Phys. Chem. C 2011, 115, 3663–3670.
- 8
- 8aM. Boronat, P. Concepción, A. Corma, M. Renz, S. Valencia, J. Catal. 2005, 234, 111–118;
- 8bM. Boronat, P. Concepción, A. Corma, M. Renz, Catal. Today 2007, 121, 39–44.
- 9S. R. Bare, S. D. Kelly, W. Sinkler, J. J. Low, F. S. Modica, S. Valencia, A. Corma, L. T. Nemeth, J. Am. Chem. Soc. 2005, 127, 12924–12932.
- 10
- 10aG. Yang, E. Pidko, E. J. M. Hensen, J. Phys. Chem. C 2013, 117, 3976–3986;
- 10bG. Yang, E. A. Pidko, E. J. M. Hensen, ChemSusChem 2013, 6, 1688–1696.
- 11R. Bermejo-Deval, R. S. Assary, E. Nikolla, M. Moliner, Y. Román-Leshkov, S.-J. Hwang, A. Palsdottir, D. Silverman, R. F. Lobo, L. A. Curtiss, M. E. Davis, Proc. Natl. Acad. Sci. USA 2012, 109, 9727–9732.
- 12R. Bermejo-Deval, R. Gounder, M. E. Davis, ACS Catal. 2012, 2, 2705–2713.
- 13Tetrahedral SnIV is expected with significant negative value (IS=−0.2 mm s−1), corroborating the hexacoordination of Sn in the sample; R. V. Parish in Mossbauer Spectroscopy Applied to Inorganic Chemistry, Vol. 1 (Ed.: ) Plenum, New York, 1984, p. 527.
10.1007/978-1-4899-0462-1_16 Google Scholar
- 14S. Roy, K. Bakhmutsky, E. Mahmoud, R. F. Lobo, R. J. Gorte, ACS Catal. 2013, 3, 573–580.
- 15T. Maly, G. T. Debelouchina, V. S. Bajaj, K. N. Hu, C. G. Joo, M. L. Mak-Jurkauskas, J. R. Sirigiri, P. C. A. van der Wel, J. Herzfeld, R. J. Temkin, R. G. Griffin, J. Chem. Phys. 2008, 128, 052211.
- 16
- 16aA. Zagdoun, A. J. Rossini, D. Gajan, A. Bourdolle, O. Ouari, M. Rosay, W. E. Maas, P. Tordo, M. Lelli, L. Emsley, A. Lesage, C. Copéret, Chem. Commun. 2012, 48, 654–656;
- 16bA. Zagdoun, G. Casano, O. Ouari, G. Lapadula, A. Rossini, M. Lelli, M. Baffert, D. Gajan, L. Veyre, W. Maas, M. Rosay, R. Weber, C. Thieuleux, C. Coperet, A. Lesage, P. Tordo, L. Emsley, J. Am. Chem. Soc. 2012, 134, 2284–2291;
- 16cD. Gajan, M. Schwarzwälder, M. P. Conley, W. R. Gruening, A. J. Rossini, A. Zagdoun, M. Lelli, M. Yulikov, G. Jeschke, C. Sauvée, O. Ouari, P. Tordo, L. Veyre, A. Lesage, C. Thieuleux, L. Emsley, C. Copéret, J. Am. Chem. Soc. 2013, 135, 15459–15466.
- 17
- 17aA. Lesage, M. Lelli, D. Gajan, M. A. Caporini, V. Vitzthum, P. Miéville, J. Alauzun, A. Roussey, C. Thieuleux, A. Mehdi, G. Bodenhausen, C. Copéret, L. Emsley, J. Am. Chem. Soc. 2010, 132, 15459–15461;
- 17bM. Lelli, D. Gajan, A. Lesage, M. A. Caporini, V. Vitzthum, P. Miéville, F. Héroguel, F. Rascon, A. Roussey, C. Thieuleux, M. Boualleg, L. Veyre, G. Bodenhausen, C. Copéret, L. Emsley, J. Am. Chem. Soc. 2011, 133, 2104–2107;
- 17cA. Rossini, A. Zagdoun, M. Lelli, A. Lesage, C. Copéret, L. Emsley, Acc. Chem. Res. 2013, 46, 1942–1951.
- 18L. Protesescu, A. J. Rossini, D. Kriegner, M. Valla, A. de Kergommeaux, M. Walter, K. V. Kravchyk, M. Nachtegaal, J. Stangl, B. Malaman, P. Reiss, A. Lesage, L. Emsley, C. C. Copéret, M. V. Kovalenko, ACS Nano 2014, 8, 2639–2648.
- 19After submission of this manuscript the following paper appeared on the use of DNP enhanced 119Sn NMR for hydrothermally synthesized Snβ: W. R. Gunther, V. K. Michaelis, M. A. Caporini, R. G. Griffin, Y. Román-Leshkov, J. Am. Chem. Soc. 2014, 136, 6219–6222.
- 20A. Zagdoun, G. Casano, O. Ouari, M. Schwarzwälder, A. J. Rossini, F. Aussenac, M. Yulikov, G. Jeschke, C. Copéret, A. Lesage, P. Tordo, L. Emsley, J. Am. Chem. Soc. 2013, 135, 12790–12797.
- 21
- 21aP. C. A. van der Wel, K. N. Hu, J. Lewandowski, R. G. Griffin, J. Am. Chem. Soc. 2006, 128, 10840–10846;
- 21bA. J. Rossini, A. Zagdoun, F. S. Hegner, M. Schwarzwälder, D. Gajan, C. Copéret, A. Lesage, L. Emsley, J. Am. Chem. Soc. 2012, 134, 16899–16908;
- 21cO. Lafon, A. S. L. Thankamony, T. Kobayashi, D. Carnevale, V. Vitzthum, I. Slowing, K. Kandel, H. Vezin, J. P. Amoureux, G. Bodenhausen, M. Pruski, J. Phys. Chem. C 2013, 117, 1375–1382;
- 21dA. J. Rossini, A. Zagdoun, M. Lelli, J. Canivet, S. Aguado, O. Ouari, M. Rosay, W. E. Maas, C. Copéret, D. Farrusseng, L. Emsley, A. Lesage, Angew. Chem. 2012, 124, 127–131;
10.1002/ange.201106030 Google ScholarAngew. Chem. Int. Ed. 2012, 51, 123–127.
- 22A. J. Rossini, A. Zagdoun, M. Lelli, D. Gajan, F. Rascón, M. Rosay, W. E. Maas, C. Copéret, A. Lesage, L. Emsley, Chem. Sci. 2012, 3, 108–115.
- 23J. Z. Hu, W. Wang, F. Liu, M. S. Solum, D. W. Alderman, R. J. Pugmire, D. M. Grant, J. Magn. Reson. Ser. A 1995, 113, 210–222.
- 24J. Herzfeld, A. E. Berger, J. Chem. Phys. 1980, 73, 6021.
- 25G. Le Caër, personal communication.
- 26M. Rosay, L. Tometich, S. Pawsey, R. Bader, R. Schauwecker, M. Blank, P. M. Borchard, S. R. Cauffman, K. L. Felch, R. T. Weber, R. J. Temkin, R. G. Griffin, W. E. Maas, Phys. Chem. Chem. Phys. 2010, 12, 5850–5860.
- 27B. M. Fung, A. K. Khitrin, K. J. Ermolaev, J. Magn. Reson. 2000, 142, 97–101.
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