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1887
Volume 60, Issue 2
  • ISSN: 2056-5135

Abstract

High-surface area γ-alumina is industrially used as a catalyst support. Catalytically active elements are doped onto the support, where they can bind to AlO, AlO or AlO sites on the surface. Pretreating the surface with alkaline earth oxides can alter the availability of these surface sites, hence affecting the catalytic activity. The surface binding sites of strontium oxide (SrO) on γ-alumina were previously unknown. Direct 27Al magic angle spinning nuclear magnetic resonance (MAS NMR) could not detect AlO sites at 9.4 T, so 1H–27Al cross-polarisation (CP) MAS NMR was used to preferentially select the surface environment signals. We directly observed the three surface environments on dehydrated γ-alumina as a function of SrO impregnation up to 4 wt% SrO. We found that Sr2+ preferentially binds to AlO and AlO surface sites. 1H MAS NMR revealed SrO impregnation causes a reduction in the terminal (−0.3 ppm) and bridging (2.2 ppm) hydroxyl environments, as well as the promotion of a new peak in between these sites, at 0.5 ppm. By using 1H–27Al CP/MAS NMR the relative proportions of surface sites on γ-alumina can be determined, allowing an optimal level of SrO doping that can saturate all the AlO sites. Importantly, this provides a method of subsequently depositing catalytically active elements on just the AlO or AlO sites, which can provide a different catalytic activity or stability compared to the AlO binding site.

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2016-01-01
2024-10-08
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References

  1. K. Wefers, C. Misra, “Oxides and Hydroxides of Aluminum”, Alcoa Technical Paper No. 19, Aluminum Company of America, USA, 1987 LINK https://www.alcoa.com/global/en/innovation/papers_patents/pdf/TP19_Wefers.pdf [Google Scholar]
  2. G. Busca, F. C. Jentoft, ‘Structural, Surface, and Catalytic Properties of Aluminas’ in “Advances in Catalysis”, ed. Volume 57, Academic Press, USA, 2014, pp. 319404 [Google Scholar]
  3. M. Trueba, S. P. Trasatti, Eur. J. Inorg. Chem., 2005, (17), 3393 LINK http://dx.doi.org/10.1002/ejic.200500348 [Google Scholar]
  4. J. S. J. Hargreaves, A. L. Munnoch, Catal. Sci. Technol., 2013, 3, (5), 1165 LINK http://dx.doi.org/10.1039/c3cy20866d [Google Scholar]
  5. K. Keyvanloo, J. B. Horton, W. C. Hecker, M. D. Argyle , Catal. Sci. Technol., 2014, 4, (12), 4289 LINK http://dx.doi.org/10.1039/c4cy00510d [Google Scholar]
  6. C. Lucarelli, S. Albonetti, A. Vaccari, C. Resini, G. Taillades, J. Roziere, K.-E. Liew, A. Ohnesorge, C. Wolff, I. Gabellini, D. Wails, Catal. Today, 2011, 175, (1), 504 LINK http://dx.doi.org/10.1016/j.cattod.2011.02.056 [Google Scholar]
  7. V. Novák, P. Kočí, M. Marek, F. Štěpánek, P. Blanco-García, G. Jones, Catal. Today, 2012, 188, (1), 62 LINK http://dx.doi.org/10.1016/j.cattod.2012.03.049 [Google Scholar]
  8. H.-Y. Chen, H.-L. Chang, Johnson Matthey Technol. Rev., 2015, 59, (1), 64 LINK http://www.technology.matthey.com/article/59/1/64-67/ [Google Scholar]
  9. J. Kašpar, P. Fornasiero, N. Hickey , Catal. Today, 2003, 77, (4), 419 LINK http://dx.doi.org/10.1016/S0920-5861(02)00384-X [Google Scholar]
  10. C.-W. Yi, J. H. Kwak, C. H. F. Peden, C Wang, J. Szanyi , J. Phys. Chem. C, 2007, 111, (41), 14942 LINK http://dx.doi.org/10.1021/jp0763376 [Google Scholar]
  11. C. Verrier, J. H. Kwak, D. H. Kim, C. H. F. Peden, J. Szanyi , Catal. Today, 2008, 136, (1–2), 121 LINK http://dx.doi.org/10.1016/j.cattod.2007.12.138 [Google Scholar]
  12. M. Taoufik, K. C. Szeto, N. Merle, I. D. Rosal, L. Maron, J. Trébosc, G. Tricot, R. M. Gauvin, L. Delevoye, Chem. Eur. J., 2014, 20, (14), 4038 LINK http://dx.doi.org/10.1002/chem.201304883 [Google Scholar]
  13. A. J. Vega, R. E. Wasylishen, ‘Quadrupolar Nuclei in Solids’, in “eMagRes”, ed. John Wiley & Sons, Inc, Hoboken, New Jersey, USA, 2010 LINK http://dx.doi.org/10.1002/9780470034590.emrstm0431.pub2 [Google Scholar]
  14. M. E. Smith, E. R. H. van Eck, Prog. Nucl. Magn. Reson. Spectrosc., 1999, 34, (2), 159 LINK http://dx.doi.org/10.1016/s0079-6565(98)00028-4 [Google Scholar]
  15. P. Nortier, P. Fourre, A. B. M. Saad, O. Saur, J. C. Lavalley, Appl. Catal., 1990, 61, (1), 141 LINK http://dx.doi.org/10.1016/S0166-9834(00)82140-5 [Google Scholar]
  16. B. A. Huggins, P. D. Ellis , J. Am. Chem. Soc., 1992, 114, (6), 2098 LINK http://dx.doi.org/10.1021/ ja00032a025 [Google Scholar]
  17. J. J. Fitzgerald, G. Piedra, S. F. Dec, M. Seger, G. E. Maciel, J. Am. Chem. Soc., 1997, 119, (33), 7832 LINK http://dx.doi.org/10.1021/ja970788u [Google Scholar]
  18. H. D. Morris, P. D. Ellis, J. Am. Chem. Soc., 1989, 111, (16), 6045 LINK http://dx.doi.org/10.1021/ja00198a012 [Google Scholar]
  19. D. Coster, A. L. Blumenfeld, J. J. Fripiat , J. Phys. Chem., 1994, 98, (24), 6201 LINK http://dx.doi.org/10.1021/j100075a024 [Google Scholar]
  20. V. Vitzthum, P. Miéville, D. Carnevale, M. A. Caporini, D. Gajan, C. Copéret, M. Lelli, A. Zagdoun, A. J. Rossini, A. Lesage, L. Emsley, G. Bodenhausen, Chem. Commun., 2012, 48, (14), 1988 LINK http://dx.doi.org/10.1039/c2cc15905h [Google Scholar]
  21. D. Lee, N. T. Duong, O. Lafon, G. De Paëpe , J. Phys. Chem. C, 2014, 118, (43), 25065 LINK http://dx.doi.org/10.1021/jp508009x [Google Scholar]
  22. R. Wischert, P. Florian, C. Copéret, D. Massiot, P. Sautet, J. Phys. Chem. C, 2014, 118, (28), 15292 LINK http://dx.doi.org/10.1021/jp503277m [Google Scholar]
  23. Y. Rozita, R. Brydson, T. P. Comyn, A. J. Scott, C. Hammond, A. Brown, S. Chauruka, A. Hassanpour, N. P. Young, A. I. Kirkland, H. Sawada, R. I. Smith , ChemCatChem, 2013, 5, (9), 2695 LINK http://dx.doi.org/10.1002/cctc.201200880 [Google Scholar]
  24. R. Rinaldi, F. Y. Fujiwara, W. Hölderich, U. Schuchardt, J. Catal., 2006, 244, (1), 92 LINK http://dx.doi.org/10.1016/j.jcat.2006.08.024 [Google Scholar]
  25. G. W. Wagner, R. A. Fry, J. Phys. Chem. C, 2009, 113, (30), 13352 LINK http://dx.doi.org/10.1021/jp902474z [Google Scholar]
  26. J. H. Kwak, J. Hu, D. Mei, C.-W. Yi, D. H. Kim, C. H. F. Peden, L. F. Allard, J. Szanyi, Science, 2009, 325, (5948), 1670 LINK http://dx.doi.org/10.1126/science.1176745 [Google Scholar]
  27. J. H. Kwak, J. Z. Hu, D. H. Kim, J. Szanyi, C. H. F. Peden, J. Catal., 2007, 251, (1), 189 LINK http://dx.doi.org/10.1016/j.jcat.2007.06.029 [Google Scholar]
  28. J. B. Peri, J. Phys. Chem., 1965, 69, (1), 220 LINK http://dx.doi.org/10.1021/j100885a033 [Google Scholar]
  29. H. Knözinger, P. Ratnasamy, Catal. Rev.: Sci. Eng., 1978, 17, (1), 31 LINK http://dx.doi.org/10.1080/03602457808080878 [Google Scholar]
  30. A. A. Tsyganenko, P. P. Mardilovich, J. Chem. Soc., Faraday Trans., 1996, 92, (23), 4843 LINK http://dx.doi.org/10.1039/ft9969204843 [Google Scholar]
  31. M. Digne, P. Sautet, P. Raybaud, P. Euzen , H. Toulhoat , J. Catal., 2004, 226, (1), 54 LINK http://dx.doi.org/10.1016/j.jcat.2004.04.020 [Google Scholar]
  32. A. R. Ferreira, E. Küçükbenli, S. de Gironcoli, W. F. Souza, S. S. X. Chiaro, E. Konstantinova, A. A. Leitão , Chem. Phys., 2013, 423, 62 LINK http://dx.doi.org/10.1016/j.chemphys.2013.06.024 [Google Scholar]
  33. E. C. Decanio, J. C. Edwards, J. W. Bruno, J. Catal., 1994, 148, (1), 76 LINK http://dx.doi.org/10.1006/jcat.1994.1187 [Google Scholar]
  34. F. Deng, G. Wang, Y. Du, C. Ye, Y. Kong, X. Li, Solid State Nucl. Magn. Reson., 1997, 7, (4), 281 LINK http://dx.doi.org/10.1016/S0926-2040(96)01281-7 [Google Scholar]
  35. M. Delgado, F. Delbecq, C. C. Santini, F. Lefebvre, S. Norsic, P. Putaj, P. Sautet, J.-M. Basset, J. Phys. Chem. C, 2012, 116, (1), 834 LINK http://dx.doi.org/10.1021/jp208709x [Google Scholar]
  36. N. Huittinen, P. Sarv, J. Lehto, J. Colloid Interface Sci., 2011, 361, (1), 252 LINK http://dx.doi.org/10.1016/j.jcis.2011.05.055 [Google Scholar]
  37. E. L. Hahn, D. E. Maxwell, Phys. Rev., 1951, 84, (6), 1246 LINK http://dx.doi.org/10.1103/PhysRev.84.1246 [Google Scholar]
  38. D. Massiot, C. Bessada, J. P. Coutures, F. Taulelle, J. Magn. Reson., 1990, 90, (2), 231 LINK http://dx.doi.org/10.1016/0022-2364(90)90130-2 [Google Scholar]
  39. S. R. Hartmann, E. L. Hahn, Phys. Rev., 1962, 128, (5), 2042 LINK http://dx.doi.org/10.1103/PhysRev.128.2042 [Google Scholar]
  40. A. J. Vega, J. Magn. Reson., 1992, 96, (1), 50 LINK http://dx.doi.org/10.1016/0022-2364(92)90287-h [Google Scholar]
  41. S. Hayashi, Solid State Nucl. Magn. Reson., 1994, 3, (2), 93 LINK http://dx.doi.org/10.1016/0926-2040(94)90027-2 [Google Scholar]
  42. S. E. Ashbrook, S. Wimperis, J. Chem. Phys., 2004, 120, (6), 2719 LINK http://dx.doi.org/10.1063/1.1638995 [Google Scholar]
  43. P. J. Chupas, C. P. Grey, J. Catal., 2004, 224, (1), 69 LINK http://dx.doi.org/10.1016/j.jcat.2004.02.013 [Google Scholar]
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