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Mesoporous silica-aluminas derived from precipitation: a study of the acidity, textural properties and catalytic performance

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Abstract

Silica-alumina covering broad range of compositions have been obtained by combined hydrolysis precipitation. These materials were characterized mainly by solid-state NMR spectroscopy. Textural properties were investigated by measurements of nitrogen sorption, and the acidity of Brønsted sites was studied by TPD and FTIR spectroscopy using ammonia as probe molecule. The catalytic performance of these materials was studied by the Brønsted acid-catalyzed acetalization reaction. New insights into the nature of the silicate compartment and the acidity of Brønsted sites of amorphous silica-alumina have been obtained. Silica-aluminas of different silica content do not represent a homologous row. They differ mainly in the connectivity of the silicate compartment. The results show that silica-alumina contain a quantitative amount of Brønsted sites. The appearance of tetrahedral Al is closely related to silica. The concentration of tetrahedral Al, and hence Brønsted acid sites, follows a volcano shape. After increasing with SiO2 content, the site concentration reaches a maximum at 20 wt% of silica and decreases again due to the marked decrease in the total alumina content in high silica samples. Surprisingly, the catalytic activity does not follow this trend. It increases especially with high silica samples due to the interplay of acid site concentration and the strength of acid sites. The aluminosilicate compartment of high silica samples shows a high Si/Al ratio. The improved acid strength of the sites overcompensates the lower site concentration, leading to a distinctly enhanced catalytic activity.

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References

  1. Khaleel AA, Klabunde KJ (2002) Chem Eur J 8:3991

    Article  CAS  Google Scholar 

  2. Yurdakovic M, Akcay M, Toubul Y, Yurdakovic K (1999) Turk J Chem 23:319

    Google Scholar 

  3. Xu M, Lunsford JH, Goodman DW, Bhattacharyya A (1997) Appl Catal A 149:289

    Article  CAS  Google Scholar 

  4. Bourne KH, Cannings FR, Pitkethly RC (1970) J Phys Chem 71:2197

    Article  Google Scholar 

  5. Tanabe K, Hölderich W (1999) Appl Catal A 181:399

    Article  CAS  Google Scholar 

  6. Bevilacqua Montanari MT, Finocchio E, Busca G (2006) Catal Today 116:132

    Article  Google Scholar 

  7. Danielle W, Schubert U, Glöckler R, Meyer A, Noweck K, Knözinger KH (2000) Appl Catal A 196:399

    Google Scholar 

  8. Crépeau G, Montouillout V, Vimont A, Mariey L, Cseri T, Maugé F (2006) J Phys Chem B 110:15172

    Article  Google Scholar 

  9. Hunger M, Freude D, Pfeifer H, Bremer H, Jank M, Wendlandt KP (1983) Chem Phys Lett 100:29

    Article  CAS  Google Scholar 

  10. Rouxhet PG, Scokart PO, Canesson P, Defossé C, Rodrique L, Declerck FD, Leonard AJ, Delmon B, Damon JP (1976) In: Kerker M (ed) Colloid and interface science, vol 3. Academic Press, New York, p 81

    Chapter  Google Scholar 

  11. Sârbu C, Delmon B (1999) Appl Catal A 185:85

    Article  Google Scholar 

  12. Metz G, Wu XL, Smith SO (1994) J Magn Reson A 110:219

    Article  CAS  Google Scholar 

  13. Bennett E, Rienstra CM, Auger M, Lakshmi KV, Griffin RF (1995) J Chem Phys 103:6951

    Article  CAS  Google Scholar 

  14. IUPAC Reporting physorption data for gas/solid systems (1985) Pure Appl Chem 57:603

    Article  Google Scholar 

  15. Loewenstein W (1954) Am Mineral 39:92

    CAS  Google Scholar 

  16. Engelhardt G, Koller H (1994) In: Diehl P, Fluck E, Günter H, Kosfeld R, Seelig J (eds) NMR basic principles and progress. Springer Verlag, Berlin, p 1

    Google Scholar 

  17. Stach H, Jänchen J, Lohse U (1992) Catal Lett 13:9

    Article  Google Scholar 

  18. Mortier WJ (1978) J Catal 55:138

    Article  CAS  Google Scholar 

  19. Barthmeuf D (1987) Mater Chem Phys 17:64

    Google Scholar 

  20. Barthomeuf D (1994) Zeolites 14:394

    Article  CAS  Google Scholar 

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Acknowledgement

The authors thank Dr. M.-M. Pohl for recording the TEM image. The excellent assistance from Dr. U. Bentrup and Mrs. M. Halle in FTIR and ICP measurements is gratefully acknowledged.

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Authors and Affiliations

  1. Leibniz-Institute for Catalysis e. V, Albert-Einstein-Str. 29a, 18059, Rostock, Germany

    M. Bartoszek, R. Eckelt, H. Kosslick & A. Schulz

  2. Institute of Chemistry, University of Rostock, Albert-Einstein-Str. 3a, 18059, Rostock, Germany

    H. Kosslick & A. Schulz

  3. BAM – Federal Institute for Materials Research and Testing, Division I.3, Working Group NMR Spectroscopy, Richard –Willstaetter Str. 11, 12489, Berlin, Germany

    Ch. Jäger & A. Pawlik

Authors
  1. M. Bartoszek
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  2. R. Eckelt
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  3. Ch. Jäger
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  4. H. Kosslick
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  5. A. Pawlik
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  6. A. Schulz
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Correspondence to H. Kosslick.

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Bartoszek, M., Eckelt, R., Jäger, C. et al. Mesoporous silica-aluminas derived from precipitation: a study of the acidity, textural properties and catalytic performance. J Mater Sci 44, 6629–6636 (2009). https://doi.org/10.1007/s10853-009-3580-y

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  • DOI: https://doi.org/10.1007/s10853-009-3580-y

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