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Acid and redox activity of template-free Al-rich H-BEA* and Fe-BEA* zeolites

Authors
Journal
Journal of Catalysis
0021-9517
Publisher
Elsevier
Identifiers
DOI: 10.1016/j.jcat.2014.06.024
Keywords
  • Beta (Bea*) Zeolite
  • Acid Strength
  • Cracking Of Decane
  • Alkylation Of Aromatics
  • Hydroamination Of Styrene With Aniline
  • Iron Zeolites
  • Fe-Beta
  • Nh3-Scr-Nox
  • Decomposition Of N2O

Abstract

Abstract Al-rich template-free BEA* zeolite (Si/Al 4.6) was synthesized and its structure was analyzed in comparison with the conventional H-BEA* zeolite of Si/Al 11.3 using XRD, N2 sorption, SEM, FTIR, 27Al 3Q and 29Si MAS NMR spectroscopy, and DFT calculation of the deprotonation energies. The Al-rich H-BEA* exhibited a high concentration of Brønsted and Lewis sites, both of high acid strength, although AlSiAl sequences were present in the framework. In Al-rich Fe-BEA* the exchanged Fe ions, Fe–oxo species, and Fe–oxo oligomers were identified by UV–vis spectroscopy. Cracking of n-decane, alkylation of benzene with benzyl alcohol and hydroamination of styrene with aniline to (anti)Markovnikov phenyl-[2-phenylethyl]amine over H-BEA*, and decomposition of N2O and NH3-SCR-NOx over Fe-BEA* were investigated in relation to the concentration and nature of acid and Fe-redox sites. The high concentration of Al-related active sites and the highly regular structure of Al-rich beta zeolite are directly manifested in enhanced activity compared with conventional Si-rich beta zeolite.

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