Characterization of MFI and BEA embedded in mesoporous molecular sieve - Thermal stability

Heidi Österholm*, Narendra Kumar, Marina Lindblad, Marja Tiitta, Tapio Salmi, Dmitry Murzin

*Korresponderande författare för detta arbete

Forskningsoutput: TidskriftsbidragArtikelVetenskapligPeer review

3 Citeringar (Scopus)

Sammanfattning

MFI and BEA zeolite seeds were embedded in MCM-41 gel mixture with or without additional aluminum isopropoxide. These novel meso-microporous molecular sieves, NK-MM-MFI and NK-MM-BEA, contain zeolite crystallites surrounded by a mesoporous ordered phase. A thorough characterization was made utilizing XRF, XRD, N 2-physisorption and 27Al MAS NMR as well as acidity and acid site strength measurements by 1H MAS NMR and NH 3-TPD. Al content was varied from 0.4 to 3.9 wt.% to tailor acidity and porosity. The embedded NK-MM-MFI and NK-MM-BEA materials were compared to pure zeolites and MCM-41. The mesoporous phase had a stronger effect on porosity and number of acid sites, while acid site strength was dominated by the microporous zeolite seeds. Total number of acid sites increased linearly with Al content, which also was true for Brønsted acidity in NK-MM-MFI, while no effect on Brønsted acidity was observed in NK-MM-BEA. The thermal stability of NK-MM-MFI and NK-MM-BEA, as well as of MFI, BEA and MCM-41, was studied by calcination in air at 773, 873 and 1173 K. The exposure to 1173 K caused a decrease in unit cell dimension of the MCM-41 phase. The unit cell shrinkage was the largest in pure MCM-41 and the smallest in NK-MM-MFI. The zeolite addition stabilized the mesoporous structure, effect of MFI was more pronounced than of BEA. Total acidity and Brønsted acidity decreased, while only minor loss of tetrahedral framework Al was observed. The loss in acidity was caused by thermal dehydroxylation and being thus reversible. It was shown that the structure, porosity and framework Al were thermally stable in NK-MM-MFI and NK-MM-BEA.

OriginalspråkEngelska
Sidor (från-till)124-132
Antal sidor9
TidskriftMicroporous and Mesoporous Materials
Volym154
DOI
StatusPublicerad - 15 maj 2012
MoE-publikationstypA1 Tidskriftsartikel-refererad

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