Time-resolved in situ
13C, 27Al, and 29Si MAS NMR and
ex situ
XRD, X-ray
fluorescence, and TG studies have been applied
for the elucidation of the mechanisms of hydrothermal synthesis of
zeolite BEA from a clear solution and a dense hydrogel. Isotopic labeling
with 29Si and 13C isotopes has been used to
follow the fate of siliceous species and structure-directing agent
((13CH3-CH3)4NOH)). The
results point to different mechanistic pathways depending on silicate
speciation in the initial reaction mixture: (i) an aggregation/nucleation
process for the reaction mixture prepared from a colloidal silica
source and (ii) solution-mediated crystallization for the reaction
mixture prepared from a dense silica hydrogel. The products obtained
have been characterized using a set of physicochemical methods including
XRD, X-ray fluorescence analysis, TEM, low-temperature nitrogen adsorption–desorption,
and NH3-TPD. The results demonstrate that the crystallization
mechanism affects the crystal size and morphology: the aggregation/nucleation
process leads to very tiny crystals with a size of 5–15 nm,
whereas solution-mediated crystallization results in dense polycrystals
with a size of 300–700 nm with the core enriched with Al. The
evaluation of the catalysts in liquid-phase alkylation of benzene
with propylene points to the higher activity of zeolite BEA obtained
from a colloidal silica source.