Highly Efficient Nanocrystalline Zirconosilicate Catalysts
for the Aminolysis, Alcoholysis, and Hydroamination Reactions
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Abstract
Nanocrystalline zirconosilicates
and titanosilicates with MFI framework
structure were hydrothermally synthesized by the addition of organosilanes
in the synthesis composition of conventional zirconosilicate and titanosilicate
materials. Materials were characterized by a complementary combination
of X-ray diffraction, nitrogen sorption, scanning/transmission electron
microscopy (S/TEM), ammonia temperature-programmed desorption (TPD),
Fourier transform infrared (FT-IR) spectroscopy, and ultraviolet–visible
(UV-vis) spectroscopic investigations. Nanocrystalline zeolite catalysts
of the present study are reusable. They exhibit significantly higher
catalytic activities in aminolysis and alcoholysis compared with the
hitherto known catalysts. A range of β-amino alcohols/β-alkoxy
alcohols with high regioselectivity were synthesized using zirconosilicates.
Application of these materials was also extended in the synthesis
of aminoesters by the hydroamination reaction of methyl acrylates
and amines. Structure activity relationship was explained based on
acidity measurements, reactivity of amines/alcohols, and adsorption
of reactants on catalysts
