Abstract
Hierarchical micro-sized zeolite aggregates with the MEL structure were prepared hydrothermally from a tetrabutylammonium hydroxide(TBAOH)-tetraethyl orthosilicate(TEOS)-H2O system. The obtained microsized silicalite-2 microspheres had sizes larger than 10 μm, high BET surface area(460 m2·g-1), and large pore volume(0.74 cm3·g-1). The formation of micro-sized spheres alleviates preparation and application difficulties.The presence of inter-crystalline mesopores originating from the spontaneous assembly of nano-sized primary particles during hydrothermal synthesis gives the advantages of nanoparticles, reducing diffusion limitations.The introduction of titanium does not strongly affect the morphology and textural properties of the MEL-type zeolite, which are quite similar to those of silicalite-2 aggregates. The micro-sized titanium silicalite-2(TS-2)microspheres showed comparable catalytic activity in phenol hydroxylation to that of titanium silicalite-1(TS-1) of size 100-200 nm, and were easily recovered by traditional filtration, simplifying the separation and recovery compared with nano-sized TS-1.
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