Growth Mechanism Study on b-axis Oriented MFI Zeolite with MD Simulation

doi:10.6023/A1203041

Abstract

Co-templating role in the growth of b-axis oriented siliceous MFI type zeolite crystals was studied by molecular dynamic (MD) simulation. A siliceous supercell consisting of 2×2×2 unit cell is adopted as the inner part of the simulated structure for the zeolite. The crystal structures, adopted as simulated growing part of the zeolite, are four cleavage surface models along a or b axis individually, which cleaved from a supercell consisting of 1×1×2 unit cell and the Si-O hanging bonds are saturated by H atoms. The dynamic behaviors of two templates (n-propylamine and hexamethylene tetramine) in the cages of channel intersections and the opening channel windows were investigated with NVT MD simulations in 450 K for 5×10⁵ fs each run, using pcff forcefields. The simulations were performed by Discover module from Accelrys Material Studio. The interaction energies between the templates and the zeolite, and the average values of coordinates imaging the trajectories of the templates in times of whole MD simulation, are used as two indicators for investigating the dynamic adsorption sites and the size match with the channel wall for the templates. The results indicate: (1) hexamethylene tetramine (HMTA) molecule is hold at the opening window of the channel along a axis (site I) and extruded out of the opening window of channel along b axis (site III) to nearby crystal-growing site (site IV); (2) mean-squared-displacement (MSD) analysis reveals that strong interaction exists between n-propylamine molecule and the zeolite because of the fact that N-atom is sticking to the adsorption site while other atoms of the molecule are rotating and moving with freedom. On the other hand, all atoms of HMTA molecule are almost frozen in the constrained space of the channel cage. As an evidently deduction, n-propylamine molecules play a major directing role in the formation and the growth of the zeolite crystals, while HMTA molecules promote the growth of the crystal surface along a axis and impede the growth of the crystal surface along b axis.

Key words: MD simulation, MFI zeolite, oriented growth, template

Cite this article

Yu Hui, Guo Juan, Wang Jing, Long Yingcai. Growth Mechanism Study on b-axis Oriented MFI Zeolite with MD Simulation[J]. Acta Chimica Sinica, 2012, 70(14): 1543-1550.

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