Nanoparticle silicalite-1 crystallization from clear solutions: Nucleation

Despite much effort spent by various research groups, there remain many aspects of nanoparticle silicalite-1 crystallization from clear solutions which require further investigation. In order to shed light, especially on the nucleation of silicalite-1, particle growth at 100 degrees C from several starting compositions known to yield colloidal silicalite-1, which have been studied previously by other researchers using various techniques, was followed in this study by laser light scattering using scattering angles of 90 degrees and 173 degrees, and zeta potential and pH measurements. Crystallinity was monitored by X-ray diffraction, Fourier transform infrared analysis and transmission electron microscopy. Thermogravimetric analyses and density measurements were also used to characterize the products obtained at various times during the syntheses. The results demonstrate that the distinct time of sudden jump in the effective diameter of the nanoparticles in solution, as observed more clearly by using the back-scattering device, and which marks the beginning of the constant linear growth rate of the particles, corresponds to the nucleation of the silicalite-1 crystal structure. This time was also shown to coincide with the exo-endo thermal switch time of the reaction mechanism, which has been observed previously by another research group. Nucleation was accompanied by an aggregation of a population of smaller particles, as indicated by the broadening of the particle size distribution, and the variation of the pH and zeta potential values during synthesis. (C) 2008 Elsevier Inc. All rights reserved.