Variation of particle size and its distribution during the synthesis of silicalite-1 nanocrystals

Recent studies imply that the external surface area of the nanozeolite product may, at least in some cases, be related to the average size of the particle population participating in aggregative nucleation, a population which itself is a product of aggregation of even smaller primary nanoparticles. This possibility puts more importance on our understanding of the variation of particle size and its distribution during the crystallization of zeolite nanoparticles. Variation of the particle size and PSD during nanoparticle silicalite-1 crystallization was followed with respect to time by a laser light scattering device with a scattering angle of 173°, for several starting synthesis compositions. Effects of varying TPAOH and water contents in the starting synthesis mixtures on the variation with time of the particle sizes and PSDs, especially across the two distinct aggregation events, were investigated. The products were also analyzed by XRD and AFM. Parallel to the decrease in the average particle size of the final product population with increasing alkalinity and organic template content, its PSD was observed to become narrower too. A reversal in the dependence on TPAOH content, of the average size of the population formed by aggregation, with respect to that of the population participating in aggregation, was observed across both aggregation events, implying that smaller particles aggregated to form larger particles, while larger particles aggregated to form smaller particles during these processes, and this was also seen from the AFM images, to be reflected to the surface features of the final product particles.

Variation of the PSDs with time during the crystallization of silicalite-1 nanoparticles from 25SiO2:xTPAOH:480H2O:100EtOH, for x = 3 (R1), 6 (R2) and 9 (R3).Figure optionsDownload as PowerPoint slideHighlights
► Product PSD gets narrower with increasing TPAOH content of the starting mixture.
► Average size of the initial nanoparticle population decreases with increasing TPAOH.
► Average size of the second population increases with increasing TPAOH.
► Average sizes of the third population and the product decrease with increasing TPAOH.