The concept of pseudomorphic transformation was used to transform amorphous mesoporous silica beads with different size (20, 50 and 75 µm) into hierarchical MFI-type zeolite beads composed of ZSM-5 nanosheets. The beads were synthesized under hydrothermal conditions at different temperatures and treatment times, with and without mechanical stirring? (à quelle étape?). The influence of the different synthesis parameters was investigated by X-Ray Diffraction, Scanning Electron Microscopy, Transmission Electron Microscopy, X-Ray Fluorescence, Nitrogen adsorption-desorption measurements, 27 Al solid-state Nuclear Magnetic Resonance, Energy-Dispersive X-Ray analysis and Thermogravimetric analysis.Well-crystallized 20 µm ZSM-5 nanosheets beads similar in size and shape to the original mesoporous amorphous silica beads were obtained after a hydrothermal treatment at 150 °C for 5 days in a tumbling oven and 2 days in static at 120 °C. The influence of the bead size on the pseudomorphic transformation was studied in order to prepare well-crystallized ZSM-5 nanosheets beads of 50 and 75 µm. Results showed that the required time of the static treatment at 120°C increases when the size of the parent silica spheres increases. This is explained by the fact that crystallization starts from the outer bead surface toward the center.
Binderless pure silica zeolites (zeosils) spheres and hollow spheres with a diameter of 20 µm composed of silicalite-1 nanosheets particles were prepared by pseudomorphic transformation of spherical silica beads using different temperatures (110, 130, and 150 °C) and treatment times (1–5 days) in order to adapt the local dissolution rate of silica to the crystallization rate of silicalite-1 nanosheets allowing to preserve the initial morphology of the silica beads. Fully crystalline beads of 20 µm were obtained at 110 °C for 5 days, whereas hollow spheres similar in size were synthesized at higher temperatures. The crystallization process seems to begin at the outer surface of the amorphous silica beads and spreads with the time in the interior of the beads leading to a dissolution of the inner amorphous part of the beads to create zeosil hollow spheres for the highest treatment temperatures (130 and 150 °C). The dissolution rate of the inner amorphous part of the beads increases by increasing the hydrothermal treatment temperature from 130 to 150 °C. The silicalite-1 beads synthesized at 110 °C for 5 days showed to be promising for rapid molecular decontamination by adsorbing n-hexane in larger amount than the silicalite-1 conventional big crystals in powder forms.
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