In the synthesis of mesoporous materials, the use of a template with an adequate porosity is normally favoured. As far as silica is concerned, many sophisticated procedures directed towards this goal have been published. It is already well documented that rice hull contains relatively pure silica after combustion of the residual organic matter. The authors of this contribution have recently demonstrated that large surface area silicates react with glycerol around 200• C to give depolymerized silica with a chemical composition similar to that of poly-alkoxides. The interest in this so-called depolymerization is to allow easy formation of reactive gels which retain the memory of the porous structure of the original starting material. Rice hull ash (RHA), obtained after combustion of the organic residues at 500• C, gives a silica characterized by mesopores with an average diameter about 3.5 nm. It is shown that RHA reacts with glycerol at 200• C to form gels which, after hydrolysis and calcination, retain the mesoporous character. The hydrolysis procedure and especially, the pH is important for the distribution of the mesoporosity. The very simple reaction of a by-product of the food industry with glycerol, a ''green reagent'', gives a mesoporous solid silica in the form of a reactive gel, with many potential uses. Its use in a new procedure for the synthesis of a supported ZSM-5 zeolite has been demonstrated.
In glycerol, near 200 degrees C, the silicate networks of mesoporous silicates and zeolites undergo a deep depolymerization process. In a few hours, depending on the initial concentration of the solid in glycerol and on the temperature, amorphous gels are obtained. In these gels, a fraction of the Si-O-Si bonds are transformed into Si-O-C. The constitutional aluminum remains bound to the silica network in the gel. The short range ordering is maintained to some extent: the size of the smallest structural unit in gels obtained from zeolites is in the range of the cubic nanometer, nm3.
As shown recently, the networks of mesoporous high-surface-area silicates and zeolites undergo a deep depolymerization process in glycerol, near 200 degrees C. Within 1 h, X-ray diffraction analysis amorphous gels are obtained. However, some local ordering subsists as demonstrated by a striking similarity between the silicon and aluminum high-resolution solid-state NMR spectra before and after the reaction. The residual organization could be investigated indirectly in studying the recrystallization of these gels in the presence or absence of structure-directing agents. Were this attempt successful, the way should be opened for the synthesis of molecular sieves starting from gels obtained from naturally occurring zeolites. Here, it will be shown that an amorphous gel obtained from HZSM-5 recovers the initial long-range structure of the parent material in a few hours at 85 degrees C in the presence of an aqueous solution of tetrapropyl ammonium (TPA) or NH3. The recrystallization of HY requires the presence of tetramethylammonium, but about 25% of the crystallization is obtained rapidly (approximately = 1 day) at 80 degrees C with ammonia. Hypotheses about the preorganized structural units are presented. The value of the Si-O-Si angle in the silica cluster seems to be of paramount importance.
4A Zeolite was synthesized using rice husk ash (RHA) as a raw material in a microwaveassisted hydrothermal synthesis. Two new procedures were proposed: procedure A, using RHA as the raw material, and procedure B, using the depolymerized RHA. Both procedures were performed using microwave-assisted hydrothermal synthesis, and neither synthesis required an aging time. Crystallinities of over 90 and 80% were reached at 100 °C after 30 min of microwave heating for procedures A and B, respectively. The obtained zeolites were used as warm mix asphalt additives, and the performance of the zeolite obtained from procedure A was better. Additionally, the zeolite obtained from procedure A and commercial silane were used separately as asphaltaggregate adhesion promoter. An increase in the adhesion percentage from 30% of a blank sample to 94% was observed.
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