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A simple kinetic model based on the zeolite acid strength, the number of Brønsted acid sites, and the catalyst efficiency was developed for the cracking of n-hexane. A series of HY zeolites with a mesopore volume from 0.04 to 0.32 cm3/g was synthesized and characterized by various physical-chemical methods and tested for n-hexane cracking. The generation of mesoporosity influenced several other important parameters, such as acidity and extra-framework aluminum. Zero-length column diffusion measurements for mesitylene showed a large decrease in the characteristic diffusion time upon the introduction of mesoporosity, which changed only slightly with a further increase in mesoporosity. Similar n-hexane physisorption enthalpies were measured for all samples. The highest initial activity for n-hexane cracking per catalyst volume was observed for the sample with an intermediate mesopore volume of 0.15 cm3/g. The three mesoporous H-USY zeolites showed the same value of the intrinsic rate constant and the same activation energy. The difference in initial activity of the mesoporous zeolites was caused by the difference in the number of Brønsted acid sites. The increase in initial activity for the mesoporous zeolites compared to a microporous zeolite was caused by an increase in the acid strength. [ABSTRACT FROM AUTHOR]

Silver nanoparticles are currently one of the most studied nanostructured nanomaterials. Because nanoparticle size and dispersion act together in determining a material's physical and chemical properties, there is a continuous quest to develop size-controlled synthesis methods. Nonetheless, the instability of the nanometer-sized particles, which is caused by their tendency to aggregate irreversibly into larger particles, remains a recurrent problem. The use of confining scaffolds, such as the regular system of cages in a crystalline zeolite-type material, is often reported in the literature as an efficient solution to overcome particle migration at the surface. Silver nanoparticles encapsulated in ZSM-5 (Ag@ZSM-5) represent a new generation of adsorbent for Xe enrichment from the atmosphere that is currently being developed at the pilot scale in a Temperature Swing Adsorption (TSA) process. In this study, we have found that the presence of Cl-containing compounds in the air (VOCs) leads to a poisoning of the active silver phase by the formation of silver chloride. By a careful study of process parameters, we have found that most of the chlorine can be removed by heat treatment above 573 K so that the adsorption properties of silver are regenerated. That said, when applying 573 K temperature regeneration at the pilot scale, we observe a very minor but observable decay of xenon adsorption capacity that continues cycle after cycle. The mechanism of capacity decay is discussed in terms of (i) the residual presence of Cl at the surface of silver nanoparticles, (ii) the aggregation of silver nanoparticles into larger particles (sintering mechanism), and (iii) the acceleration of silver particle migration to the surface and sintering. [ABSTRACT FROM AUTHOR]

Whereas the synthesis principles of supported metal catalysts are well documented in the open literature, impregnation protocols on shaped bodies represent sensitive industrial know-how and are, therefore, rarely found. We investigated various synthesis parameters for both wetness (WI) and dry (DI) impregnations to prepare Pd/γ–Al2O3 alumina beads. Two kinds of catalysts were achieved: homogeneously dispersed catalysts with no metal gradient across the beads and eggshell catalysts. A combination of optical images, Castaing microprobe analysis, elemental analysis, and TEM made it possible to discriminate between catalysts according to their metal loading, location across the bead diameter, and metal dispersion. Regardless of the macropore structure of the alumina beads, we found that volatile solvents (acetone) were preferred for preparing homogeneous catalysts by WI, whereas the use of a viscous aqueous solution (water/glycerol) in DI resulted in an eggshell-type catalyst. The atomic layer deposition (ALD) method was also investigated as a physical vapor phase deposition method for preparing eggshell catalysts. Representative-shaped catalysts were tested for CO oxidation as a model reaction in order to highlight the differences between catalysts with a homogeneous metal distribution (no metal gradient) and eggshell-type. [ABSTRACT FROM AUTHOR]