Abstract

Hierarchical Beta zeolites have been prepared employing two strategies of synthesis for the generation of mesopores with different size distribution. In both cases, the starting gel was subjected to pre-crystallization to induce the formation of protozeolitic nanounits. The first strategy involves the reorganization of the protozeolitic nanounits by incorporation of a surfactant (cetyltrimethylammonium bromide, CTAB), whereas the second one is based on the use of a silanization agent (phenylaminopropyl-trimethoxysilane, PHAPTMS) that it is grafted to the outer part of the nanounits to avoid their total merge during the crystallization process. In addition, conventional Beta zeolite and ordered mesoporous aluminosilicates have been prepared and employed as reference samples. All materials have been characterized by a number of techniques, whereas their catalytic behavior has been evaluated in the cracking of high density polyethylene (HDPE). The h-Beta (CTAB) sample shows a narrower mesopore size distribution, more uniform and stable tetrahedral Al species and a higher acid strength than the material obtained from silanized nanounits, although the latter exhibits a larger accessibility as denoted by its higher mesopore/external surface area (351m2/g in h-Beta (PHAPTMS) versus 228m2/g in h-Beta (CTAB)). While the ordered mesoporous aluminosilicates were almost inactive in HDPE cracking (<5wt% of conversion) due to its weak acidity, high plastic conversions were obtained over the zeolite Beta samples (>50wt% of conversion). The results obtained indicate that the overall catalytic activity depends mainly on the accessibility to the active sites, whereas the product selectivity is rather determined by the acid strength of the zeolite catalysts. Thus, h-Beta (CTAB) sample promoted in a great extension both end-chain cracking and aromatization reactions due to its high acid strength.

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