Síntese e caracterização da zeólita HZSM-5 nanocristalina com porosidade hierárquica aplicada no craqueamento de polímeros

Zeolites are widely used by the industry in catalysis processes, adsorption, separation and ion exchange. However, the presence of only micropores limits the diffusion of bulky molecules in their channels, favoring the occurrence of adverse reactions due to long residence time of the reactants an...

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Autor principal: Figueiredo, Aneliése Lunguinho
Outros Autores: Fernandes Júnior, Valter José
Formato: doctoralThesis
Idioma:por
Publicado em: Universidade Federal do Rio Grande do Norte
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Endereço do item:https://repositorio.ufrn.br/jspui/handle/123456789/20554
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Resumo:Zeolites are widely used by the industry in catalysis processes, adsorption, separation and ion exchange. However, the presence of only micropores limits the diffusion of bulky molecules in their channels, favoring the occurrence of adverse reactions due to long residence time of the reactants and products are transported through the micropores of the zeolite. In order to overcome this problem has been studied in this work synthesis methods for obtaining hierarchical nanocrystalline ZSM-5 zeolite synthesized in the absence of organic template. First it carried out a synthesis of zeolite ZSM-5 by the seed-assisted method from an organic-templatefree system, where the samples were synthesized utilizing three different types of seeds: two of these based on aqueous clear solutions containing the ZSM-5 precursors (non-silanized and silanized) and the third seed based on a commercial ZSM-5 zeolite in powder form, in order to direct the formation of the MFI structure. The second method used was the silanization process, using as silanizante agent phenylaminopropyltrimethoxysilane (PHAPTMS), in order to lessen or prevent the growth of zeolitic crystals of ZSM-5, obtaining favoring smaller crystals. The synthesis of ZSM-5 was also performed in the absence of organic template 180°C for 27 hours after addition of PHAPTMS. All synthesized samples were characterized by several techniques, among them X Ray Diffraction (XRD), Fourier Transform Infrared Spectroscopy (FTIR), Argon adsorption-desorption, Electronic Microscopy (SEM and TEM), and Temperature Programmed Desorption of Ammonia (NH3-TPD). It was noted that the use of seeds gives a higher BET surface area and causes an increase in the external surface area outside due to the decreasing size of the crystals. Similarly for sample functionalized with silanizante agent (MFI (PHAPTMS)), which is the lowest a dual system of pores, the first associated with the microporosity of the zeolite ZSM-5 (0.5 - 2 nm) and the other related to intercrystalline mesopores (2 - 6 nm), confirming the obtaining of HZSM-5 zeolite hierarchical. All samples were synthesized globular agglomerates formed by small nanounits (30 - 90 nm) with different size and morphology of crystals of zeolite HZSM-5 used as reference. The catalytic tests using the cracking of low density polyethylene (LDPE) and pyrolysis of poly(ethylene terephthalate) - PET proved that the improvement in the textural properties of the synthesized zeolite is advantageous in such processes, with a better performance when compared to the reference sample, generating products which can be useful feedstocks in the petrochemical industry.