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Synthesis and Characterization of Hierarchical ZSM-5 Zeolites with Outstanding Mesoporosity and Excellent Catalytic Properties.

ABSTRACT: A novel soft-template (ST) is fabricated and successfully employed as mesoporogen to synthesis hierarchical ZSM-5 zeolites with outstanding mesoporosity and high hierarchy factors. The as-produced soft-template can connect steadily with the MFI frameworks by covalent bonds of -Si-O-Si- during the high-temperature hydrothermal crystallization process. This type of connection mode can effectively avoid the formation of amorphous materials, and the specific structure of this soft-template can efficiently introduce plentiful of mesopores with few micropores being consumed. The particles of as-synthesized hierarchical ZSM-5 zeolites are in size of about 1 ?m, which are made up of nanocrystals of 60-150 nm. The structure parameters of these samples are characterized with the techniques of X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, nitrogen sorption, scanning electron microscope (SEM), transmission electron microscope (TEM), NH3 temperature-programmed desorption (NH3-TPD) and thermogravimetric (TG). Due to the nature of zeolites and great microporosity, these hierarchical samples present great tolerance of hydrothermal treatment. And because of the intracrystalline mesopores, large external surface areas, and abundant accessible acid sites, whether in conversion rate of reactants or selectivity of products, the hierarchical samples exhibit excellent catalytic performance in the reactions of alkylation between benzene and benzyl alcohol, cracking of 1,3,5-tri-isopropylbenzene, and thermal cracking of low-density polyethylene (LDPE), respectively.

SUBMITTER: Song G

PROVIDER: S-EPMC6237675 | biostudies-literature | 2018 Nov

REPOSITORIES: biostudies-literature

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Synthesis and Characterization of Hierarchical ZSM-5 Zeolites with Outstanding Mesoporosity and Excellent Catalytic Properties.

Song Guoqiang G Chen Wenting W Dang Peipei P Yang Shengyuan S Zhang Yuan Y Wang Yuanyi Y Xiao Ruidi R Ma Rong R Li Fuxiang F

Nanoscale research letters 20181115 1

A novel soft-template (ST) is fabricated and successfully employed as mesoporogen to synthesis hierarchical ZSM-5 zeolites with outstanding mesoporosity and high hierarchy factors. The as-produced soft-template can connect steadily with the MFI frameworks by covalent bonds of -Si-O-Si- during the high-temperature hydrothermal crystallization process. This type of connection mode can effectively avoid the formation of amorphous materials, and the specific structure of this soft-template can effic ...[more]

PMID: 30443775

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Project description:In this paper, the ultrasonic-assisted desilication technique was reported as an attractive and efficient way for the preparation of hierarchical zeolites with MFI structure type. The prepared materials were used as active catalysts for the dehydration of ethanol into diethyl ether and ethylene. For all catalysts, the selectivity to diethyl ether was ca 95% or higher up to 210 °C, with catalytic activity in the range of 40-68%. In case of desilicated zeolites, at 270-290 °C, the conversion of ethanol was full with selectivity to ethylene ca 80%. MFI-type commercial zeolite was treated with a sodium and/or tetrabutylammonium hydroxide aqueous solutions (NaOH or NaOH/TBAOH) for 30 min. In the case of the application of ultrasounds, a QSonica Q700 sonicator (60 W and 20 kHz) equipped with a "1" diameter horn was used. In all cases, desilication was performed in an ice bath in order to keep the procedure conditions at low temperature. It was indicated that the use of ultrasounds during desilication procedure caused higher extraction of silicon and aluminum, which was connected with an elevated mesoporosity in relation to the samples modified in the absence of ultrasounds. Ultrasonic-assisted treatment of MFI-type zeolite caused also an apparent formation of numerous holes inside zeolite grains, resembling the look of "swiss cheese". Furthermore, it was indicated that the samples prepared using ultrasonic irradiation exhibited enhanced catalytic properties in the dehydration of ethanol. For instance, MFI-type zeolite treated with NaOH/TBAOH alkaline mixture containing 10 mol% of TBAOH in the presence of ultrasounds (M-10 s) demonstrated higher both conversion of ethanol (59% vs. 47%) and selectivity to diethyl ether (95% vs. 93%) in comparison with zeolite modified conventionally (M-10c). The best catalyst was zeolite ultrasonically desilicated with NaOH/TBAOH solution of 70 mol% of TBAOH (M-70s). Generally, this catalyst indicated the highest conversion of ethanol, very high selectivity to diethyl ether (94-100%) at 150-210 °C and the highest selectivity to ethylene among investigated catalysts (21%, 66% and 84%) at 230 °C, 250 oC and 270 °C.

Dataset Information

Synthesis and Characterization of Hierarchical ZSM-5 Zeolites with Outstanding Mesoporosity and Excellent Catalytic Properties.

Publications

Synthesis and Characterization of Hierarchical ZSM-5 Zeolites with Outstanding Mesoporosity and Excellent Catalytic Properties.

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