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Uniform hierarchical MFI nanosheets prepared via anisotropic etching for solution-based sub-100-nm-thick oriented MFI layer fabrication.

ABSTRACT: Zeolite nanosheets have shown unprecedented opportunities for a wide range of applications, yet developing facile methods for fabrication of uniform zeolite nanosheets remains a great challenge. Here, a facile approach involving anisotropic etching with an aqueous solution of tetrapropylammonium hydroxide (TPAOH) was developed for preparing uniform high-aspect ratio hierarchical MFI nanosheets. In addition, the mechanism associated with the formation of MFI nanosheets was proposed. In the next step, a dynamic air-liquid interface-assisted self-assembly method and single-mode microwave heating were used for b-oriented MFI nanosheets monolayer deposition and controlled in-plane solution-based epitaxial growth, respectively, ensuring the formation of well-intergrown b-oriented MFI layers with sub-100-nm thickness. Moreover, our study indicated that b-oriented ultrathin MFI layers could be fabricated on diverse substrates demonstrating excellent anticorrosion capacity, ionic sieving properties, and n-/i-butane isomer separation performance.

SUBMITTER: Liu Y

PROVIDER: S-EPMC7021496 | biostudies-literature | 2020 Feb

REPOSITORIES: biostudies-literature

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Uniform hierarchical MFI nanosheets prepared via anisotropic etching for solution-based sub-100-nm-thick oriented MFI layer fabrication.

Liu Yi Y Qiang Weili W Ji Taotao T Zhang Mu M Li Mingrun M Lu Jinming J Liu Yi Y

Science advances 20200214 7

Zeolite nanosheets have shown unprecedented opportunities for a wide range of applications, yet developing facile methods for fabrication of uniform zeolite nanosheets remains a great challenge. Here, a facile approach involving anisotropic etching with an aqueous solution of tetrapropylammonium hydroxide (TPAOH) was developed for preparing uniform high-aspect ratio hierarchical MFI nanosheets. In addition, the mechanism associated with the formation of MFI nanosheets was proposed. In the next s ...[more]

PMID: 32110732

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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.

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Uniform hierarchical MFI nanosheets prepared via anisotropic etching for solution-based sub-100-nm-thick oriented MFI layer fabrication.

Publications

Uniform hierarchical MFI nanosheets prepared via anisotropic etching for solution-based sub-100-nm-thick oriented MFI layer fabrication.

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