Fabrication of titanosilicate pillared MFI zeolites with tailored catalytic activity

doi:10.1007/s11705-019-1859-3

Front. Chem. Sci. Eng.

2020, Vol. 14

Issue (5) : 772-782 https://doi.org/10.1007/s11705-019-1859-3

RESEARCH ARTICLE

Fabrication of titanosilicate pillared MFI zeolites with tailored catalytic activity

Baoyu Liu¹(

), Qiaowen Mu¹, Jiajin Huang¹, Wei Tan¹, Jing Xiao²(

)

¹. School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China
². School of Chemistry and Chemical Technology, South China University of Technology, Guangzhou 510640, China

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Abstract

Titanosilicate pillared MFI zeolite nanosheets were successfully synthesized by infiltrating the mixed tetraethyl orthosilicate (TEOS)/tetrabutyl orthotitanate (TBOT) solvent into the gallery space between adjacent MFI zeolite layers. The obtained zeolite catalysts were characterized using powder X-ray diffraction, N₂ adsorption/desorption isotherms, scanning electron microscopy, transmission electron microscopy, ultraviolet–visible spectroscopy, X-ray photoelectron spectroscopy, and Fourier-transform infrared spectroscopy techniques. The H₂O₂ oxidation of dibenzothiophene (DBT) was used to evaluate the catalytic performance of the obtained titanosilicate pillared MFI zeolites. The conversion of DBT and selectivity of dibenzothiophene sulfone (DBTS) were most affected by the textural properties of the zeolites. This was attributed to the DBT and DBTS molecules being larger than micropores of the MFI zeolites. The conversion of DBT and yield of DBTS could be systematically tailored by tuning the molar ratio of the TEOS/TBOT solvent. These results implied that a balance between the meso- and microporosity of zeolites and tetrahedrally coordinated Ti(IV) active sites of titanosilicate pillars can be achieved for the preparation of desired catalysts during the oxidation of bulk S compounds.

Keywords MFI zeolite catalysis nanosheets fabrication

Corresponding Author(s): Baoyu Liu,Jing Xiao

Just Accepted Date: 15 November 2019 Online First Date: 03 January 2020 Issue Date: 25 May 2020

Cite this article:

Baoyu Liu,Qiaowen Mu,Jiajin Huang, et al. Fabrication of titanosilicate pillared MFI zeolites with tailored catalytic activity[J]. Front. Chem. Sci. Eng., 2020, 14(5): 772-782.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-019-1859-3
https://academic.hep.com.cn/fcse/EN/Y2020/V14/I5/772

Fig.1 Low- and high-angle X-ray diffraction patterns of Si/Ti-∞, Si/Ti-10, Si/Ti-20, and Si/Ti-40.

Fig.2 Energy dispersive X-ray spectroscopy mapping images of Si/Ti-10, Si/Ti-20, and Si/Ti-40 samples.

Fig.3 (a) N₂ adsorption-desorption isotherms and (b) corresponding Barrett-Joyner-Halenda pore size distribution of Si/Ti-∞, Si/Ti-10, Si/Ti-20, and Si/Ti-40 samples.

Tab.1 Textural properties of titanosilicate pillared MFI zeolites

Fig.4 Scanning electron microscopy images of (a) Si/Ti-∞, (b) Si/Ti-10, (c) Si/Ti-20, (d) Si/Ti-40 samples.

Fig.5 Transmission electron microscopy images of (a) Si/Ti-∞, (b) Si/Ti-10, (c) Si/Ti-20, and (d) Si/Ti-40 samples.

Fig.6 Scheme 1 Schematic representation of pillaring process for synthesis of titanosilicate pillared MFI zeolite nanosheets.

Fig.7 Ultraviolet–visible absorbance spectra of titanosilicate pillared MFI zeolite nanosheets.

Fig.8 Fourier-transform infrared spectra of synthesized titanosilicate zeolites.

Fig.9 XPS profiles of (a) Si/Ti-10, (b) Si/Ti-20, and (c) Si/Ti-40 samples.

Fig.10 Catalytic oxidation of dibenzothiophene over titanosilicate pillared MFI zeolites (a) conversion, (b) selectivity, (c) yield, (d) rate constant of dibenzothiophene oxidation, and (e) rate constant vs. ratio of external surface area to BET surface area (S_ext/S_BET).

Fig.11 Scheme 2 Proposed reaction network for H₂O₂ oxidation of dibenzothiophene over titanosilicate zeolites.

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