Hierarchical ZSM-5 zeolite with radial mesopores: Preparation, formation mechanism and application for benzene alkylation

doi:10.1007/s11705-019-1853-9

Front. Chem. Sci. Eng.

2020, Vol. 14

Issue (2) : 248-257 https://doi.org/10.1007/s11705-019-1853-9

RESEARCH ARTICLE

Hierarchical ZSM-5 zeolite with radial mesopores: Preparation, formation mechanism and application for benzene alkylation

Darui Wang, Hongmin Sun, Wei Liu, Zhenhao Shen, Weimin Yang(

)

State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Shanghai Research Institute of Petrochemical Technology, Sinopec, Shanghai 201208, China

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Abstract

Hierarchical ZSM-5 zeolite with radial mesopores is controllably synthesized using piperidine in a NaOH solution. The piperidine molecules enter the zeolite micropores and protect the zeolite framework from extensive desilication. The areas containing fewer aluminum atoms contain fewer piperidine protectant molecules and so they dissolve first. Small amounts of mesopores are then gradually generated in areas with more aluminum atoms and more piperidine protectant. In this manner, radial mesopores are formed in the ZSM-5 zeolite with a maximal preservation of the micropores and active sites. The optimal hierarchical ZSM-5 zeolite, prepared with a molar ratio of piperidine to zeolite of 0.03, had a mesopore surface area of 136 m²·g⁻¹ and a solid yield of 80%. The incorporation of the radial mesopores results in micropores that are interconnected which shortened the average diffusion path length. Compared to the parent zeolite, the hierarchical ZSM-5 zeolite possesses more accessible acid sites and has a higher catalytic activity and a longer lifetime for the alkylation of benzene.

Keywords hierarchical ZSM-5 zeolite protective desilication piperidine radial mesopores benzene alkylation

Corresponding Author(s): Weimin Yang

Just Accepted Date: 15 October 2019 Online First Date: 11 December 2019 Issue Date: 24 March 2020

Cite this article:

Darui Wang,Hongmin Sun,Wei Liu, et al. Hierarchical ZSM-5 zeolite with radial mesopores: Preparation, formation mechanism and application for benzene alkylation[J]. Front. Chem. Sci. Eng., 2020, 14(2): 248-257.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-019-1853-9
https://academic.hep.com.cn/fcse/EN/Y2020/V14/I2/248

Fig.1 XRD patterns of (a) PZ, (b) AT, (c) PI 0.02, (d) PI 0.03 and (e) PI 0.04.

Tab.1 The physical properties of the parent and desilicated ZSM-5 zeolites

Fig.2 (A) N₂ isotherms and (B) BJH pore size distributions of (a) PZ, (b) AT, (c) PI 0.02, (d) PI 0.03 and (e) PI 0.04.

Fig.3 SEM images of (a) PZ, (b) AT and (c) PI 0.03.

Fig.4 TEM images of (a) PZ, (b) AT and (c) PI 0.03.

Fig.5 TEM images of PI 0.03 desilicated at different times: (a) 0, (b) 5, (c) 10, (d) 20, (e) 30 and (f) 40 min.

Fig.6 Chemical shift in ¹²⁹Xe MAS NMR spectra of (a) PZ and (b) PI 0.03.

Fig.7 (A) The adsorption isotherms and (B) kinetic curves of diethylbenzene by (a) IGA: PZ and (b) IGA:PI 0.03.

Fig.8 Arrhenius plot illustrating the activity difference between (a) PZ and (b) PI 0.03.

Tab.2 The catalytic performance of PZ and PI 0.03 in benzene alkylation

Fig.9 Change in conversion with time on stream over (a) PZ and (b) PI 0.03.

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