Constructing hierarchical ZSM-5 coated with small ZSM-5 crystals via oriented-attachment and <i>in situ</i> assembly for methanol-to-aromatics reaction

doi:10.1007/s11705-024-2432-2

2024, Vol. 18

Issue (7) : 76 https://doi.org/10.1007/s11705-024-2432-2

Constructing hierarchical ZSM-5 coated with small ZSM-5 crystals via oriented-attachment and in situ assembly for methanol-to-aromatics reaction

Ning Yang, Tingjun Fu(

), Chuntao Cao, Xueqing Wu, Huiling Zheng, Zhong Li

State Key Laboratory of Clean and Efficient Coal Utilization, College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, China

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Abstract

Developing hierarchical and nanoscale ZSM-5 catalysts for diffusion-limited reactions has received ever-increasing attention. Here, ZSM-5 architecture integrated with hierarchical pores and nanoscale crystals was successfully prepared via in situ self-assembly of nanoparticles-coated silicalite-1. First, the oriented attachment of amorphous nanoparticles on external surface of silicalite-1 was achieved by controlling the alkalinity of Si-Al coating solution. The partial exposure of the external surface of silicalite-1 ensured the uniform removal of silicon in the bulk phase for the creation of hierarchical pores during the subsequent desilication-recrystallization. The uniform removal of silicon species in the bulk phase was mainly due to the synergistic effect of surface protection and alkaline etching, which could be balanced by regulating the relative amount of tetrapropylammonium cation and OH^– in desilication-recrystallization solution. Importantly, the removed silicon from silicalite-1 recrystallized and in situ assembled into final ZSM-5 nanocrystals induced by surface Si-Al nanoparticles. The hierarchical pores and nanoscale crystals on this integrated architecture not only promoted the removal of coke precursors from micropores but also provided large external specific surface (91 m²·g^–1) for coke deposition. Consequently, a much longer catalytic lifetime was achieved for methanol-to-aromatics reaction compared to conventional hollow structure ZSM-5 (84 h vs 46 h), with relatively high stability.

Keywords hierarchical ZSM-5 nanocrystal integrated architecture diffusion coke

Corresponding Author(s): Tingjun Fu

Just Accepted Date: 28 February 2024 Issue Date: 27 May 2024

Cite this article:

Ning Yang,Tingjun Fu,Chuntao Cao, et al. Constructing hierarchical ZSM-5 coated with small ZSM-5 crystals via oriented-attachment and in situ assembly for methanol-to-aromatics reaction[J]. Front. Chem. Sci. Eng., 2024, 18(7): 76.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2432-2
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I7/76

Fig.1 Schematic diagram of the synthetic route of (a) HIZ@NZ5 and (e) HOZ5; TEM images: (b, h) S-1; (c1) S-1@NZ5; (d1) HIZ@NZ5; (f1) HOZ5; (g1) S-1@Z5; SEM images: (c2) S-1@NZ5; (d2) HIZ@NZ5; (f2) HOZ5; (g2) S-1@Z5.

Fig.2 (a) XRD patterns; (b) relative crystallinity; (c) N₂ adsorption-desorption isotherms; and (d) pore size distribution of S-1@NZ5, HIZ@NZ5, S-1@Z5 and HOZ5.

Tab.1 Textural properties of S-1@NZ5, HIZ@NZ5, S-1@Z5 and HOZ5

Fig.3 TEM images of the parent and subsequent desilication-recrystallization samples showing the influence of alkalinity of growth solution on S-1 seed secondary growth.

Tab.2 Textural properties of the samples obtained under different desilication-recrystallization conditions

Fig.4 TEM images of the samples obtained by desilication-recrystallization under different treatments using S-1@NZ5 as the parent, which was obtained from the growth solution with pH = 10.

Fig.5 TEM images of HIZ@NZ5 at different crystallization stages: (a) before crystallization; (b) 1 h; (c) 5 h; (d) 24 h.

Fig.6 Formation mechanism of hierarchical structure coated with small ZSM-5 crystals and hollow structure ZSM-5.

Fig.7 TEM images of the final integrated ZSM-5 architecture obtained with different SiO₂/Al₂O₃ ratios of S-1 growth solution.

Fig.8 (a) Methanol conversion; (b) liquid hydrocarbon yield; (c) selectivity of benzene (B), ethylbenzene (EB), toluene (T), xylene (X), trimethylbenzene (TMB) and C_9+A in aromatics; (d) aromatic distribution; (e) NH₃-TPD profiles and (f) Py-IR spectra for HIZ@NZ5 with different SiO₂/Al₂O₃ ratios and HOZ5.

Fig.9 (a) TG curves; (c) coke formation rate; (c) relationship between external specific surface area and lifetime; (d) GC-MS signals of soluble coke species in spent catalysts after reaction for 5 h.

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