NDLI: Catalytic conversion of methanol to aromatics over nano-sized HZSM-5 zeolite modified by ZnSiF<sub>6</sub>·6H<sub>2</sub>O

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Catalytic conversion of methanol to aromatics over nano-sized HZSM-5 zeolite modified by ZnSiF₆·6H₂O

Content Provider	Royal Society of Chemistry (RSC)
Author	Jia, Yanming Wang, Junwen Ding, Chuanmin Zhang, Kan Chen, Guoliang Yang, Yufei Liu, Shibin Liu, Ping
Copyright Year	2017
Abstract	ZnSiF6-modified nano-sized HZSM-5 zeolites (NZ2, NZ3 and NZ4 catalysts) were prepared and investigated as catalysts for the conversion of methanol to aromatics. Moreover, the ZnNZ1 catalyst, prepared by ion exchange using zinc nitrate, was also introduced as a reference sample. The effects of modification on the framework, textural properties and acidity of the parent nano-sized HZSM-5 zeolite (NZ1) were investigated by XRD, FT-IR, 29Si MAS-NMR, SEM, N2 adsorption–desorption, ICP, NH3-TPD, infrared spectroscopy of adsorbed pyridine (Py-IR), UV-vis spectra, X-ray photoelectron spectroscopy (XPS) and n-butylamine and tert-butylamine titration. The results showed that the amount of total acid sites, especially the external surface acid sites of the NZ2, NZ3 and NZ4 catalysts, significantly decreased, which may largely be attributed to the passivation effect of SiF62− on the surface acidity of the parent NZ1 catalyst. Moreover, the amount of Lewis acid sites (L acid sites) increased, whereas the amount of Brønsted acid sites (B acid sites) obviously decreased with the introduction of zinc species. The emergence of new Zn-Lewis acid sites (⊖ZO⋯H⋯O–Zn⊕ species) was beneficial to improving the selectivity to BTX (benzene (B), toluene (T) and xylene (X)) due to their high activity for dehydroaromatization. The FT-IR spectra in the OH− vibration region and the 29Si MAS-NMR spectra show that the treatment of ZnSiF6 could effectively repair partial lattice defects of zeolite and could thus improve the catalyst stability. TG analysis of all the deactivated catalysts showed that the coke amount and the average rate of coke formation decreased over NZ2, NZ3 and NZ4 catalysts, and this may largely be ascribed to their lower surface acidity. The catalytic performance of these materials on the conversion of methanol to aromatics showed that the NZ3 catalyst had the highest selectivity to BTX of about 51.3% and the longest catalytic lifetime of about 234 h under the operating conditions of T = 425 °C, p = 0.1 MPa and WHSV = 0.8 h−1. The improvement in the selectivity to BTX and the catalyst lifetime of the NZ3 catalyst could be ascribed to the synergistic effect among the Zn-Lewis acid sites (⊖ZO⋯H⋯O–Zn⊕ species), external surface acidity and intact framework structure.
Starting Page	1776
Ending Page	1791
Page Count	16
File Format	HTM / HTML PDF
ISSN	20444753
Volume Number	7
Issue Number	8
Journal	Catalysis Science & Technology
DOI	10.1039/c7cy00143f
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Infrared spectroscopy Acid Zinc nitrate Tert-Butylamine Fourier-transform infrared spectroscopy X-ray crystallography Bildschirmtext Xylene WHSV X-ray photoelectron spectroscopy Methanol Crystal structure N-Butylamine Toluene Ion Zeolite Photoemission spectroscopy Zinc Ammonia Pyridine Lewis Benzene ICP Titration Passivation (chemistry)
Content Type	Text
Resource Type	Article
Subject	Catalysis

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