Dealumination and desilication for Al-rich HZSM-5 zeolite via steam-alkaline treatment and its application in methanol aromatization

Abstract

The hierarchical HZSM-5 was prepared via dealumination and desilication of commercial Al-rich HZSM-5, and characterized by X-ray diffraction, ²⁷Al magic-angle spinning nuclear magnetic resonance, inductively coupled plasma mass spectrometry, scanning electron microscope, transmission electron microscope, N₂ adsorption-desorption, NH₃ temperature-programmed desorption, performed thermogravimetric and Raman spectrum. The results showed that partial framework of HZSM-5 was removed after steam treatment at 0.15 MPa, 500°C for 3 h. HZSM-5 with high specific surface area and much mesoporosity was obtained by the subsequent alkaline treatment. The regulation of acid quantity was achieved by altering the concentration of alkaline. Dealumination and desilication of Al-rich HZSM-5 zeolites became more effective using a combination of steam and alkaline treatments than using alkaline treatment alone. Methanol aromatization reaction was employed to evaluate the catalytic performance of treated HZSM-5 at 0.15 MPa, 450°C and MHSV of 1.5 h⁻¹. The results indicated that after steam treatment, HZSM-5 further treated with 0.2 mol/L NaOH exhibits the best catalytic performance: the selectivity of aromatics reached 42.1% and the lifetime of catalyst attained 212 h, which are much better than untreated HZSM-5.

Graphical abstract

Keywords

steam treatment / alkaline treatment / hierarchical ZSM-5 / methanol aromatization

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Acknowledgements

The funding from the National Natural Science Foundation of China (Grant No. 21776076) and Technology admin. of Department of PetroChina Company Limited are gratefully acknowledged.

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