Abstract

Mesoporous HZSM-5 prepared by alkaline treatment (also termed desilication) has drawn significant attention due to its potential in large-scale production and in versatile applications, such as separation and catalysis. Alkali-treated HZSM-5 contains considerable amounts of non-framework (amorphous) Lewis acidic Al species on the external surface, and is deemed to be essential in affecting its catalytic performances. This study intends to clarify the catalytic nature of amorphous Al species of alkali-treated HZSM-5 in methanol aromatization. Physicochemical characterizations, including N2 adsorption, scanning electron microscopy (SEM), X-ray diffraction (XRD), magic-angle-spinning nuclear magnetic resonance (MAS NMR), inductively coupled plasma (ICP) analysis, NH3 temperature-programmed desorption (TPD), and methanol-TPD, were performed. The outcomes showed that non-framework Al promotes the hydride transfer in mesoporous HZSM-5, thereby facilitating the aromatization reaction. Among aromatic products, durene can be promoted by non-framework Al through methylation/transalkylation of other aromatics, particularly xylenes, instead of being promoted by reduced space confinement in mesoporous HZSM-5.

Highlights

  • Designing and utilizing hierarchically-structured HZSM-5 zeolites is burgeoning.According to the Web of Science database using “hierarchical”, “HZSM-5”, and “zeolites” as keywords, the number of relevant papers published per year increased approximately threefold from 2012(40 papers) to 2016 (121 papers)

  • The success of the applications of multilevel porous HZSM-5 is mainly caused by the auxiliary mesoporosity, which can enhance the accessibility of the inner space in micropores [2]

  • This study aims to explore the influences of non-framework Lewis acidic Al species of alkali-treated HZSM-5 in methanol to aromatics (MTA)

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Summary

Introduction

Designing and utilizing hierarchically-structured (or mesoporous) HZSM-5 zeolites is burgeoning. This increase can be attributed to the great potential of hybrid meso-/microporous HZSM-5 in industrial applications, such as separation/adsorption, ion exchange, and heterogeneous catalysis [1]. The destructive method using alkaline treatment (desilication) is more applicable, reliable, and cost-effective (e.g., this method does not use any expensive template as the bottom-up method does [10]) in large-scale production. Pilot-scale production (35 kg per batch in a 1.5 m3 reactor) of desilicated HZSM-5 catalysts in practicable granular forms has been successfully demonstrated by Pérez-Ramírez and his coworkers [8,12]

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