Physicochemical and Catalytic Properties of the Mo–Zr/ZSM-5 Catalysts of Methane Dehydroaromatization

Zh. B. Budaev; Будаев Ж. Б.; L. L. Korobitsyna; Коробицына Л. Л.; A. A. Stepanov; Степанов А. А.; E. Y. Gerasimov; Герасимов Е. Ю.; A. V. Vosmerikov; Восмериков А. В.

doi:10.31857/S0044453723110055

Physicochemical and Catalytic Properties of the Mo–Zr/ZSM-5 Catalysts of Methane Dehydroaromatization

Authors: Budaev Z.B.¹^,2, Korobitsyna L.L.¹, Stepanov A.A.¹, Gerasimov E.Y.³, Vosmerikov A.V.¹^,2
Affiliations:
1. Institute of Petroleum Chemistry, Siberian Branch, Russian Academy of Sciences
2. Tomsk State University
3. Federal Research Center Boreskov Institute of Catalysis
Issue: Vol 97, No 11 (2023)
Pages: 1584-1593
Section: ХИМИЧЕСКАЯ КИНЕТИКА И КАТАЛИЗ
Submitted: 26.12.2023
Published: 01.11.2023
URL: https://ogarev-online.ru/0044-4537/article/view/233060
DOI: https://doi.org/10.31857/S0044453723110055
EDN: https://elibrary.ru/KSNHRP
ID: 233060

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Abstract

The effect of the method for the introduction of zirconium in the 4Mo/ZSM-5 catalyst and of its amount on the physicochemical and catalytic properties of the catalyst during the nonoxidative conversion of methane into aromatic hydrocarbons (benzene and naphthalene) has been studied. The catalyst was modified with zirconium by impregnation and solid phase mixing. The resulting zeolite catalysts were studied by IR spectroscopy, X-ray diffraction analysis, low-temperature nitrogen adsorption, temperature-programmed ammonia desorption, scanning and transmission electron microscopy, and simultaneous thermal analysis. With an increase in the zirconium concentration introduced in the 4Mo/ZSM-5 catalyst, the strength and concentration of its strong acid sites that are responsible for methane aromatization decrease regardless of the method of modification. The particle size and morphology of the catalyst, the distribution of Mo and Zr in them, and the presence of coke deposits on their surface were determined by scanning and transmission electron microscopy. The catalytic tests and subsequent thermal analysis of the samples showed that the addition of zirconium to the 4Mo/ZSM-5 catalyst leads not only to an increase in its catalytic activity, but also to operational stability due to the lower rate of coke formation. It was established that 4Mo/ZSM-5 modified with 1 wt % Zr by solid-phase synthesis is the most effective catalyst in methane dehydroaromatization (DHA).

Keywords

methane dehydroaromatization, metal zeolite catalysts, ZSM-5 type zeolite, micro-mesoporous structure, acidity, conversion, activity

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