Control of aluminum distribution in ZSM-5 zeolite for enhancement of its catalytic performance for propane aromatization

doi:10.1007/s11705-024-2439-8

2024, Vol. 18

Issue (8) : 86 https://doi.org/10.1007/s11705-024-2439-8

Control of aluminum distribution in ZSM-5 zeolite for enhancement of its catalytic performance for propane aromatization

Zhao Ma^1,², Dezhi Shi^1,², Sen Wang¹(

), Mei Dong¹(

), Weibin Fan¹(

)

¹. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
². University of Chinese Academy of Sciences, Beijing 100049, China

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Abstract

Regulation of aluminum distribution in zeolite framework is an effective method for improving its catalytic performance for propane aromatization. Herein, we found that recrystallization and post-realuminization of ZSM-5 cannot only create hollow structures to enhance the diffusion ability, but also adjust the content and position of paired aluminum species in its framework. Various characterizations results confirmed that increase of paired aluminum content and inducement of more aluminum atoms sited in the intersection cavity are beneficial to the formation of aromatic products in propane aromatization. As a result, the hollow-structured ZSM-5 zeolite with more paired aluminum (H-200-hollow) showed higher propane conversion and aromatics selectivity than other samples at the same conditions. The catalytic performance of H-200-hollow can be further improved by ion-exchanging with a small amount of Ga(III) species. The propane conversion and aromatics selectivity of Ga-200-hollow reached as high as 95% and 70%, respectively, at 540 °C and 1 atm.

Keywords propane aromatization zeolite aluminum distribution recrystallization and post-realuminization

Corresponding Author(s): Sen Wang,Mei Dong,Weibin Fan

Just Accepted Date: 19 April 2024 Issue Date: 17 June 2024

Cite this article:

Zhao Ma,Dezhi Shi,Sen Wang, et al. Control of aluminum distribution in ZSM-5 zeolite for enhancement of its catalytic performance for propane aromatization[J]. Front. Chem. Sci. Eng., 2024, 18(8): 86.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2439-8
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I8/86

Fig.1 (a) XRD patterns and (b) N₂ sorption isotherms of H-40-hol, H-100-hol, H-200-hol, and H-300-hol catalysts.

Fig.2 TEM images of (a) H-40-hol, (b) H-100-hol, (c) H-300-hol, and (d) H-200-hol; (e–i) STEM-EDX elemental mappings of Si, Al, O elements of H-200-hol obtained by line scanning and face scanning.

Tab.1 Elemental compositions and textual properties of H-40-hol, H-100-hol, H-200-hol, and H-300-hol

Tab.2 Acidic properties of H-40-hol, H-100-hol, H-200-hol, and H-300-hol

Fig.3 (a) NH₃-TPD profiles and (b) Py-IR spectra of H-40-hol, H-100-hol, H-200-hol, and H-300-hol.

Tab.3 Distributions of Al atoms in the frameworks of H-40-hol, H-100-hol, H-200-hol, and H-300-hol

Fig.4 (a, b) Dependences of C₃H₈ conversion and aromatics selectivity on the time-on-stream over H-40-hol, H-100-hol, H-200-hol, and H-300-hol; (c) relationship between aromatics yield and Al_pairs content; (d) the product distribution of H-200-hol with the time-on-stream.

Fig.5 In situ DR UV-Vis spectra for propane aromatization over (a) H-40-hol and (b) H-200-hol at 300 °C.

Fig.6 (a) Catalytic results of Ga-200-hol in propane aromatization at 540 °C, 1 atm and WHSV of 0.8 h^?1; (b) XRD pattern of Ga-200-hol; (c) N₂ sorption isotherm of Ga-200-hol; (d) SEM image of Ga-200-hol; (e) TEM image of Ga-200-hol; (f–l) STEM and EDX elemental mappings of Ga-200-hol.

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