Citation: Ying-Jie LI, Xu-Chang WANG, Jia-Jun ZHENG, Bo QIN, Yan-Ze DU, Rui-Feng LI. Synthesis and Catalytic Performance of Hierarchical Ultrastable Y-Type Zeolite with Ubstantially Increasing Acid Sites[J]. Chinese Journal of Inorganic Chemistry, ;2022, 38(12): 2401-2411. doi: 10.11862/CJIC.2022.230 shu

Synthesis and Catalytic Performance of Hierarchical Ultrastable Y-Type Zeolite with Ubstantially Increasing Acid Sites

Ying-Jie LI ¹ ,
Xu-Chang WANG ¹ ,
Jia-Jun ZHENG ^1,, ,
Bo QIN ² ,
Yan-Ze DU ² ,
Rui-Feng LI ^1,,

1.
College of Chemistry and Chemical Engineering, State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China
2.
Dalian Research Institute of Petroleum & Petrochemicals, SINOPEC, Dalian, Liaoning 116045, China

Corresponding author: Jia-Jun ZHENG, zhengjiajun@tyut.edu.cn Rui-Feng LI, rfli@tyut.edu.cnh
Received Date: 28 May 2022
Revised Date: 13 August 2022

Figures(12)

Ultrastable Y-type (USY) zeolite catalysts with high acid content and high hydrothermal stability (USY-c-w) were obtained by crystallizing an industrial USY-zeolite in a traditional hydrothermal system with the help of a surfactant cetyltrimethylammonium bromide (CTABr). The physicochemical properties of as-synthesized USY-zeolite samples were analyzed by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), solid-state NMR, N₂ adsorption-desorption, ammonia temperature programmed desorption (NH₃-TPD), FT-IR, and pyridine infrared spectroscopy (Py-IR). Catalytic cracking of 1, 3, 5-triisopropylbenzene (TIPB) was selected as a probe reaction to investigate the catalytic performance of as-synthesized catalysts and compare it with that of the industrial USY-zeolite. The results exhibited that after hydrothermal re-crystallization, the framework of USY-zeolite suffered from a partial reformation. Desilicication by steam or alkali treatment results in the formation of a large number of silanol nests, which reacts with Al species resulting from the non-framework aluminum in the USY-zeolite and then promotes the formation of the"new"framework Al. This offers as-synthesized sample with a less Si/Al ratio (n_Si/n_Al) and with increasing acid sites. The increased Al content in the zeolite framework was confirmed by the results of XRD, FTIR, X-ray energy dispersive spectrum (EDS), and NMR. For example, the framework Si/Al ratio decreased from 10 (industrial USY-zeolite) to 3.0 (USY-045-07C). The NH₃-TPD experiment and Py-IR provided direct evidence supporting the increased acidity in as-synthesized catalysts. Moreover, the results obtained by the N₂ adsorption-desorption experiment, SEM, and TEM also showed that abundant mesopores were also introduced into as-synthesized samples with more weak acid sites along with more medium-strong acid ones. During the catalytic cracking of TIPB, as-synthesized USY-c-w showed more excellent catalytic performance with higher conversion of TIPB than the reference sample.
- ultrastable Y-type zeolite,
- cetyltrimethylammonium bromide,
- hydrothermal crystallization,
- hydrothermal stability
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