Integration of Pt/Fe-silicalite-1 and acidic zeolite as a bifunctional catalyst for boosting ethane dehydroaromatization

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL AIChE Journal Pub Date : 2025-01-29 DOI:10.1002/aic.18747

Lizhi Wu, Ying Zhang, Caixin Zou, Qin Sun, Baozhen Li, Wenchun Zheng, Jiamin Liu, Juncheng He, Yu Tang, Li Tan

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Abstract

Ethane dehydrogenation to aromatics (EDA) is one of the most promising routes to produce aromatics. Herein, the tandem of dehydrogenation component and acidic zeolite are prepared and investigated for EDA. Pt/Fe-S-1 coupled with ZSM-5 of Si/Al of 14 via mixing homogeneously shows excellent EDA performance with 54.0% ethane conversion, 61.5% aromatics selectivity as well as a deactivation rate constant of 0.00010 h⁻¹. According to catalysts characterizations and controlled experiments, it is confirmed the highly dispersed positive Pt^δ+ species around Fe species over Pt/Fe-S-1 is the active sites for ethane dehydrogenation to ethylene and subsequent naphthenes dehydrogenation to aromatics, Brønsted acid sites of ZSM-5 and MFI pore are responsible for ethylene oligomerization and cyclization to naphthenes and further naphthenes dehydrogenation to aromatics. The short spatial space between dehydrogenation active sites and acid sites is beneficial for EDA. And the ethylene generation rate is the rate-determining step of EDA.

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乙烷脱氢制芳烃（EDA）是生产芳烃最有前景的途径之一。本文制备并研究了用于 EDA 的脱氢组分和酸性沸石串联物。铂/铁-S-1 与硅/铝含量为 14 的 ZSM-5 通过混合均匀后显示出优异的 EDA 性能，乙烷转化率为 54.0%，芳烃选择性为 61.5%，失活速率常数为 0.00010 h-1。根据催化剂表征和对照实验证实，Pt/Fe-S-1 上铁元素周围高度分散的正铂δ+ 物种是乙烷脱氢成乙烯和环烷脱氢成芳烃的活性位点，ZSM-5 和 MFI 孔的布氏硬度酸位点是乙烯低聚和环化成环烷和环烷脱氢成芳烃的活性位点。脱氢活性位点与酸性位点之间的空间较短，有利于 EDA。乙烯生成速率是 EDA 的决定性步骤。

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.