Influence of Channel, Construction and Brønsted Acid Sites on the Catalytic Conversion Pathways of Isobutane Over MFI, TON and RFE Zeolites

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL Catalysis Letters Pub Date : 2024-11-13 DOI:10.1007/s10562-024-04847-z

Yibin Hou, Rongxin Zhang, Zijian Wang, Bin Lu, Jieguang Wang

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Abstract

Despite thorough exploration of the acidity properties and pore structure effects of zeolite catalysts on catalytic conversion, a comprehensive understanding of how these factors influence reaction pathways is still lacking. Herein, three common zeolites (ZSM-5, ZSM-22 and ZSM-48) of different shapes and size dimensions were introduced into catalytic conversion of isobutane, with combination of X-ray diffraction (XRD), transmission electron microscopy (TEM), N₂ adsorption and desorption, solid-state ²⁹Si and ²⁷Al MAS NMR, ammonia temperature programmed desorption (NH₃-TPD) and pyridine adsorption infrared spectroscopy (Py-FTIR) to characterize their structure and acidity. And channels and topologies were associated with stability and catalytic activity. ZSM-5 performed best, showing the most active sites. Furthermore, ZSM-48 led to an increase in the propene yield by suppressing inhibitory secondary reactions in the monomolecular reaction pathway. Moreover, the amount of Brønsted acid sites (BASs) of ZSM-22 were a key factor in promoting light alkene formation. However, 1D channels contributed to the deactivation of ZSM-22 and ZSM-48. The detailed reaction pathways of zeolite catalysts with diverse pore structures and acidities are crucial for optimizing their catalytic performance.

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MFI、TON 和 RFE 沸石上异丁烷催化转化途径的通道、结构和布氏酸位点的影响

尽管对沸石催化剂的酸性和孔结构对催化转化的影响进行了深入探讨，但仍缺乏对这些因素如何影响反应途径的全面了解。本文将三种不同形状和尺寸的常见沸石（ZSM-5、ZSM-22 和 ZSM-48）引入异丁烷的催化转化中，结合 X 射线衍射（XRD）、透射电子显微镜（TEM）、N2 吸附和脱附、固体电子显微镜（TEM）、X 射线衍射（XRD）和透射电子显微镜（TEM）等技术，研究了沸石催化剂对异丁烷催化转化的影响、N2吸附和解吸、固态 29Si 和 27Al MAS NMR、氨温程控解吸（NH3-TPD）和吡啶吸附红外光谱（Py-FTIR）来表征其结构和酸性。通道和拓扑结构与稳定性和催化活性有关。ZSM-5 表现最好，显示出最多的活性位点。此外，ZSM-48 通过抑制单分子反应途径中的抑制性二级反应，提高了丙烯产量。此外，ZSM-22 的布氏酸位点（BAS）数量是促进轻烯形成的关键因素。然而，1D 通道导致 ZSM-22 和 ZSM-48 失活。具有不同孔结构和酸度的沸石催化剂的详细反应途径对于优化其催化性能至关重要。

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.