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用于改善正癸烷加氢异构化性能的ZSM-22沸石的液相介导Si-OH修复

Liquid-Mediated Si-OH Healing of ZSM-22 Zeolites for Improved Performance in N-Decane Hydroisomerization.

作者信息

Chang Tong, Deng Renhui, Xie Jiaxin, Tang Jianyu, Gu Wenyao, Peng Zimin, Liu Suyao

机构信息

Department of Applied Chemistry, Yuncheng University, Yuncheng 044000, China.

Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province, College of Chemistry and Chemical Engineering, Shantou University, Shantou 515063, China.

出版信息

Molecules. 2025 Aug 8;30(16):3319. doi: 10.3390/molecules30163319.

DOI:10.3390/molecules30163319
PMID:40871472
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12388793/
Abstract

The abundant Si-OH groups serving as the defect sites in the ZSM-22 zeolite framework are not only closely associated with physicochemical properties and catalytic performance but are also the primary sites for attack by water molecules, thereby restricting applications involving or producing water. In the present study, a liquid-mediated healing process was used to convert the Si-OH groups in ZSM-22 zeolite into Si-O-Si bonds. The systematic investigation of the treatment solution's composition and the hydrothermal conditions revealed that the crystallinity of ZSM-22 zeolite can be effectively enhanced following optimal healing treatment. Furthermore, the healed ZSM-22 zeolite exhibited enhanced ordering degree and pore connectivity without significant changes to the Si/Al and morphology. Moreover, the decline in Si-OH groups reduced the Lewis acid sites without altering the Brønsted acidity, which led to a slight decrease in the dispersion of Pt particles. In n-decane hydroisomerization, compared to the parent ZSM-22 zeolite catalyst, the healed catalyst demonstrates higher reactant conversion and increased isomer yield, attributing to its enhanced confinement within the micropore voids, which leads to a reduced yield of multi-branched isomers susceptible to cracking. This study presents a potential application of ZSM-22 zeolite in hydroisomerization for complex and challenging feedstocks.

摘要

作为ZSM - 22沸石骨架中缺陷位点的大量硅羟基,不仅与物理化学性质和催化性能密切相关,而且还是水分子攻击的主要位点,从而限制了涉及水或产生水的应用。在本研究中,采用液介导修复过程将ZSM - 22沸石中的硅羟基转化为硅氧硅键。对处理溶液组成和水热条件的系统研究表明,经过最佳修复处理后,ZSM - 22沸石的结晶度可有效提高。此外,修复后的ZSM - 22沸石有序度和孔连通性增强,而硅铝比和形态没有显著变化。此外,硅羟基的减少降低了路易斯酸位点,而不改变布朗斯特酸度,这导致铂颗粒的分散略有下降。在正癸烷加氢异构化反应中,与母体ZSM - 22沸石催化剂相比,修复后的催化剂表现出更高的反应物转化率和更高的异构体产率,这归因于其在微孔空隙中增强的限域作用,这导致易裂化的多支链异构体产率降低。本研究展示了ZSM - 22沸石在针对复杂且具有挑战性的原料进行加氢异构化方面的潜在应用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/89a5/12388793/2749f88ba8ec/molecules-30-03319-g012.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/89a5/12388793/3d2bdb7aec86/molecules-30-03319-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/89a5/12388793/01f6f4dc8af5/molecules-30-03319-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/89a5/12388793/1b55463c3b42/molecules-30-03319-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/89a5/12388793/cbd816d82c8e/molecules-30-03319-g005.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/89a5/12388793/a3e8daa0ab99/molecules-30-03319-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/89a5/12388793/69c5cb48b7ed/molecules-30-03319-g008.jpg
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本文引用的文献

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