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γ-氧化铝与沸石物理混合及顺序使用在甲醇制丙烯反应中催化性能的对比研究

Comparative study of the catalytic performance of physically mixed and sequentially utilized γ-alumina and zeolite in methanol-to-propylene reactions.

作者信息

Mortazavi-Manesh Anahita, Safari Nasser, Golbodaqi Mojtaba, Latifi Shirin, Fatehi Haghighat Mohammad, Bahadoran Farzad

机构信息

Department of Chemistry, Faculty of Chemistry and Petroleum Science, Shahid Beheshti University, GC, Tehran 1983969411, Iran.

Gas Research Division, Research Institute of Petroleum Industry (RIPI), Tehran 1485733111, Iran.

出版信息

R Soc Open Sci. 2024 Sep 18;11(9):240469. doi: 10.1098/rsos.240469. eCollection 2024 Sep.

DOI:10.1098/rsos.240469
PMID:39295919
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11408930/
Abstract

This study aimed to investigate the catalytic performance of H-ZSM-5 zeolite compared with physically mixed and sequentially used synthesized γ-alumina and zeolite in the methanol-to-propylene (MTP) reaction. A facile, green and cost-effective method was first applied to prepare a mesoporous γ-AlO support using a combination of sol-gel and hydrothermal methods via a few consecutive steps. This process was carried out using aluminium nitrate and polyethylene glycol with different molecular weights as non-ionic surfactants. X-ray diffraction, transmission electon microscopy, thermogravimetric analysis, ammonia temperature programmed desorption and Brunauer-Emmett-Teller analysis were then used to characterize the prepared γ-AlO catalyst. Afterwards, the catalytic activity of the commercial H-ZSM-5 zeolite (Si/Al = 200) and the effect of the presence of the γ-alumina physically mixed and unmixed with the zeolite were also researched in the MTP reaction. Accordingly, methanol conversion and product selectivity were monitored via gas chromatography. The physically mixed mesoporous γ-AlO and H-ZSM-5 zeolite exhibited the highest catalytic activity in terms of both conversion and selectivity at 400°C. To our knowledge, this research represents the first documented use of γ-alumina and zeolite simultaneously as catalysts in the MTP reaction within the English literature. It is hoped that this work will offer valuable insights for advancing the development of catalytic systems in methanol conversion processes.

摘要

本研究旨在研究H-ZSM-5沸石与物理混合及依次使用的合成γ-氧化铝和沸石在甲醇制丙烯(MTP)反应中的催化性能。首先应用一种简便、绿色且经济高效的方法,通过连续几步采用溶胶-凝胶法和水热法相结合来制备介孔γ-AlO载体。该过程使用硝酸铝和不同分子量的聚乙二醇作为非离子表面活性剂。然后使用X射线衍射、透射电子显微镜、热重分析、氨程序升温脱附和布鲁诺尔-埃米特-泰勒分析来表征所制备的γ-AlO催化剂。之后,还研究了商业H-ZSM-5沸石(硅铝比 = 200)的催化活性以及γ-氧化铝与沸石物理混合和未混合时的影响在MTP反应中的情况。相应地,通过气相色谱法监测甲醇转化率和产物选择性。在400°C时,物理混合的介孔γ-AlO和H-ZSM-5沸石在转化率和选择性方面均表现出最高的催化活性。据我们所知,本研究是英文文献中首次记录同时使用γ-氧化铝和沸石作为MTP反应催化剂的情况。希望这项工作将为推进甲醇转化过程中催化体系的发展提供有价值的见解。

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本文引用的文献

1
Temperature-dependent synthesis of dimethyl ether (DME) from methanol over beta zeolite: a novel approach to a sustainable fuel.β沸石上甲醇制二甲醚(DME)的温度依赖性合成:一种可持续燃料的新方法。
R Soc Open Sci. 2023 Aug 23;10(8):230524. doi: 10.1098/rsos.230524. eCollection 2023 Aug.
2
Production of Gamma Alumina Using Plasma-Treated Aluminum and Water Reaction Byproducts.利用等离子体处理的铝与水反应副产物制备γ-氧化铝
Materials (Basel). 2020 Mar 13;13(6):1300. doi: 10.3390/ma13061300.
3
Synthesis and characterization high purity alumina nanorods by a novel and simple method using nanocellulose aerogel template.
通过使用纳米纤维素气凝胶模板的新颖简单方法合成并表征高纯度氧化铝纳米棒。
Heliyon. 2019 Jun 1;5(6):e01816. doi: 10.1016/j.heliyon.2019.e01816. eCollection 2019 Jun.
4
Chemical recycling of carbon dioxide to methanol and dimethyl ether: from greenhouse gas to renewable, environmentally carbon neutral fuels and synthetic hydrocarbons.二氧化碳化学循环转化为甲醇和二甲醚:从温室气体到可再生、环境碳中和燃料及合成烃。
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Low-temperature synthesis of gamma-alumina nanocrystals from aluminum acetylacetonate in nonaqueous media.在非水介质中由乙酰丙酮铝低温合成γ-氧化铝纳米晶体。
Small. 2007 May;3(5):763-7. doi: 10.1002/smll.200700027.
6
An oft-studied reaction that may never have been: direct catalytic conversion of methanol or dimethyl ether to hydrocarbons on the solid acids HZSM-5 or HSAPO-34.一个可能从未发生过的经常被研究的反应:甲醇或二甲醚在固体酸HZSM-5或HSAPO-34上直接催化转化为碳氢化合物。
J Am Chem Soc. 2002 Apr 17;124(15):3844-5. doi: 10.1021/ja016499u.