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负载在离子液体修饰的分级八面沸石上的杂多酸作为甘油缩醛化制丙酮缩甘油的高效催化剂。

Heteropolyacid supported on ionic liquid decorated hierarchical faujasite zeolite as an efficient catalyst for glycerol acetalization to solketal.

作者信息

Sadjadi Samahe, Tarighi Sara, Delangiz Motahareh, Heravi Majid

机构信息

Gas Conversion Department, Faculty of Petrochemicals, Iran Polymer and Petrochemical Institute, P.O. Box 14975-112, Tehran, Iran.

Department of Chemistry, School of Physic and Chemistry, Alzahra University, P.O. Box 1993891176, Vanak, Tehran, Iran.

出版信息

Sci Rep. 2023 Sep 21;13(1):15703. doi: 10.1038/s41598-023-42956-8.

Abstract

To handle huge amount of glycerol produced in biodiesel industry, glycerol is transformed to value-added products. In this regard, glycerol acetalization to solketal is industrially attractive. As in this process various by-products can be formed, designing highly selective catalysts is of great importance. In this line, we wish to report a novel catalyst that benefits from strong acidity, high specific surface area and thermal stability, which can selectively form solketal in glycerol acetalization. To prepare the catalyst, hierarchical zeolite was prepared via a novel method, in which partially dealuminated NaY was treated with PluronicF-127 and then reacted with NHNO to furnish the H-form zeolite. Hierarchical faujasite was then achieved through calcination and template removal. Subsequently, it was functionalized with ionic liquid and used for the immobilization of heteropolyacid. The results indicated the importance of the mesoprosity of zeolite and the presense of ionic liquid functionality for achiveing high solketal yield. Moreover, among three investigated heteropolyacids, phosphomolybdic acid exhibited the highest catalytic activity. In fact, using 10 wt% catalyst at 55 °C and glycerol to acetone molar ratio of 1:20, solketal with yield of 98% was furnished under solvent-less condition. Besides, the catalyst was recyclable with low leaching of heteropolyacid.

摘要

为了处理生物柴油工业中产生的大量甘油,甘油被转化为高附加值产品。在这方面,甘油缩醛化生成丙酮缩甘油在工业上具有吸引力。由于在这个过程中会形成各种副产物,设计高选择性催化剂非常重要。在这方面,我们希望报道一种新型催化剂,它具有强酸性、高比表面积和热稳定性,能够在甘油缩醛化反应中选择性地生成丙酮缩甘油。为了制备该催化剂,通过一种新方法制备了分级沸石,其中用普朗尼克F-127处理部分脱铝的NaY,然后与NHNO反应得到H型沸石。然后通过煅烧和去除模板得到分级八面沸石。随后,用离子液体对其进行功能化,并用于固定杂多酸。结果表明,沸石的介孔性和离子液体功能对于获得高丙酮缩甘油产率很重要。此外,在所研究的三种杂多酸中,磷钼酸表现出最高的催化活性。实际上,在55℃、甘油与丙酮摩尔比为1:20的无溶剂条件下,使用10 wt%的催化剂,丙酮缩甘油的产率达到了98%。此外,该催化剂可循环使用,杂多酸的浸出率较低。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ecca/10514292/9826e6709917/41598_2023_42956_Fig1_HTML.jpg

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