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超临界CO与HZSM-5催化的甲醛-异丁烯普林斯反应合成3-甲基-3-丁烯-1-醇

Synthesis of 3-methyl-3-buten-1-ol by supercritical CO in coordination with HZSM-5-catalyzed formaldehyde-isobutene Prins reaction.

作者信息

Yuan Hang, Cao Gui-Ping, Lv Hui

机构信息

Department of Chemical Engineering and Technology, School of Chemical Engineering, East China University of Science and Technology, Shanghai, P.R. China.

出版信息

Turk J Chem. 2024 Jun 26;48(4):597-619. doi: 10.55730/1300-0527.3682. eCollection 2024.

Abstract

The reaction solvent and catalyst play essential roles in the Prins reaction for the synthesis of 3-methyl-3-buten-1-ol (MBO) from formaldehyde and isobutene. The reactivity of the solid base-catalyzed Prins condensation reaction by formaldehyde and isobutene in supercritical CO was investigated using CsHPO-modified HZSM-5. We found that the alkaline sites of the alkali-loaded catalyst could extract the α-H on isobutene to generate olefin carbon-negative ions, while the supercritical CO with weak Lewis acidity could activate formaldehyde to carbon-positive ions, which can combine more easily with carbon-negative isobutene to react, thus improving the reactivity of the reaction system.

摘要

反应溶剂和催化剂在由甲醛和异丁烯合成3-甲基-3-丁烯-1-醇(MBO)的普林斯反应中起着至关重要的作用。使用CsHPO改性的HZSM-5研究了在超临界CO₂中固体碱催化的甲醛与异丁烯的普林斯缩合反应的反应活性。我们发现,负载碱的催化剂的碱性位点可以提取异丁烯上的α-H以生成烯烃碳负离子,而具有弱路易斯酸性的超临界CO₂可以将甲醛活化为碳正离子,其可以更容易地与碳负性的异丁烯结合反应,从而提高反应体系的反应活性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f1ce/11407352/26a1e758a254/tjc-48-04-597f1.jpg

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