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用于CO/环氧丙烷环加成反应的具有双路易斯酸碱位点的胺改性Zr-Mg混合氧化物气凝胶纳米结构设计

Design of Amine-Modified Zr-Mg Mixed Oxide Aerogel Nanoarchitectonics with Dual Lewis Acidic and Basic Sites for CO/Propylene Oxide Cycloaddition Reactions.

作者信息

Lin Yi-Feng, Lai Yu-Rou, Sung Hsiang-Ling, Chung Tsair-Wang, Lin Kun-Yi Andrew

机构信息

Department of Chemical Engineering and Research Center for Circular Economy, Chung Yuan Christian University, Chungli District, Taoyuan 32023, Taiwan.

R&D Center for Membrane Technology, Chung Yuan Christian University, Chungli District, Taoyuan 32023, Taiwan.

出版信息

Nanomaterials (Basel). 2022 Oct 1;12(19):3442. doi: 10.3390/nano12193442.

DOI:10.3390/nano12193442
PMID:36234572
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9565247/
Abstract

The utilization of CO attracts much research attention because of global warming. The CO/epoxide cycloaddition reaction is one technique of CO utilization. However, homogeneous catalysts with both Lewis acidic and basic and toxic solvents, such as DMF, are needed in the CO/epoxide cycloaddition reaction. As a result, this study focuses on the development of heterogeneous catalysts with both Lewis acidic and basic sites for the CO utilization of the CO/epoxide cycloaddition reactions without the addition of a DMF toxic solvent. For the first time, the Zr-Mg mixed oxide aerogels with Lewis acidic and basic sites are synthesized for the CO/propylene oxide (PO) cycloaddition reactions. To further increase the basic sites, 3-Aminopropyl trimethoxysilane (APTMS) with -NH functional group is successfully grafted on the Zr-Mg mixed oxide aerogels. The results indicate that the highest yield of propylene carbonate (PC) is 93.1% using the as-developed APTMS-modified Zr-Mg mixed oxide aerogels. The as-prepared APTMS-modified Zr-Mg mixed oxide aerogels are great potential in industrial plants for CO reduction in the future.

摘要

由于全球变暖，一氧化碳的利用引起了众多研究关注。一氧化碳/环氧化物环加成反应是一氧化碳利用的一种技术。然而，在一氧化碳/环氧化物环加成反应中需要同时具有路易斯酸性和碱性且含有有毒溶剂（如N,N-二甲基甲酰胺）的均相催化剂。因此，本研究聚焦于开发具有路易斯酸性和碱性位点的多相催化剂，用于在不添加N,N-二甲基甲酰胺有毒溶剂的情况下进行一氧化碳/环氧化物环加成反应的一氧化碳利用。首次合成了具有路易斯酸性和碱性位点的锆-镁混合氧化物气凝胶用于一氧化碳/环氧丙烷（PO）环加成反应。为了进一步增加碱性位点，成功地将具有-NH官能团的3-氨丙基三甲氧基硅烷（APTMS）接枝到锆-镁混合氧化物气凝胶上。结果表明使用所开发的APTMS改性锆-镁混合氧化物气凝胶，碳酸丙烯酯（PC）的最高产率为93.1%。所制备的APTMS改性锆-镁混合氧化物气凝胶在未来工业装置中减少一氧化碳排放方面具有巨大潜力。

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