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Ag NPs 负载在 COF 上,在 DBU 的存在下作为高效催化体系,在大气压下通过 CO 固定到炔丙胺中合成四氢酸。

Ag NPs decorated on a COF in the presence of DBU as an efficient catalytic system for the synthesis of tetramic acids via CO fixation into propargylic amines at atmospheric pressure.

机构信息

Department of Chemistry, University of Kalyani, Kalyani, Nadia, 741235, W.B., India.

出版信息

Dalton Trans. 2019 Apr 2;48(14):4657-4666. doi: 10.1039/c9dt00017h.

DOI:10.1039/c9dt00017h
PMID:30893416
Abstract

CO2 fixation reactions by inserting it in reactive organic compounds are very challenging for the utilization of this abundant and harmful gas present in air and thus to mitigate this greenhouse gas responsible for global warming. This can be achieved by appropriate design of functionalized porous nanocatalysts having high surface areas and porosity and good CO2 uptake capacity. Herein, we first report the decoration of silver nanoparticles (NPs) over the surface of a covalent organic framework (COF) material TpPa-1 synthesized through the polycondensation of 2,4,6-triformylphloroglucinol (TFP) and p-phenylenediamine. The resulting material Ag@TpPa-1 was thoroughly characterized by N2 adsorption/desorption, powder X-ray diffraction (PXRD), FE-SEM, TEM, UV-Vis, FT IR and thermogravimetric techniques. This Ag NP decorated porous COF in the presence of DBU exhibited excellent catalytic activity for the synthesis of tetramic acids from a variety of propargylic amine derivatives at 60 °C under atmospheric pressure of carbon dioxide via formation of oxazolidinones, where CO2 acts as a C1 reagent. The Ag@TpPa-1 catalyst exhibited excellent recycling efficiency for the synthesis of tetramic acid with no leaching of Ag from the catalyst surface.

摘要

通过将其插入反应性有机化合物中来固定 CO2 反应,对于利用空气中丰富且有害的这种气体非常具有挑战性,从而减轻这种导致全球变暖的温室气体。这可以通过设计具有高表面积和孔隙率以及良好 CO2 吸收能力的功能化多孔纳米催化剂来实现。在此,我们首次报道了通过 2,4,6-三(三氟甲基)苯甲醛(TFP)和对苯二胺的缩聚反应合成的共价有机骨架(COF)材料 TpPa-1 表面上银纳米颗粒(NPs)的修饰。所得材料 Ag@TpPa-1 通过 N2 吸附/解吸、粉末 X 射线衍射(PXRD)、FE-SEM、TEM、UV-Vis、FTIR 和热重技术进行了彻底的表征。在 DBU 的存在下,Ag NP 修饰的多孔 COF 在 60°C 下、在大气压力下的二氧化碳存在下,通过形成恶唑烷酮,将二氧化碳作为 C1 试剂,从各种炔丙基胺衍生物中高效合成四氢酸。Ag@TpPa-1 催化剂在合成四氢酸时表现出优异的循环效率,没有 Ag 从催化剂表面浸出。

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