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Encapsulation of Silver Nanoparticles in an Amine‐Functionalized Porphyrin Metal–Organic Framework and Its Use as a Heterogeneous Catalyst for CO2 Fixation under Atmospheric Pressure
Chemistry - An Asian Journal ( IF 4.1 ) Pub Date : 2018-07-30 , DOI: 10.1002/asia.201800815
Gargi Dutta 1 , Ajay Kumar Jana 1 , Dheeraj Kumar Singh 2 , M. Eswaramoorthy 2 , Srinivasan Natarajan 1
Affiliation  

A new porphyrin‐based compound, [Zn3(C40H24N8)(C20H8N2O4)2(DEF)2](DEF)3 (1; DEF=N,N‐diethylformamide), has been synthesized by employing 5,10,15,20‐tetrakis(4‐pyridyl)porphyrin, 1,2‐diamino‐3,6‐bis(4‐carboxyphenyl)benzene, and Zn2+ salt at 100 °C under solvothermal conditions. The structure, as determined by single‐crystal XRD studies, is three‐dimensional with threefold interpenetration. The usefulness of free −NH2 groups in the ligand was exploited for anchoring silver nanoparticles through a simple solution‐based route. The silver‐loaded sample, Ag@1, was characterized by powder XRD, energy‐dispersive X‐ray spectroscopy, high‐resolution TEM, SEM, X‐ray photoelectron spectroscopy, and inductively coupled plasma MS analysis, which clearly indicated that silver nanoparticles with a size of 3.83 nm were uniformly distributed within the metal–organic framework (MOF). The Ag@1 sample was evaluated for possible catalytic activity for the carboxylation of a terminal alkyne by employing CO2 under atmospheric pressure; this gave excellent results. The Ag@1 catalyst was found to be robust, active, and recyclable. The present studies suggest that porphyrin MOFs not only exhibit interesting structures, but also show good heterogeneous catalytic activity towards the fixation of CO2.

中文翻译:

氨基官能化卟啉金属-有机骨架中银纳米粒子的包封及其在常压下用作固定CO2的非均相催化剂的用途

一种新的基于卟啉的化合物[Zn 3(C 40 H 24 N 8)(C 20 H 8 N 2 O 42(DEF)2 ](DEF)31 ; DEF = NN-二乙基甲酰胺),通过在溶剂热下于100°C下使用5,10,15,20-四(4-吡啶基)卟啉,1,2-二氨基-3,6-双(4-羧基苯基)苯和Zn 2+盐合成条件。通过单晶XRD研究确定的结构是具有三重互穿的三维结构。游离-NH 2的有用性配体中的基团被用于通过简单的基于溶液的途径锚定银纳米颗粒。载银样品Ag @ 1的特征在于粉末XRD,能量色散X射线光谱,高分辨率TEM,SEM,X射线光电子能谱和电感耦合等离子体MS分析,清楚地表明了银纳米颗粒尺寸为3.83 nm的金属均匀分布在金属有机框架(MOF)中。通过在大气压下使用CO 2来评估Ag 1样品对于末端炔烃羧化的可能催化活性。这给出了极好的结果。Ag @ 1发现该催化剂坚固,活性和可回收。目前的研究表明,卟啉MOFs不仅表现出令人感兴趣的结构,而且还表现出对固定CO 2的良好的多相催化活性。
更新日期:2018-07-30
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