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钯纳米颗粒修饰的后合成改性Zr-UiO-66金属有机框架作为C-C偶联反应中可重复使用的多相催化剂的稳定性

Stabilization of Palladium-Nanoparticle-Decorated Postsynthesis-Modified Zr-UiO-66 MOF as a Reusable Heterogeneous Catalyst in C-C Coupling Reaction.

作者信息

Mohammadi Leila, Hosseinifard Mojtaba, Vaezi Mohammad Reza

机构信息

Department of Nano Technology and Advanced Materials, Materials and Energy Research Center, Karaj, Iran.

Department of Energy, Materials and Energy Research Center, Karaj, Iran.

出版信息

ACS Omega. 2023 Feb 24;8(9):8505-8518. doi: 10.1021/acsomega.2c07661. eCollection 2023 Mar 7.

Abstract

Here we prepared a highly efficient and reusable catalyst by a step-by-step postsynthesis modification of UiO-66-NH metal-organic frameworks (MOFs) with nitrogen-rich organic ligands and used it as support for the preparation of UiO-66-NH@cyanuric chloride@2-aminopyrimidine/Pd. The catalytic performance's results of UiO-66-NH@cyanuric chloride@2-aminopyrimidine/PdNPs, UiO-66-NH/PdNPs, and UiO-66-NH@cyanuric chloride/PdNPs indicate high efficiency of the modulation of the microenvironment of the palladium NPs. The addition of N-rich organic ligands through postsynthesis modification caused a unique structure of the final composite in favor of the progress of the C-C coupling reaction. Various techniques, including FT-IR, XRD, SEM, TEM, EDS, and elemental mapping, were used to characterize UiO-66-NH@cyanuric chloride@2-aminopyrimidine/Pd, indicating its successful preparation. Three C-C coupling reactions, including the Suzuki, Heck, and Sonogashira coupling reactions, were promoted using the produced catalyst. As a result of the postsynthesis modification (PSM), the proposed catalyst displays improved catalytic performance. In addition, the suggested catalyst was highly recyclable up to ten times without leaching of PdNPs.

摘要

在此,我们通过用富氮有机配体对UiO-66-NH金属有机框架(MOF)进行逐步后合成修饰,制备了一种高效且可重复使用的催化剂,并将其用作制备UiO-66-NH@三聚氯氰@2-氨基嘧啶/Pd的载体。UiO-66-NH@三聚氯氰@2-氨基嘧啶/PdNPs、UiO-66-NH/PdNPs和UiO-66-NH@三聚氯氰/PdNPs的催化性能结果表明,钯纳米颗粒微环境的调节具有高效性。通过后合成修饰添加富氮有机配体导致最终复合材料具有独特结构,有利于碳-碳偶联反应的进行。采用多种技术,包括傅里叶变换红外光谱(FT-IR)、X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、能谱分析(EDS)和元素映射,对UiO-66-NH@三聚氯氰@2-氨基嘧啶/Pd进行了表征,表明其制备成功。使用所制备的催化剂促进了三种碳-碳偶联反应,包括铃木(Suzuki)、赫克(Heck)和索尼加希拉(Sonogashira)偶联反应。作为后合成修饰(PSM)的结果,所提出的催化剂表现出改进的催化性能。此外,所建议的催化剂可高度循环使用多达十次,且钯纳米颗粒无浸出。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/88ff/9996586/e198eb9f3e4d/ao2c07661_0009.jpg

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