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使用可磁回收的Pd@SPIONs催化剂实现N-杂芳烃和硝基芳烃的简便转移氢化反应

Facile Transfer Hydrogenation of N-Heteroarenes and Nitroarenes Using Magnetically Recoverable Pd@SPIONs Catalyst.

作者信息

Alghamdi Huda S, Ajeebi Afnan M, Aziz Md Abdul, Alzahrani Atif Saeed, Shaikh M Nasiruzzaman

机构信息

Interdisciplinary Research Center for Hydrogen and Energy Storage (IRC-HES), King Fahd University of Petroleum and Minerals (KFUPM), Dhahran 31261, Saudi Arabia.

Material Science Engineering Department, King Fahd University of Petroleum and Minerals (KFUPM), Dhahran31261, Saudi Arabia.

出版信息

ACS Omega. 2024 Mar 1;9(10):11377-11387. doi: 10.1021/acsomega.3c07550. eCollection 2024 Mar 12.

Abstract

Catalysts with active, selective, and reusable features are desirable for sustainable development. The present investigation involved the synthesis and characterization of bear-surfaced ultrasmall Pd particles (<1 nm) loaded onto the surface of magnetic nanoparticles (8-10 nm). The amount of Pd loading onto the surface of magnetite is recorded as 2.8 wt %. The characterization process covered the utilization of scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), transmission electron microscopy (TEM), inductively coupled plasma (ICP), and X-ray photoelectron spectroscopy (XPS) methods. The Pd@FeO catalyst has shown remarkable efficacy in the hydrogenation of quinoline, resulting in the production of >99% N-ring hydrogenated (py-THQ) product. Additionally, the catalyst facilitated the conversion of nitroarenes into their corresponding aniline derivatives, where hydrogen was achieved by HO molecules with the aid of tetrahydroxydiboron (THDB) as an equilibrium supportive at 80 °C in 1 h. The high efficiency of a transfer hydrogenation catalyst is closely related to the metal-support synergistic effect. The broader scope of functional group tolerance is evaluated. The potential mechanism underlying the hydrogenation process has been elucidated through the utilization of isotopic labeling investigations. The application of the heterocyclic compound hydrogenation reaction is extended to formulate the medicinally important tubular polymerization inhibitor drug synthesis. The investigation of the recyclability of Pd@FeO has been conducted.

摘要

具有活性、选择性和可重复使用特性的催化剂对可持续发展至关重要。本研究涉及负载在磁性纳米颗粒(8 - 10纳米)表面的熊面超小钯颗粒(<1纳米)的合成与表征。负载在磁铁矿表面的钯含量记录为2.8重量%。表征过程涵盖了扫描电子显微镜(SEM)、能量色散光谱(EDS)、透射电子显微镜(TEM)、电感耦合等离子体(ICP)和X射线光电子能谱(XPS)方法的应用。Pd@FeO催化剂在喹啉的氢化反应中表现出显著的效果,生成了>99%的N环氢化(py - THQ)产物。此外,该催化剂促进了硝基芳烃向其相应苯胺衍生物的转化,其中氢气是在80°C下借助四羟基二硼(THDB)作为平衡支持物,由HO分子在1小时内实现的。转移氢化催化剂的高效率与金属 - 载体协同效应密切相关。评估了官能团耐受性的更广泛范围。通过同位素标记研究阐明了氢化过程的潜在机制。扩展了杂环化合物氢化反应的应用,以用于合成具有药用重要性的管状聚合抑制剂药物。已对Pd@FeO的可回收性进行了研究。

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