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基于高负载磁性离子纳米颗粒网络的可持续钌催化需氧氧化反应。

A sustainable Ru catalyzed aerobic oxidation based on high loading magnetic ionic nanoparticles network.

作者信息

Asgari Sepideh, Ghahremani Mina, Najafvand-Derikvandi Sepideh, Moradi Hesamodin, Tavakolian Mina, Mansouri Fariborz, Karimi Babak

机构信息

Department of Chemistry, Institute for Advanced Studies in Basic Sciences, Prof. Yousef Sobouti Boulevard, Zanjan, 45137-66731, Iran.

Department of Chemical Technologies, Iranian Research Organization for Science and Technology (IROST), Tehran, Iran.

出版信息

Sci Rep. 2025 Aug 3;15(1):28291. doi: 10.1038/s41598-025-07505-5.

DOI:10.1038/s41598-025-07505-5
PMID:40754608
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12319111/
Abstract

In this study, we describe the production of a novel high loading magnetic ionic nanoparticle network (HMINN) encompassing a functionalized imidazolium structure bridging between the core-shell magnetic nanoparticles. The network was constructed through the in situ radical polymerization of tris-vinyl imidazolium moieties on the surface of mercaptopropyl functionalized silica-coated magnetite. The structural and chemical features of the resulting material were comprehensively characterized utilizing various analytical methods such as N adsorption-desorption, FTIR, TGA, HRTEM, ICP, XPS, VSM and elemental analysis. This material was then served to produce a Ru-supported catalyst for the oxidation of alcohols and amines under aerobic conditions. The aerobic oxidation of a diverse variety of benzylic, aliphatic, allylic, cyclic, and heterocyclic substrates was efficiently accomplished in the presence of Ru@HMINN under additive-free conditions and excellent E-factor and EcoScale factor, affording good to excellent yields of the related aldehydes and nitriles. Some of the advantages are the highly available active sites, high ionic density and porous high loading network, the outstanding dispersion of the catalyst in organic media, and the superior ability of imidazolium units to stabilize the Ru nanoparticles while allowing convenient separation of the whole system by applying an external magnet.

摘要

在本研究中,我们描述了一种新型高负载磁性离子纳米粒子网络(HMINN)的制备,该网络包含一个功能化的咪唑结构,连接在核壳磁性纳米粒子之间。该网络是通过在巯基丙基功能化的二氧化硅包覆磁铁矿表面原位自由基聚合三乙烯基咪唑部分构建而成。利用各种分析方法,如N吸附-脱附、傅里叶变换红外光谱(FTIR)、热重分析(TGA)、高分辨透射电子显微镜(HRTEM)、电感耦合等离子体质谱(ICP)、X射线光电子能谱(XPS)、振动样品磁强计(VSM)和元素分析,对所得材料的结构和化学特征进行了全面表征。然后,该材料被用于制备一种Ru负载催化剂,用于在有氧条件下氧化醇和胺。在无添加剂条件下,Ru@HMINN存在时,各种苄基、脂肪族、烯丙基、环状和杂环底物的有氧氧化反应能够高效完成,且具有优异的E因子和生态规模因子,相关醛和腈的产率良好至优异。一些优点包括高可用性的活性位点、高离子密度和多孔高负载网络、催化剂在有机介质中的出色分散性,以及咪唑单元在稳定Ru纳米颗粒的同时通过施加外部磁场方便分离整个体系的卓越能力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f93e/12319111/c662ee00d006/41598_2025_7505_Fig8_HTML.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f93e/12319111/cb193655ccaa/41598_2025_7505_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f93e/12319111/c662ee00d006/41598_2025_7505_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f93e/12319111/831efbfdc353/41598_2025_7505_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f93e/12319111/dbdfc855fc43/41598_2025_7505_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f93e/12319111/ce10fc16a5cf/41598_2025_7505_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f93e/12319111/0c2122b52f54/41598_2025_7505_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f93e/12319111/3be9c0e91624/41598_2025_7505_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f93e/12319111/cb193655ccaa/41598_2025_7505_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f93e/12319111/c662ee00d006/41598_2025_7505_Fig8_HTML.jpg

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