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超临界水辅助制备可回收金纳米颗粒及其在可持续条件下交叉偶联反应中的催化应用。

Supercritical water assisted preparation of recyclable gold nanoparticles and their catalytic utility in cross-coupling reactions under sustainable conditions.

作者信息

Raheem Abbasriyaludeen Abdul, Thangasamy Pitchai, Sathish Marappan, Praveen Chandrasekar

机构信息

Materials Electrochemistry Division, Central Electrochemical Research Institute (CSIR Laboratory) Alagappapuram Karaikudi-630003 Tamil Nadu India

Academy of Scientific and Innovative Research (AcSIR) Ghaziabad-201002 Uttar Pradesh India.

出版信息

Nanoscale Adv. 2019 Jun 27;1(8):3177-3191. doi: 10.1039/c9na00240e. eCollection 2019 Aug 6.

DOI:10.1039/c9na00240e
PMID:36133589
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9418514/
Abstract

Preparation of gold nanoparticles (AuNPs) in environmentally friendly water without using any reducing agents under supercritical conditions is demonstrated. PXRD, XPS, FE-SEM and HR-TEM analysis confirmed the formation of phase-pure and crystalline AuNPs of the size of ∼10-30 nm. The catalytic potential of AuNPs was manifested through a generalized green procedure that could accommodate both Sonogashira as well as Suzuki coupling under aqueous conditions at low catalytic loading (0.1 mol%). The AuNP catalyst was found to be recuperated after the reaction and reused for up to six catalytic cycles with no leaching out of gold species as confirmed through ICP-OES analysis. With no confinement of AuNP catalysis to cross-coupling reaction, synthetic extension to one-flask preparation of π-conjugated semiconductors (4 examples) and their optoelectronic properties were also investigated. Other significant features of the present work include short reaction time, site-selectivity, wide substrate scope, high conversion, good chemical yields and applicability in gram-scale synthesis. Overall, the results of this paper signify an operationally sustainable supercritical fluid processing method for the synthesis of AuNPs and their catalytic application towards cross-coupling reactions in green media.

摘要

本文展示了在超临界条件下,无需使用任何还原剂,在环境友好型水中制备金纳米颗粒(AuNPs)的方法。粉末X射线衍射(PXRD)、X射线光电子能谱(XPS)、场发射扫描电子显微镜(FE-SEM)和高分辨透射电子显微镜(HR-TEM)分析证实,形成了尺寸约为10 - 30 nm的纯相且结晶的AuNPs。AuNPs的催化潜力通过一种通用的绿色方法得以体现,该方法能够在低催化负载量(0.1 mol%)的水性条件下,实现Sonogashira偶联反应以及Suzuki偶联反应。通过电感耦合等离子体发射光谱(ICP-OES)分析证实,AuNP催化剂在反应后能够回收,并可重复使用多达六个催化循环,且没有金物种浸出。由于AuNP催化不限于交叉偶联反应,因此还研究了其在一锅法制备π共轭半导体(4个实例)方面的合成扩展及其光电性质。本工作的其他显著特点包括反应时间短、位点选择性、底物范围广、转化率高、化学产率良好以及在克级合成中的适用性。总体而言,本文的结果表明了一种在操作上可持续的超临界流体处理方法,用于合成AuNPs及其在绿色介质中对交叉偶联反应的催化应用。

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