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钯纳米粒子在铃木-宫浦偶联反应中的尺寸依赖性催化活性及归宿

Size-Dependent Catalytic Activity and Fate of Palladium Nanoparticles in Suzuki-Miyaura Coupling Reactions.

作者信息

Chatterjee Sujit, Bhattacharya Swapan Kumar

机构信息

Department of Chemistry, Jadavpur University, Kolkata 700032, India.

出版信息

ACS Omega. 2018 Oct 9;3(10):12905-12913. doi: 10.1021/acsomega.8b01598. eCollection 2018 Oct 31.

Abstract

Stable, catalytically active palladium nanoparticles of various average diameters (1.9-7.4 nm) have been synthesized and characterized by X-ray diffraction, spectroscopy, and microscopy techniques to demonstrate remarkable size-dependent and renewed catalytic activity toward the Suzuki-Miyaura coupling reaction in green protocol. The catalytic activity is found to depend on the amount of the reducing agent, stabilizer-precursor ratio, solvent composition, and aryl halides used. The product obtained by this reaction is characterized by H NMR, C NMR, and IR spectroscopy analyses. A newly developed kinetic equation illustrates that while the catalyst particles of the lowest dimension are gradually exposed to the reactants and hence activated due to partial removal of capping polymer from the catalyst surface, others are deactivated due to agglomeration during the progress of the reaction, as conformed by the microscopic profiles of the used and unused catalysts.

摘要

已经合成了具有各种平均直径(1.9 - 7.4纳米)的稳定、具有催化活性的钯纳米颗粒,并通过X射线衍射、光谱学和显微镜技术对其进行了表征,以证明在绿色方案中,其对铃木-宫浦偶联反应具有显著的尺寸依赖性和新的催化活性。发现催化活性取决于还原剂的用量、稳定剂与前体的比例、溶剂组成以及所使用的芳基卤化物。通过该反应得到的产物通过1H NMR、13C NMR和红外光谱分析进行表征。一个新开发的动力学方程表明,虽然尺寸最小的催化剂颗粒由于从催化剂表面部分去除封端聚合物而逐渐暴露于反应物并因此被激活,但其他颗粒在反应过程中由于团聚而失活,这一点通过使用过的和未使用的催化剂的微观轮廓得到证实。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8de1/6645063/c9f591c5e2b4/ao-2018-01598m_0001.jpg

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