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磁性可回收的钯-四氧化三铁异二聚体纳米晶体催化有机反应的机理研究

Mechanistic studies of magnetically recyclable Pd - Fe3O4 heterodimeric nanocrystal-catalyzed organic reactions.

作者信息

Byun Sangmoon, Chung Jooyoung, Kwon Jungmin, Moon Kim B

机构信息

Department of Chemistry, College of Natural Sciences, Seoul National University, Seoul 151-747 (Korea), Fax: (+82) 2-872-7505.

出版信息

Chem Asian J. 2015 Apr;10(4):982-8. doi: 10.1002/asia.201403201. Epub 2015 Jan 23.

DOI:10.1002/asia.201403201
PMID:25620124
Abstract

Recently, we have reported several catalytic applications of new Pd - Fe3 O4 heterodimeric nanocrystals as magnetically separable catalysts. Successful applications of the nanocrystals towards various useful organic reactions such as Suzuki, Heck, and Sonogashira coupling reactions, direct C - H arylation, and Wacker oxidation have been recorded. However, detailed mechanistic courses of the reactions have not been delineated, and it was not clear whether these processes proceeded through a homogeneous or heterogeneous mechanism. Here, we report detailed mechanistic investigations of the reactions employing the Pd - Fe3 O4 nanoparticle catalysts. Suzuki coupling and Wacker oxidation reactions were chosen as two representative heterogeneous reactions employing the Pd - Fe3 O4 catalysts, and general kinetic studies, hot filtration tests, and three-phase tests were carried out for the two reactions. The studies showed that the reactions most probably proceed via a solution-phase mechanism.

摘要

最近,我们报道了新型钯-四氧化三铁异二聚体纳米晶体作为磁分离催化剂的几种催化应用。已记录到这些纳米晶体在各种有用的有机反应中成功应用,如铃木反应、赫克反应、索尼加什ira偶联反应、直接碳-氢键芳基化反应和瓦克氧化反应。然而,这些反应的详细机理过程尚未阐明,并且不清楚这些过程是通过均相还是非均相机理进行的。在此,我们报道了使用钯-四氧化三铁纳米颗粒催化剂对这些反应进行的详细机理研究。选择铃木偶联反应和瓦克氧化反应作为使用钯-四氧化三铁催化剂的两个代表性非均相反应,并对这两个反应进行了一般动力学研究、热过滤试验和三相试验。研究表明,这些反应很可能通过溶液相机理进行。

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