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功能化多壁碳纳米管(MWNTs)负载锰(III)希夫碱配合物对间二甲苯的合成、表征及催化氧化作用。

Synthesis, characterization and catalytic oxidation of para-xylene by a manganese(III) Schiff base complex on functionalized multi-wall carbon nanotubes (MWNTs).

机构信息

Institute of Nano Science and Nano Technology, University of Kashan, Kashan, P. O. Box. 87317-51167, IR Iran.

出版信息

Dalton Trans. 2010 Aug 21;39(31):7330-7. doi: 10.1039/b923416k. Epub 2010 Jul 2.

Abstract

In the present study, hydroxyl functionalized manganese(III) Schiff-base; [Mn((OH)(2)-salophen)Cl] [(OH)(2)-salophen] = (N,N'-bis(4-hydroxysalicylidene)phenylene-1,2-diamine); has been covalently anchored on modified multi-wall carbon nanotubes (MWNTs); [Mn((OH)(2)-salophen)Cl]@MWNTs]. The new modified MWNTs have been characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron (XPS), thermal analysis, FT-IR spectroscopy and elemental analysis. The results suggest that the symmetrical Schiff-base is a bivalent anion with tetradentate N(2)O(2) donors derived from the phenolic oxygen and azomethine nitrogen. 4-Hydroxy salophen; [(OH)(2)-salophen], complex of manganese, grafted on the walls of MWNTs have been investigated as catalysts for the aerobic oxidation of para-xylene in the absence of added halogen promoters and using tert-butylhydroperoxide (TBHP) as the initiator at low temperatures. The major products include toluic acid, toluyl aldehyde and toluyl alcohol. The MWNTs-grafted complex did not undergo any colour change during the reaction and could be easily separated and reused many times. In contrast, the neat complex, while they were active in the first cycle, was completely destroyed during the run and changed colour. They, however, gave lower conversions compared to the grafted catalyst.

摘要

在本研究中,羟基功能化锰(III)希夫碱; [Mn((OH)(2)-salophen)Cl] [(OH)(2)-salophen] = (N,N'-双(4-羟基水杨醛)亚苯基-1,2-二胺); 已共价锚定在改性多壁碳纳米管 (MWNTs); [Mn((OH)(2)-salophen)Cl]@MWNTs]。新的改性 MWNTs 通过透射电子显微镜 (TEM)、X 射线衍射 (XRD)、X 射线光电子 (XPS)、热分析、FT-IR 光谱和元素分析进行了表征。结果表明,对称希夫碱是一种二价阴离子,具有来自酚氧和亚胺氮的四齿 N(2)O(2)供体。已研究了接枝在 MWNTs 壁上的 4-羟基水杨醛; [(OH)(2)-salophen]、锰配合物作为无外加卤素促进剂的条件下,在低温下使用叔丁基过氧化氢 (TBHP)作为引发剂,用于对二甲苯的有氧氧化的催化剂。主要产物包括对甲苯酸、对甲苯醛和对甲苯醇。在反应过程中,接枝的配合物没有发生任何颜色变化,并且可以很容易地多次分离和重复使用。相比之下,尽管 neat complex 在第一个循环中具有活性,但在运行过程中完全被破坏并变色。然而,它们的转化率低于接枝催化剂。

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