Oxidation of ethylbenzene using some recyclable cobalt nanocatalysts: The role of linker and electrochemical study

被引:101
作者
Arshadi, M. [1 ]
Ghiaci, M. [1 ]
Ensafi, A. A. [1 ]
Karimi-Maleh, H. [1 ]
Suib, Steven L. [2 ]
机构
[1] Isfahan Univ Technol, Dept Chem, Esfahan 8415683111, Iran
[2] Univ Connecticut, Dept Chem, Storrs, CT 06269 USA
基金
美国国家科学基金会;
关键词
Cobalt; Ethylbenzene; Oxidation; Acetophenone; Carbon nanotubes; SiO2-Al2O3; KINETIC RESOLUTION; CATALYTIC-ACTIVITY; TERMINAL EPOXIDES; MOLECULAR-SIEVES; COMPLEXES; RESONANCE; MCM-41;
D O I
10.1016/j.molcata.2011.01.027
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In this paper some Co(II)-Schiff base complexes were immobilized on SiO2-Al2O3 mixed-oxide using two linkers with different flexibilities (3-aminopropyl and 2-aminoethyl-3-aminopropyl). The synthesized materials were characterized by FT-IR spectroscopy, UV-Vis, CHN elemental analysis, ICP-MS, EPR, SEM, TEM, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The catalytic activity of the heterogenized Co(II)-Schiff base complexes in the oxidation of ethylbenzene was studied without the need of any solvent, at 353 K, using tert-butyl hydroperoxide as oxygen source. The best catalyst has a higher catalytic activity (86%) and selectivity to acetophenone (99%) at TBHP/ethylbenzene molar ratio (1:1), and could be reused at least 4 times without significant loss in acetophenone yield, suggesting that no complex leaching took place under the reaction conditions. The electrochemical data about oxidation of the immobilized Co(II)-Schiff base complexes at the surface of multi-walled carbon nanotubes was also studied. The results indicate that the Co-complexes anchored on the modified SiO2-Al2O3 mixed-oxide have an easily oxidizable environment, which led to higher catalytic activity and selectivity. (C) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码:71 / 83
页数:13
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