Catalysis of chitosan-supported iron tetraphenylporphyrin for aerobic oxidation of cyclohexane in absence of reductants and solvents

被引:123
作者
Guo, CC [1 ]
Huang, G [1 ]
Zhang, XB [1 ]
Guo, DC [1 ]
机构
[1] Hunan Univ, Coll Chem & Chem Engn, Changsha 410082, Peoples R China
基金
中国国家自然科学基金;
关键词
chitosan; supported metalloporphyrins; cyclohexane oxidation; oxygen;
D O I
10.1016/S0926-860X(03)00108-X
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
The chitosan-supported iron(Ill) tetraphenylporphyrin was prepared and characterized structurally, and its ability to catalyse oxidation of cyclohexane into cyclohexanone and cyclohexanol with air in absence of any reductants and solvents was studied. The research results showed that the amino groups of the chitosan coordinated axially with the iron atoms of chloro [tetraphenylporphinatoiron (111)] to form chitosan-supported ironporphyrin, which has better catalytic power for cyclohexane oxidation with air than the corresponding unsupported ironporphyrin. Under reaction conditions of 418 K and 0.8 MPa, the cyclohexane oxidation catalyzed by chitosan-supported iron(III) tetraphenylporphyrin had 1.40 x 10(5) catalyst mole turnover (based on the iron atom), 10.48% cyclohexane conversion and the 79.20% cyclohexanone and cyclohexanol selectivity, respectively. The turnover in cyclohexane oxidation catalyzed by the supported ironporphyrin is about 22 times bigger than that by unsupported ironporphyrin and the conversion is about double. The values are also higher than 3.9% conversion and 78% selectivity catalyzed by soluble cobalt catalyst used in industry at present. This paper has also investigated the influences of reaction time, temperature and pressure on the catalyst turnover, cyclohexane conversion and ratio of cyclohexanol to cyclohexanone in the cyclohexane oxidation catalyzed by the chitosan-supported iron(111) tetraphenylporphyrin. (C) 2003 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:261 / 267
页数:7
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