Heterogeneous oxidation of cyclohexanone catalyzed by TS-1:Combined experimental and DFT studies |
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| Authors: | Changjiu Xia Long Ju Yi Zhao Hongyi Xu Bin Zhu Feifei Gao Min Lin Zhenyu Dai Xiaodong Zou Xingtian Shu |
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| Institution: | 1. Department of Materials and Environmental Chemistry, Stockholm University, SE-106 91 Stockholm, Sweden;2. State Key Laboratory of Catalytic Materials and Reaction Engineering, Research Institute of Petroleum Processing, SIN0PEC, Beijing100083, China |
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| Abstract: | The reaction mechanism of the oxidation of cyclohexanone catalyzed by titanium silicate zeolite TS-1 using aqueous H2O2 as the oxidant was investigated by combining density function theory (DFT) calculations with experimental studies. DFT calculations showed that H2O2 was adsorbed and activated at the tetrahedral Ti sites. By taking into account the adsorption energy, molecular size, steric hindrance and structural information, a reaction mechanism of Baeyer-Villiger oxidation catalyzed by TS-1 that involves the activation of H2O2 was proposed. Experimental studies showed that the major products of cyclohexanone oxidation by H2O2 catalyzed by a hollow TS-1 zeolite wereε-carprolactone, 6-hydroxyhexanoic acid, and adipic acid. These products were analyzed by GC-MS and were in good agreement with the proposed mechanism. Our studies showed that the reaction mechanism on TS-1 zeolite was different from that on Sn-beta zeolite. |
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| Keywords: | Titanium silicate Zeolite Cyclohexanone Baeyer-Villiger oxidation Hydrogen peroxide Lewis acid catalysis |
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