Theoretical study on vapour phase Beckmann rearrangement of cyclohexanone oxime over a high silica MFI zeolite

被引：34
|
作者：
Ishida, M
Suzuki, T
Ichihashi, H
Shiga, A
机构：
[1] Sumitomo Chem Co Ltd, Tsukuba Res Lab, Tsukuba, Ibaraki 3003294, Japan
[2] Sumitomo Chem Co Ltd, Basic Chem Res Lab, Sobiraki, Niihama 7925821, Japan
来源：
CATALYSIS TODAY | 2003年 / 87卷 / 1-4期
关键词：
cyclohexanone; Beckmann rearrangement; double numerical polarization;
D O I：
10.1016/j.cattod.2003.10.021
中图分类号：
O69 [应用化学];
学科分类号：
081704 ;
摘要：
We have studied an activation mechanism of cyclohexanone oxime in a cavity of high silica MFI zeolite by using PIO analysis proposed by Fujimoto et al. DFT calculation reveals that the bond length of N-OH becomes longer when water coordinates on oxygen of oxime. The PIO clearly shows out-of-phase interaction between N and O. This out-of-phase interaction is also observed in the PIO of oxime/MFI zeolite cluster model and weakens the N-O bond. Hydrogen bond of Si-OH of nest silanols to oxime is a trigger of vapour phase Beckmann rearrangement. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码：187 / 194
页数：8
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