Characterization of active sites working on FSM-16 during the vapor-phase Beckmann rearrangement of cyclohexanone oxime

被引：25
|
作者：
Shouro, D [1 ]
Ohya, Y [1 ]
Mishima, S [1 ]
Nakajima, T [1 ]
机构：
[1] Shinshu Univ, Grad Sch Sci & Technol, Nagano 3808553, Japan
来源：
APPLIED CATALYSIS A-GENERAL | 2001年 / 214卷 / 01期
关键词：
ring opening of epsilon-caprolactam; deactivation; FSM-16; Beckmann rearrangement;
D O I：
10.1016/S0926-860X(01)00479-3
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 behaviors of E-caprolactam, cyclohexanone oxime and Beckmann rearrangement by-products on FSM-16 and Al2O3/FSM-16 have been investigated in detail by means of TPD and reactions in the presence of organic acids and pyridine. The TPD spectra on FSM-16 of epsilon -caprolactam. cyclohexanone oxime, Beckmann rearrangement by-products and mixtures of by-products can be explained by postulating that there are four kinds of active sites, i.e. two kinds of nitrile formation sites (Sites A and R), a cyclohexanone formation site (Site B) and a nitrile adsorption site (Site alpha). The TPDs of cyclohexanone oxime adsorbed on Al2O3/FSM-16 in the presence and absence of water vapor suggest that the presence of water accelerates the formation of cyclohexanone on Site B. Addition of acetic acid suppresses conversion of epsilon -caprolactam to nitriles, and that addition of pyridine has no effect on the TPD spectrum. Addition of acetic acid to the reactant during the Beckmann rearrangement on Al2O3/FSM-16 improved the epsilon -caprolactam yield and catalyst's life. (C) 2001 Elsevier Science B,V. All rights reserved.
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收藏
页码：59 / 67
页数：9
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