Beckmann rearrangement of cyclohexanone oxime over Al-MCM-41 and P modified Al-MCM-41 molecular sieves

被引:32
作者
Zhang, Dongshun [1 ]
Wang, Rijie [1 ]
Yang, Xiaoxia [1 ]
机构
[1] Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
关键词
Phosphorus modified Al-MCM-41; Beckmann rearrangement; Cyclohexanone oxime; Caprolactam; EPSILON-CAPROLACTAM; BETA ZEOLITES; ACTIVE-SITES; MFI ZEOLITES; CATALYSTS; MCM-41; ACIDS; PHOSPHORUS; SI-MCM-41; SILICA;
D O I
10.1016/j.catcom.2010.11.006
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
P modified Al-MCM-41 molecular sieves were prepared via impregnating method and applied to vapor-phase Beckmann rearrangement reaction. The catalysts were characterized by XRD, N-2 adsorption, ICP-OES, NH3-TPD and Al-27 and P-31 MAS NMR spectroscopy. NH3-TPD results reveal that P modification of Al-MCM-41 can increase the number as well as the strength of weak acid sites, whereas the introduction of P decreases the number of intermediate acid sites. Al-27 and P-31 MAS NMR results indicate that formation of Si-O-P-O-Al seems to be favored in P modified Al-MCM-41 catalysts. Overall, these results indicate that P modified Al-MCM-41 catalysts can improve their selectivity for caprolactam. In addition, more abound weak acid sites with certain acid strength are favorable to Beckmann rearrangement. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:399 / 402
页数:4
相关论文
共 27 条
  • [1] Esterification of alkyl acids with alkanols over MCM-41 molecular sieves: Influence of hydrophobic surface on condensation reaction
    Ajaikumar, S.
    Pandurangan, A.
    [J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2007, 266 (1-2) : 1 - 10
  • [2] Highly active and selective Nb modified MCM-41 catalysts for Beckmann rearrangement of cyclohexanone oxime to ε-caprolactam
    Anilkumar, M.
    Hoelderich, W. F.
    [J]. JOURNAL OF CATALYSIS, 2008, 260 (01) : 17 - 29
  • [3] Stabilization effect of phosphorus on steamed H-MFI zeolites
    Caeiro, G.
    Magnoux, P.
    Lopes, J. M.
    Ribeiro, F. Ramoa
    Menezes, S. M. C.
    Costa, A. F.
    Cerqueira, H. S.
    [J]. APPLIED CATALYSIS A-GENERAL, 2006, 314 (02) : 160 - 171
  • [4] Active sites for the liquid-phase Beckmann rearrangement of cyclohexanone, acetophenone and cyclododecanone oximes, catalyzed by beta zeolites
    Camblor, MA
    Corma, A
    Garcia, H
    Semmer-Herledan, V
    Valencia, S
    [J]. JOURNAL OF CATALYSIS, 1998, 177 (02) : 267 - 272
  • [5] Beckmann rearrangement of cyclohexanone oxime over mesoporous Si-MCM-41 and Al-MCM-41 molecular sieves
    Chaudhari, K
    Bal, R
    Chandwadkar, AJ
    Sivasanker, S
    [J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2002, 177 (02) : 247 - 253
  • [6] Synthesis and characterization of novel mesoporous aluminosilicate MCM-41 containing aluminophosphate building units
    Conesa, TD
    Mokaya, R
    Campelo, JM
    Romero, AA
    [J]. CHEMICAL COMMUNICATIONS, 2006, (17) : 1839 - 1841
  • [7] Lewis acids:: From conventional homogeneous to green homogeneous and heterogeneous catalysis
    Corma, A
    García, H
    [J]. CHEMICAL REVIEWS, 2003, 103 (11) : 4307 - 4365
  • [8] Catalytic application of mesoporous molecular sieves to vapor-phase Beckmann rearrangement of cyclohexanone oxime
    Dai, LX
    Koyama, K
    Tatsumi, T
    [J]. CATALYSIS LETTERS, 1998, 53 (3-4) : 211 - 214
  • [9] Highly selective vapor phase Beckmann rearrangement over H-USY zeolites
    Dai, LX
    Koyama, K
    Miyamoto, M
    Tatsumi, T
    [J]. APPLIED CATALYSIS A-GENERAL, 1999, 189 (02) : 237 - 242
  • [10] Beckmann rearrangement of cyclohexanone oxime over Silicalite-1: an FT-IR spectroscopic study
    Flego, C
    Dalloro, L
    [J]. MICROPOROUS AND MESOPOROUS MATERIALS, 2003, 60 (1-3) : 263 - 271