Mesoporous molecular sieve Al-MCM-41 as a novel catalyst for vapor-phase Beckmann rearrangement of cyclohexanone oxime

被引:35
作者
Ko, AN [1 ]
Hung, CC [1 ]
Chen, CW [1 ]
Ouyang, KH [1 ]
机构
[1] Tunghai Univ, Dept Chem, Taichung 40704, Taiwan
关键词
Al-MCM-41; Beckmann rearrangement; epsilon-caprolactam; cyclohexanone oxime; solid acid;
D O I
10.1023/A:1009038701442
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
Vapor-phase Beckmann rearrangement of cyclohexanone oxime to epsilon -caprolactam has been studied at 1 atm and 300-400 degreesC using mesoporous molecular sieve Al-MCM-41. Benzene and ethanol are utilized as solvents for cyclohexanone oxime. Increasing the reaction temperature enhances the catalyst activity and stability whereas epsilon -caprolactam selectivity varies only slightly. Ethanol exhibits much better catalytic results than benzene. Excellent catalyst performance is attained at 1 atm, 400 degreesC and W/F-C 149.2 g h/mol by using ethanol in the feed; the cyclohexanone oxime conversion and the epsilon -caprolactam selectivity remain higher than 99 and 90%, respectively, during at least 1200 h process time. The highly efficient catalysis on Al-MCM-41 is attributed to its large surface area, uniform mesopores as well as the weak and medium acidity.
引用
收藏
页码:219 / 224
页数:6
相关论文
共 24 条
[1]  
BASF, 1976, Patent No. 1227028
[2]   A NEW FAMILY OF MESOPOROUS MOLECULAR-SIEVES PREPARED WITH LIQUID-CRYSTAL TEMPLATES [J].
BECK, JS ;
VARTULI, JC ;
ROTH, WJ ;
LEONOWICZ, ME ;
KRESGE, CT ;
SCHMITT, KD ;
CHU, CTW ;
OLSON, DH ;
SHEPPARD, EW ;
MCCULLEN, SB ;
HIGGINS, JB ;
SCHLENKER, JL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1992, 114 (27) :10834-10843
[3]   KINETICS OF AND CATALYST DECAY ACCOMPANYING THE GAS-PHASE REARRANGEMENT OF CYCLOHEXANONE-OXIME OVER A HY ULTRASTABLE ZEOLITE [J].
BURGUET, MC ;
AUCEJO, A ;
CORMA, A .
CANADIAN JOURNAL OF CHEMICAL ENGINEERING, 1987, 65 (06) :944-949
[4]   BECKMANN REARRANGEMENT OF CYCLOPENTANONE OXIME CATALYZED BY DECATIONATED ZEOLITE [J].
BUTLER, JD ;
POLES, TC .
JOURNAL OF THE CHEMICAL SOCIETY-PERKIN TRANSACTIONS 2, 1973, (09) :1262-1266
[5]   Mesoporous aluminosilicate of the MCM-41 type:: Its catalytic activity in n-hexane isomerization [J].
Chaudhari, K ;
Das, TK ;
Chandwadkar, AJ ;
Sivasanker, S .
JOURNAL OF CATALYSIS, 1999, 186 (01) :81-90
[6]   STUDIES ON MESOPOROUS MATERIALS .1. SYNTHESIS AND CHARACTERIZATION OF MCM-41 [J].
CHEN, CY ;
LI, HX ;
DAVIS, ME .
MICROPOROUS MATERIALS, 1993, 2 (01) :17-26
[7]   Novel efficient synthesis of β-naphthyl methyl ether using sulfated mesoporous molecular sieve Al-MCM-41 [J].
Chen, LW ;
Chou, CY ;
Ko, AN .
APPLIED CATALYSIS A-GENERAL, 1999, 178 (01) :L1-L6
[8]   Synthesis and characterization of the mesoporous galloaluminosilicate molecular sieve MCM-41 [J].
Cheng, CF ;
Klinowski, J .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1996, 92 (02) :289-292
[9]   HYDROCRACKING OF VACUUM GAS-OIL ON THE NOVEL MESOPOROUS MCM-41 ALUMINOSILICATE CATALYST [J].
CORMA, A ;
MARTINEZ, A ;
MARTINEZSORIA, V ;
MONTON, JB .
JOURNAL OF CATALYSIS, 1995, 153 (01) :25-31
[10]   FACTORS AFFECTING SELECTIVITY IN THE REARRANGEMENT OF CYCLOHEXANONE OXIME TO CAPROLACTAM OVER MODIFIED ALUMINAS [J].
CURTIN, T ;
MCMONAGLE, JB ;
HODNETT, BK .
APPLIED CATALYSIS A-GENERAL, 1992, 93 (01) :75-89