Effect of alkali and alkaline earth metal ions on the catalytic epoxidation of styrene with molecular oxygen using cobalt(II)-exchanged zeolite X

被引:192
作者
Sebastian, Jince [1 ]
Jinka, Krishna Mohan [1 ]
Jasra, Raksh Vir [1 ]
机构
[1] Cent Salt & Marine Chem Res Inst, Silicates & Catalysis Discipline, Bhavnagar 364002, Gujarat, India
关键词
molecular oxygen; styrene; styrene oxide; NaCo(II)X; epoxidation; alkali and alkaline earth-exchanged zeolite X;
D O I
10.1016/j.jcat.2006.09.005
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
Liquid-phase catalytic epoxidation of styrene to styrene epoxide was carried out at 373 K using molecular oxygen at atmospheric pressure, in the presence of Co(II)-exchanged zeolite X. Styrene conversion of > 99% with styrene oxide selectivity up to 68% was achieved using NaCoX. Alkali and alkaline earth metal cations were introduced into the zeolite catalyst to increase styrene conversion and styrene oxide selectivity. Replacing the sodium ions with alkali metal cations increased styrene oxide selectivity from 68% for NaCoX19 to 77% for CsCoX20. Styrene oxide selectivity further increased on replacing the sodium ions with alkaline earth metal cations, and styrene oxide selectivity up to 85% and styrene conversion > 99% was obtained with CaCoX, SrCoX, and BaCoX. This is the first report of such a high styrene epoxide selectivity with a heterogeneous catalyst observed for styrene epoxidation using molecular oxygen. The presence of a small amount of water in the reaction system increases styrene conversion without affecting styrene oxide selectivity. The cobalt-exchanged zeolite X catalysts showed similar catalytic activity even after three catalytic reaction cycles. (c) 2006 Elsevier Inc. All rights reserved.
引用
收藏
页码:208 / 218
页数:11
相关论文
共 64 条
[1]   Intrazeolite photochemistry .17. Zeolites as electron donors: Photolysis of methylviologen incorporated within zeolites [J].
Alvaro, M ;
Garcia, H ;
Garcia, S ;
Marquez, F ;
Scaiano, JC .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (16) :3043-3051
[2]  
Barrer R.M., 1978, ZEOLITES CLAY MINERA
[3]  
Base D., 1999, MICROPOR MESOPOR MAT, V33, P265
[4]   Role of cobalt molecular sieves in the liquid-phase oxidation of cyclohexane to adipic acid [J].
Belkhir, I ;
Germain, A ;
Fajula, F ;
Fache, E .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1998, 94 (12) :1761-1764
[5]  
Breck D.W, 1974, ZEOLITE MOL SIEVES
[6]   Structure of a cyclopropane sorption complex of dehydrated fully Cd2+-exchanged zeolite A [J].
Choi, EY ;
Kim, Y ;
Seff, K .
MICROPOROUS AND MESOPOROUS MATERIALS, 2000, 41 (1-3) :61-68
[7]   Epoxidation of styrene by anhydrous H2O2 over TS-1 and γ-Al2O3 catalysts:: effect of reaction water, poisoning of acid sites and presence of base in the reaction mixture [J].
Choudhary, VR ;
Patil, NS ;
Bhargava, SK .
CATALYSIS LETTERS, 2003, 89 (1-2) :55-62
[8]   SYNTHETIC MODELS FOR OXYGEN-BINDING HEMOPROTEINS [J].
COLLMAN, JP .
ACCOUNTS OF CHEMICAL RESEARCH, 1977, 10 (07) :265-272
[9]   Cobalt catalyzed autoxidation of monoterpenes in acetic acid and acetonitrile solutions [J].
da Silva, MJ ;
Robles-Dutenhefner, P ;
Menini, L ;
Gusevskaya, EV .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2003, 201 (1-2) :71-77
[10]   New perspectives on basic zeolites as catalysts and catalyst supports [J].
Davis, RJ .
JOURNAL OF CATALYSIS, 2003, 216 (1-2) :396-405