Noncatalytic and catalytic conversion of ethane over V-Mg oxide catalysts prepared via solid reaction or mesoporous precursors

被引:35
作者
Chao, ZS [1 ]
Ruckenstein, E [1 ]
机构
[1] SUNY Buffalo, Dept Chem Engn, Amherst, NY 14260 USA
关键词
ethane; ethene; oxidative dehydrogenation; oxygenates; catalyst; mesoporous; vanadium; magnesium;
D O I
10.1016/j.jcat.2003.11.004
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
This paper deals with both noncatalytic and catalytic conversions of ethane. The effects of reactor configuration (empty tube, tube containing inert material or containing catalyst, and inert material), reaction temperature, reactant composition, and flow rate, as well as catalyst composition and structure, were systematically investigated. Two groups of V-Mg oxides, namely Meso-VMg (originated from mesostructured V-Mg oxide) and Mix-VMg (prepared via a solid reaction between vanadia and magnesia), were employed as catalysts. High conversions and selectivities were obtained at high temperatures during the ethane thermolysis to ethene, accompanied, however, by high carbon depositions, especially in the presence of a catalyst. The contribution of homogeneous reactions to the ODH of ethane was important at high, but less important at low temperatures particularly when the fraction of reactor occupied by inert silica granules was large. For the Mix-VMg catalysts, the ethane conversion and the ethene yield increased but the selectivity to ethene decreased with decreasing V/Mg atomic ratio. The Meso-VMg catalysts exhibited in most cases higher yields and selectivities to ethene than the Mix-VMg ones. In addition, a higher fraction of ethane converted to oxygenates (mainly formaldehyde) as liquid products was obtained over the Meso-VMg catalysts. Magnesium vanadates were identified in the Mix-VMg catalysts; they may represent the active phase for this series of catalysts. A V2O3 phase, which may contain highly dispersed magnesia, was identified and suggested to be responsible together with the large surface area for the high performance of the Meso-VMg catalysts. (C) 2003 Elsevier Inc. All rights reserved.
引用
收藏
页码:17 / 31
页数:15
相关论文
共 70 条
[21]   From microporous to mesoporous molecular sieve materials and their use in catalysis [J].
Corma, A .
CHEMICAL REVIEWS, 1997, 97 (06) :2373-2419
[22]   A Raman spectroscopy study of alumina-supported vanadium oxide catalyst during propane oxidative dehydrogenation with Online activity measurement [J].
Cortez, GG ;
Bañares, MA .
JOURNAL OF CATALYSIS, 2002, 209 (01) :197-201
[23]   REACTIVITY OF SUPPORTED VANADIUM-OXIDE CATALYSTS - THE PARTIAL OXIDATION OF METHANOL [J].
DEO, G ;
WACHS, IE .
JOURNAL OF CATALYSIS, 1994, 146 (02) :323-334
[24]   Oxidative dehydrogenation of ethane over a perovskite-based monolithic reactor [J].
Donsì, F ;
Pirone, R ;
Russo, G .
JOURNAL OF CATALYSIS, 2002, 209 (01) :51-61
[25]   Layered double hydroxide-derived vanadium catalysts for oxidative dehydrogenation of propane influence of interlayer-doping versus layer-doping [J].
Dula, R ;
Wcislo, K ;
Stoch, J ;
Grzybowska, B ;
Serwicka, EM ;
Kooli, F ;
Bahranowski, K ;
Gawel, A .
APPLIED CATALYSIS A-GENERAL, 2002, 230 (1-2) :281-291
[26]   Short contact time oxidative dehydrogenation of propane [J].
Fathi, M ;
Lodeng, R ;
Nilsen, ES ;
Silberova, B ;
Holmen, A .
CATALYSIS TODAY, 2001, 64 (1-2) :113-120
[27]   EFFECT OF COEXISTENCE OF MAGNESIUM VANADATE PHASES IN THE SELECTIVE OXIDATION OF PROPANE TO PROPENE [J].
GAO, XT ;
RUIZ, P ;
XIN, Q ;
GUO, XX ;
DELMON, B .
JOURNAL OF CATALYSIS, 1994, 148 (01) :56-67
[28]  
HABER J, 1998, NATO ASI SERIES
[29]   Excellent promotion by lithium of a lanthanum-calcium oxide catalyst for oxidative dehydrogenation of ethane to ethene [J].
Ji, L ;
Liu, JS .
CHEMICAL COMMUNICATIONS, 1996, (10) :1203-1203
[30]  
Kniel L., 1980, ETHYLENE KEYSTONE PE