Fundamental insights into the oxidative dehydrogenation of ethane to ethylene over catalytic materials discovered by an evolutionary approach

被引:39
作者
Grubert, G
Kondratenko, E
Kolf, S
Baerns, M
van Geem, P
Parton, R
机构
[1] Inst Appl Chem Berlin Adlershof eV, D-12489 Berlin, Germany
[2] DSM Res BV, NL-6160 MD Geleen, Netherlands
关键词
oxidative dehydrogenation; high-throughput synthesis and testing; evolutionary approach; transient study;
D O I
10.1016/S0920-5861(03)00132-9
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
An evolutionary optimisation procedure combined with high-throughput synthesis and testing has been applied for discovering new catalytic materials for the oxidative dehydrogenation of ethane to ethylene (ODHE). After 10 generations comprising a total of 600 vanadium-free catalytic compositions supported on alpha-Al2O3, Cr/Co/Sn/W and Cr/Mo mixed oxides have been identified as new well performing catalytic materials for the ODHE reaction; ethylene yields of up to 20% and selectivities of 55-65% (500degreesC; C2H6:O-2:Ar = 20:10:70) were achieved. The surface and bulk characteristics of the new catalytic materials derived from near-surface composition, binding energies of the elements (XPS), and phase analysis (XRD) as well as from their surface area (BET) lead to the assumption that for both systems (Cr/Mo or Co/Cr/Sn/W oxide) the active phase is located in the X-ray amorphous part of the material. Based on transient and isotopic experiments it was concluded that the ODHE reaction follows the Mars-Van Krevelen mechanism. The different selectivities towards CO2 and CO between the two systems have been attributed to parallel and consecutive reaction schemes of the product formation, derived from transient experiments. From the fundamental insights obtained improvements of the catalytic performance in the ODHE reaction are suggested. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码:337 / 345
页数:9
相关论文
共 28 条
[1]   Oxidative dehydrogenation of ethane and propane over magnesium-cobalt phosphates COxMg3-x(PO4)2 [J].
Aaddane, A ;
Kacimi, M ;
Ziyad, M .
CATALYSIS LETTERS, 2001, 73 (01) :47-53
[2]   Simple chemical processes based on low molecular-mass alkanes as chemical feedstocks [J].
Baerns, M ;
Buyevskaya, O .
CATALYSIS TODAY, 1998, 45 (1-4) :13-22
[3]   Supported metal oxide and other catalysts for ethane conversion:: a review [J].
Bañares, MA .
CATALYSIS TODAY, 1999, 51 (02) :319-348
[4]   Oxidative dehydrogenation of ethane and n-butane on VOx/Al2O3 catalysts [J].
Blasco, T ;
Galli, A ;
Nieto, JML ;
Trifiro, F .
JOURNAL OF CATALYSIS, 1997, 169 (01) :203-211
[5]   Oxidative dehydrogenation of ethane at millisecond contact times:: Effect of H2 addition [J].
Bodke, AS ;
Henning, D ;
Schmidt, LD ;
Bharadwaj, SS ;
Maj, JJ ;
Siddall, J .
JOURNAL OF CATALYSIS, 2000, 191 (01) :62-74
[6]  
BORESKOV GK, 1984, HETEROGENEOUS CATALY
[7]   Titania-supported cobalt and cobalt-phosphorus catalysts: Characterization and performances in ethane oxidative dehydrogenation [J].
Brik, Y ;
Kacimi, M ;
Ziyad, M ;
Bozon-Verduraz, F .
JOURNAL OF CATALYSIS, 2001, 202 (01) :118-128
[8]  
Buyevskaya O., 2002, CATALYSIS, V16, P155
[9]   Fundamental and combinatorial approaches in the search for and optimisation of catalytic materials for the oxidative dehydrogenation of propane to propene [J].
Buyevskaya, OV ;
Brückner, A ;
Kondratenko, EV ;
Wolf, D ;
Baerns, M .
CATALYSIS TODAY, 2001, 67 (04) :369-378
[10]   Ethylene and propene by oxidative dehydrogenation of ethane and propane - 'Performance of rare-earth oxide-based catalysts and development of redox-type catalytic materials by combinatorial methods' [J].
Buyevskaya, OV ;
Wolf, D ;
Baerns, M .
CATALYSIS TODAY, 2000, 62 (01) :91-99