SBA-15-supported molybdenum oxides as efficient catalysts for selective oxidation of ethane to formaldehyde and acetaldehyde by oxygen

被引:77
作者
Lou, Yinchuan [1 ]
Wang, Huichun [1 ]
Zhang, Qinghong [1 ]
Wang, Ye [1 ]
机构
[1] Xiamen Univ, State Key Lab Phys Chem Solid Surfaces, Coll Chem & Chem Engn, Xiamen 361005, Peoples R China
基金
中国国家自然科学基金;
关键词
molybdenum oxide; SBA-15; selective oxidation; ethane; formaldehyde; acetaldehyde;
D O I
10.1016/j.jcat.2007.02.011
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
The selective oxidation of ethane was investigated over SBA-15-supported molybdenum oxide catalysts. Our characterizations suggest that the MoOx species were dispersed mostly in mesoporous channels of SBA- 15 at Mo content <9.5 wt%. At higher Mo content (15.4 and 20.1 wt%), MoOx nanoparticles together with small amount of MoO3 crystallites were found. The growth of MoOx species in mesoporous channels to MoOx nanoparticles causes the collapse of the silica wall of SBA-15. The rate of ethane conversion per Mo atom over the catalyst with Mo content of 9.5-20.1 wt% was significantly higher than that over the catalyst with lower Mo content, suggesting that polymeric MoOx clusters and MoOx nanoparticles are more active toward ethane activation. The catalysts with highly dispersed MoOx species favor the selectivity of acetaldehyde, whereas those containing polymeric Moos clusters or MoOx nanoparticles show higher formaldehyde formation rates. Formaldehyde is likely produced through the consecutive oxidation of ethylene. (C) 2007 Elsevier Inc. All rights reserved.
引用
收藏
页码:245 / 255
页数:11
相关论文
共 38 条
[1]   Scientific basis for process and catalyst design in the selective oxidation of methane to formaldehyde [J].
Arena, F ;
Parmaliana, A .
ACCOUNTS OF CHEMICAL RESEARCH, 2003, 36 (12) :867-875
[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]  
BANARES MA, 1993, ACS SYM SER, V523, P355
[4]   Supported metal oxide and other catalysts for ethane conversion:: a review [J].
Bañares, MA .
CATALYSIS TODAY, 1999, 51 (02) :319-348
[5]   Structure and properties of oxidative dehydrogenation catalysts based on MoO3/Al2O3 [J].
Chen, K ;
Xie, S ;
Bell, AT ;
Iglesia, E .
JOURNAL OF CATALYSIS, 2001, 198 (02) :232-242
[6]   The relationship between the electronic and redox properties of dispersed metal oxides and their turnover rates in oxidative dehydrogenation reactions [J].
Chen, KD ;
Bell, AT ;
Iglesia, E .
JOURNAL OF CATALYSIS, 2002, 209 (01) :35-42
[7]  
ERDOHELYI A, 1992, J CATAL, V135, P563
[8]   Comparison of silica-supported MoO3 and V2O5 catalysts in the selective partial oxidation of methane [J].
Faraldos, M ;
Banares, MA ;
Anderson, JA ;
Hu, HC ;
Wachs, IE ;
Fierro, JLG .
JOURNAL OF CATALYSIS, 1996, 160 (02) :214-221
[9]   Catalytic performance of mesoporous VOx/SBA-15 catalysts for the partial oxidation of methane to formaldehyde [J].
Fornés, V ;
López, C ;
López, HH ;
Martínez, A .
APPLIED CATALYSIS A-GENERAL, 2003, 249 (02) :345-354
[10]   CATALYTIC SYNTHESIS OF METHANOL AND FORMALDEHYDE BY PARTIAL OXIDATION OF METHANE [J].
HALL, TJ ;
HARGREAVES, JSJ ;
HUTCHINGS, GJ ;
JOYNER, RW ;
TAYLOR, SH .
FUEL PROCESSING TECHNOLOGY, 1995, 42 (2-3) :151-178