SBA-15-supported iron phosphate catalyst for partial oxidation of methane to formaldehyde

被引:79
作者
Wang, Y [1 ]
Wang, XX [1 ]
Su, Z [1 ]
Guo, Q [1 ]
Tang, QH [1 ]
Zhang, QH [1 ]
Wan, HL [1 ]
机构
[1] Xiamen Univ, Dept Chem, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
关键词
methane; partial oxidation; formaldehyde; iron phosphate; SBA-15;
D O I
10.1016/j.cattod.2004.06.037
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
SBA-15-supported iron phosphate (FePO4) has been characterized with XRD, TEM, Raman spectroscopy and H-2-TPR, and studied for the partial oxidation of CH4 with O-2. The characterizations suggest that the FePO4 species with loading amount lower than 40wt.% are encapsulated within the mesoporous channels of SBA-15, and these species possibly exist as small FePO4 clusters with the local coordination environment of iron being similar to that in the crystalline FePO4. However, these encapsulated FePO4 clusters could be reduced at remarkably lower temperatures than the crystalline FePO4. The SBA-15-supported FePO4 catalysts exhibit higher CH4 conversion and HCHO selectivity than the unsupported and the MCM-41-supported ones in the partial oxidation of CH4 with O-2. The catalyst with a loading amount of 5 wt.% shows the highest HCHO selectivity at a given CH4 conversion and the highest HCHO formation rate based on the amount of FePO4 in the catalyst. It is likely that the improved catalytic performances of the SBA-15-supported samples are related to the enhanced redox properties of FePO4 species, the large porous diameter and the high inertness of SBA-15. (C) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:155 / 161
页数:7
相关论文
共 17 条
[1]   Methane partial oxidation by unsupported and silica supported iron phosphate catalysts - Influence of reaction conditions and co-feeding of water on activity and selectivity [J].
Alptekin, GO ;
Herring, AM ;
Williamson, DL ;
Ohno, TR ;
McCormick, RL .
JOURNAL OF CATALYSIS, 1999, 181 (01) :104-112
[2]  
Brown M.J., 1991, CATAL TODAY, V8, P305, DOI 10.1016/0920-5861(91)80056-F
[3]   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
[4]   Excellent catalytic performances of SBA-15-supported vanadium oxide for partial oxidation of methane to formaldehyde [J].
Lin, BM ;
Wang, XX ;
Guo, Q ;
Yang, W ;
Zhang, QH ;
Wang, Y .
CHEMISTRY LETTERS, 2003, 32 (09) :860-861
[5]   Highly efficient VOx/SBA-15 mesoporous catalysts for oxidative dehydrogenation of propane [J].
Liu, YM ;
Cao, Y ;
Zhu, KK ;
Yan, SR ;
Dai, WL ;
He, HY ;
Fan, KN .
CHEMICAL COMMUNICATIONS, 2002, (23) :2832-2833
[6]   Selective photo-assisted oxidation of methane into formaldehyde on mesoporous VOx/SBA-15 catalysts [J].
López, HH ;
Martínez, A .
CATALYSIS LETTERS, 2002, 83 (1-2) :37-41
[7]   Methane partial oxidation by silica-supported iron phosphate catalysts. Influence of iron phosphate content on selectivity and catalyst structure [J].
McCormick, RL ;
Alptekin, GO ;
Williamson, DL ;
Ohno, TR .
TOPICS IN CATALYSIS, 2000, 10 (1-2) :115-122
[8]   Direct conversion of methane into oxygenates [J].
Otsuka, K ;
Wang, Y .
APPLIED CATALYSIS A-GENERAL, 2001, 222 (1-2) :145-161
[9]   NATURAL-GAS CONVERSION TO LIQUID FUELS AND CHEMICALS - WHERE DOES IT STAND [J].
PARKYNS, ND ;
WARBURTON, CI ;
WILSON, JD .
CATALYSIS TODAY, 1993, 18 (04) :385-442
[10]   PARTIAL OXIDATION OF METHANE [J].
PITCHAI, R ;
KLIER, K .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1986, 28 (01) :13-88