Structural features of Na2WO4-MOx/SiO2 catalysts in oxidative coupling of methane reaction

被引:55
作者
Malekzadeh, A. [1 ]
Dalai, A. K. [2 ]
Khodadadi, A. [3 ]
Mortazavi, Y. [3 ]
机构
[1] Damghan Univ Basic Sci, Sch Chem, Damghan, Iran
[2] Univ Saskatchewan, Dept Chem Engn, Saskatoon, SK S7N 5C5, Canada
[3] Univ Tehran, Dept Chem Engn, Tehran, Iran
关键词
OCM; surface morphology; transition metal oxide; redox catalyst; alkali ions;
D O I
10.1016/j.catcom.2007.09.026
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
Oxidative coupling of methane conversion (OCM) and C-2 selectivity on Na2WO4-MOx/SiO2 catalysts, where M is V, Cr, Mn, Fe, Co or Zn are related to surface morphology, textural properties and reduction behavior of the catalysts. The catalysts are prepared by sequential impregnation of aqueous solution of metal salts and then sodium tungstate on the silica followed by drying and calcination at 800 degrees C for 8 h. Methane conversion increases with the transition metal compound of the catalysts in the order of V similar to Cr similar to Zn < Fe similar to Co < Mn while the C-2 selectivity enhances in the order of V similar to Cr << Fe similar to Co similar to Zn < Mn. XRD and SEM results reveal some interactions between the V and Cr oxides and silica support, decreasing the tungstate peaks intensities and deteriorating catalyst bulk properties and both OCM conversion and selectivity. Both silica and Mn, Fe, Co and Zn transition metals, however, interact with sodium tungstate, forming an OCM selective catalyst. TPR analyses combined with the XRD and SEM results show that the metal-metal and metal-support interactions, which take place due to the presence of sodium ion, depend on the transition metal that in turn affect catalyst performance. Moderation of the transition metal-tungstate interaction is proposed as the main chemical role of sodium ion in these series of catalysts. Results reveal that this interaction improves the redox properties of catalyst, which are related to the transition metals, forming a selective catalyst. (c) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:960 / 965
页数:6
相关论文
共 17 条
[1]  
Fang X., 1992, J MOL CATALYSIS CHIN, V6, P427
[2]   Surface WO4 tetrahedron:: the essence of the oxidative coupling of methane over M-W-Mn/SiO2 catalysts [J].
Ji, SF ;
Xiao, TC ;
Li, SB ;
Chou, LJ ;
Zhang, B ;
Xu, CZ ;
Hou, RL ;
York, APE ;
Green, MLH .
JOURNAL OF CATALYSIS, 2003, 220 (01) :47-56
[3]   Methane activation over Mn2O3-Na2WO4/SiO2 catalyst and oxygen spillover [J].
Jiang, ZC ;
Gong, H ;
Li, SB .
SPILLOVER AND MIGRATION OF SURFACE SPECIES ON CATALYSTS, 1997, 112 :481-490
[4]   OXIDE SUPPORT INTERACTION AND SURFACE RECONSTRUCTION IN THE NA2WO4/SIO2 SYSTEM [J].
JIANG, ZC ;
YU, CJ ;
FANG, XP ;
LI, SB ;
WANG, HL .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (49) :12870-12875
[5]   Catalytic conversion of methane to more useful chemicals and fuels: a challenge for the 21st century [J].
Lunsford, JH .
CATALYSIS TODAY, 2000, 63 (2-4) :165-174
[6]   THE CATALYTIC OXIDATIVE COUPLING OF METHANE [J].
LUNSFORD, JH .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION IN ENGLISH, 1995, 34 (09) :970-980
[7]   CRITICAL PERFORMANCE EVALUATION OF CATALYSTS AND MECHANISTIC IMPLICATIONS FOR OXIDATIVE COUPLING OF METHANE [J].
MAITRA, AM .
APPLIED CATALYSIS A-GENERAL, 1993, 104 (01) :11-59
[8]   Oxidative coupling of methane over lithium doped (Mn+W)/SiO2 catalysts [J].
Malekzadeh, A. ;
Khodadadi, A. ;
Dalai, A. K. ;
Abedini, M. .
JOURNAL OF NATURAL GAS CHEMISTRY, 2007, 16 (02) :121-129
[9]   Critical influence of mn on low-temperature catalytic activity of Mn/Na2WO4/SiO2 catalyst for oxidative coupling of methane [J].
Malekzadeh, A ;
Abedini, M ;
Khodadadi, AA ;
Amini, M ;
Mishra, HK ;
Dalai, AK .
CATALYSIS LETTERS, 2002, 84 (1-2) :45-51
[10]  
Malekzadeh A., 2001, CATAL COMMUN, V2, P241, DOI DOI 10.1016/S1566-7367(01)00034-6