La-promoted Na2WO4/Mn/SiO2 catalysts for the oxidative conversion of methane simultaneously to ethylene and carbon monoxide

被引:55
作者
Wu, Jingjing [1 ]
Zhang, Haili [1 ]
Qin, Song [1 ]
Hu, Changwei [1 ]
机构
[1] Sichuan Univ, Coll Chem, Minist Educ, Key Lab Green Chem & Technol, Chengdu 610064, Peoples R China
基金
中国国家自然科学基金;
关键词
oxidative coupling of methane; La-promoted Na2WO4/Mn/SiO2 catalyst; surface oxygen species;
D O I
10.1016/j.apcata.2007.02.009
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
A series of La-promoted 5 wt% Na2WO4/2 wt% Mn/SiO2 catalysts were prepared by varying the impregnation sequence and the concentration of La promoter, and their catalytic performance for the oxidative conversion of methane was investigated in a micro-quartz-tube reactor. The catalysts were characterized by X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD). It was found that the existence of Mn ions was in favor of the dispersion of La species on the catalyst, and the addition of La promoter could increase the dispersion of Na2WO4, which enriched the amount of surface oxygen species connected with the metal atoms. This oxygen species was found to be active for the oxidative coupling of methane to C-2 hydrocarbons. The selectivity and yield of C-2 hydrocarbons with a C2H4/CO ratio of 1/1 reached the optimized value of about 56% and 25%, respectively, at 800 degrees C, over the 5 wt% Na2WO4/2 wt% La-2 wt% Mn/SiO2 catalyst prepared by co-impregnation of La and Mn. (C) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:126 / 134
页数:9
相关论文
共 40 条
[1]  
AN CT, 1996, J CATAL, V163, P399
[2]   COMPETITION BETWEEN THE GAS AND SURFACE-REACTIONS FOR THE OXIDATIVE COUPLING OF METHANE .1. NONISOTHERMAL RESULTS IN CATALYTIC JET-STIRRED REACTOR [J].
BARBE, P ;
LI, YD ;
MARQUAIRE, PM ;
COME, GM ;
BARONNET, F .
CATALYSIS TODAY, 1994, 21 (2-3) :409-415
[3]   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
[4]   Influence of SnO2-doped W-Mn/SiO2 for oxidative conversion of methane to high hydrocarbons at elevated pressure [J].
Chou, LJ ;
Cai, YC ;
Zhang, B ;
Niu, JZ ;
Ji, SF ;
Li, SB .
APPLIED CATALYSIS A-GENERAL, 2003, 238 (02) :185-191
[5]   CeO2-promoted W-Mn/SiO2 catalysts for conversion of methane to C3-C4 hydrocarbons at elevated pressure [J].
Chou, LJ ;
Cai, YC ;
Zhang, B ;
Niu, JZ ;
Ji, SF ;
Li, SB .
CHEMICAL COMMUNICATIONS, 2002, (09) :996-997
[6]   Competition between gas and surface reactions in the oxidative coupling of methane .2. Isothermal experiments in a catalytic jet-stirred gas phase reactor [J].
Come, GM ;
Li, YD ;
Barbe, P ;
Gueritey, N ;
Marquaire, PM ;
Baronnet, F .
CATALYSIS TODAY, 1996, 30 (1-3) :215-222
[7]   Oxidative coupling of methane catalyzed unexpected synergistic effect of the by rare earth oxides oxide mixtures [J].
Dedov, AG ;
Loktev, AS ;
Moiseev, II ;
Aboukais, A ;
Lamonier, JF ;
Filimonov, IN .
APPLIED CATALYSIS A-GENERAL, 2003, 245 (02) :209-220
[8]   OXIDATIVE COUPLING OF METHANE OVER OXIDE-SUPPORTED BARIUM CATALYSTS [J].
DISSANAYAKE, D ;
LUNSFORD, JH ;
ROSYNEK, MP .
JOURNAL OF CATALYSIS, 1993, 143 (01) :286-298
[9]  
Fang X., 1992, J MOL CATALYSIS CHIN, V6, P427
[10]  
Fang X., 1992, J MOL CATAL, V6, P255