Partial oxidation of methane to synthesis gas over MgO-supported Rh catalysts: the effect of precursor of MgO

被引:65
作者
Ruckenstein, E [1 ]
Wang, HY [1 ]
机构
[1] SUNY Buffalo, Dept Chem Engn, Buffalo, NY 14260 USA
关键词
methane partial oxidation; syngas; Rh catalyst; MgO;
D O I
10.1016/S0926-860X(99)00495-0
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
Five magnesium-containing precursors were used to prepare magnesium oxides of different surface areas. With these oxides as supports, catalysts (1 wt.% Rh loading) with different Rh dispersions after reduction were prepared. At a T-furnace of 750 degrees C and 1 atm, all these catalysts provided a conversion >80% and selectivities of 95-96% to CO and 96-98% to H-2, at the high space velocity of 7.2 x 10(5) ml g(-1) h(-1), with very high stability. No significant deactivation of the catalyst was observed for up to 96 h of reaction. However, no notable effect of the precursor of MgO was noted and possible explanations are provided. Temperature-programmed reduction (TPR) experiments indicated the presence of up to three kinds of rhodium-containing species, Rh2O3, Rh2O3-interacting with the support, and MgRh2O4, in the oxidized MgO-supported Rh catalysts. The strong interactions between rhodium and magnesium oxides are suggested to be responsible for the high stability of the catalyst. It was found that the methane conversion increased with the amount of catalyst when it was below 5.0 mg, but remained almost unchanged when it was greater than 5.0 mg. The catalytic assays also provided some information about the reaction mechanism. (C) 2000 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:33 / 41
页数:9
相关论文
共 20 条
[1]   HEAT-TRANSPORT LIMITATIONS AND REACTION SCHEME OF PARTIAL OXIDATION OF METHANE TO SYNTHESIS GAS OVER SUPPORTED RHODIUM CATALYSTS [J].
BOUCOUVALAS, Y ;
ZHANG, ZL ;
VERYKIOS, XE .
CATALYSIS LETTERS, 1994, 27 (1-2) :131-142
[2]   An investigation of the use of zirconia as a support for rhodium catalysts [J].
Burch, R ;
Loader, PK .
APPLIED CATALYSIS A-GENERAL, 1996, 143 (02) :317-335
[3]   ARE THE EQUILIBRIUM CONCENTRATIONS OF CO AND H-2 EXCEEDED DURING THE OXIDATION OF CH4 OVER A NI/YB2O3 CATALYST [J].
DISSANAYAKE, D ;
ROSYNEK, MP ;
LUNSFORD, JH .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (15) :3644-3646
[4]   PARTIAL OXIDATION OF METHANE TO CARBON-MONOXIDE AND HYDROGEN OVER A NI/AL2O3 CATALYST [J].
DISSANAYAKE, D ;
ROSYNEK, MP ;
KHARAS, KCC ;
LUNSFORD, JH .
JOURNAL OF CATALYSIS, 1991, 132 (01) :117-127
[5]   Redox behavior of high surface area Rh-loaded Ce0.5Zr0.5O2 mixed oxide [J].
Fornasiero, P ;
Kaspar, J ;
Graziani, M .
JOURNAL OF CATALYSIS, 1997, 167 (02) :576-580
[6]   SYNTHESIS GAS-FORMATION BY DIRECT OXIDATION OF METHANE OVER RH MONOLITHS [J].
HICKMAN, DA ;
HAUPFEAR, EA ;
SCHMIDT, LD .
CATALYSIS LETTERS, 1993, 17 (3-4) :223-237
[7]   SYNTHESIS GAS-FORMATION BY DIRECT OXIDATION OF METHANE OVER PT MONOLITHS [J].
HICKMAN, DA ;
SCHMIDT, LD .
JOURNAL OF CATALYSIS, 1992, 138 (01) :267-282
[8]   PRODUCTION OF SYNGAS BY DIRECT CATALYTIC-OXIDATION OF METHANE [J].
HICKMAN, DA ;
SCHMIDT, LD .
SCIENCE, 1993, 259 (5093) :343-346
[9]   PULSE-MS STUDY OF THE PARTIAL OXIDATION OF METHANE OVER NI/LA2O3 CATALYST [J].
HU, YH ;
RUCKENSTEIN, E .
CATALYSIS LETTERS, 1995, 34 (1-2) :41-50
[10]   Rhodium-oxide species formed on progressive oxidation of rhodium clusters dispersed on alumina [J].
Hwang, CP ;
Yeh, CT ;
Zhu, QM .
CATALYSIS TODAY, 1999, 51 (01) :93-101