Partial oxidation of methane to syngas over Ni/MgO, Ni/CaO and Ni/CeO2

被引:142
作者
Tang, S [1 ]
Lin, J [1 ]
Tan, KL [1 ]
机构
[1] Natl Univ Singapore, Dept Phys, Surface Sci Lab, Singapore 119260, Singapore
关键词
partial oxidation of methane (POM); syngas; nickel catalyst; carbon deposition;
D O I
10.1023/A:1019034412036
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
Partial oxidation of methane to syngas at atmospheric pressure and 750 degrees C was examined over Ni/MgO, Ni/CaO and Ni/CeO2 catalysts with nickel loading of 13 wt%. All catalysts had similar high conversion of methane and high selectivity to syngas, which nearly approached the values predicted by thermodynamic equilibrium. However, only Ni/MgO showed high resistance to carbon deposition under thermodynamically severe conditions (CH4/O-2 = 2.5, a higher CH4 to O-2 ratio than the stoichiometric ratio). Its catalytic activity remained stable during 100 h of reaction, with no detectable carbon deposition. The oxidation of carbon deposited from pure CH4 decomposition and from pure CO disproportionation was investigated by in situ TFO-MS study which showed that both were effectively inhibited over Ni/MgO. In addition, the catalysts were characterized by TPR, XRD and XPS. It was revealed that the excellent performance of Ni/MgO resulted from the formation of an ideal solid solution between NiO and MgO.
引用
收藏
页码:169 / 175
页数:7
相关论文
共 35 条
[1]   MAGNESIA-SUPPORTED NICKEL-CATALYSTS .1. FACTORS AFFECTING THE STRUCTURE AND MORPHOLOGICAL PROPERTIES [J].
ARENA, F ;
HORRELL, BA ;
COCKE, DL ;
PARMALIANA, A ;
GIORDANO, N .
JOURNAL OF CATALYSIS, 1991, 132 (01) :58-67
[2]   SELECTIVE OXIDATION OF METHANE TO SYNTHESIS GAS-USING TRANSITION-METAL CATALYSTS [J].
ASHCROFT, AT ;
CHEETHAM, AK ;
FOORD, JS ;
GREEN, MLH ;
GREY, CP ;
MURRELL, AJ ;
VERNON, PDF .
NATURE, 1990, 344 (6264) :319-321
[3]   SELECTIVE OXIDATION OF METHANE TO CARBON-MONOXIDE ON SUPPORTED PALLADIUM CATALYST [J].
BHATTACHARYA, AK ;
BREACH, JA ;
CHAND, S ;
GHORAI, DK ;
HARTRIDGE, A ;
KEARY, J ;
MALLICK, KK .
APPLIED CATALYSIS A-GENERAL, 1992, 80 (01) :L1-L5
[4]   Catalytic reforming of methane with carbon dioxide over nickel catalysts .1. Catalyst characterization and activity [J].
Bradford, MCJ ;
Vannice, MA .
APPLIED CATALYSIS A-GENERAL, 1996, 142 (01) :73-96
[5]   SELECTIVE OXIDATION OF METHANE TO CO AND H2 OVER UNREDUCED NIO-RARE EARTH OXIDE CATALYSTS [J].
CHOUDHARY, VR ;
RANE, VH ;
RAJPUT, AM .
CATALYSIS LETTERS, 1993, 22 (04) :289-297
[6]   LOW-TEMPERATURE OXIDATIVE CONVERSION OF METHANE TO SYNGAS OVER NIO-CAO CATALYST [J].
CHOUDHARY, VR ;
RAJPUT, AM ;
PRABHAKAR, B .
CATALYSIS LETTERS, 1992, 15 (04) :363-370
[7]   SELECTIVE OXIDATION OF METHANE TO CO AND H2 OVER NI/MGO AT LOW-TEMPERATURES [J].
CHOUDHARY, VR ;
MAMMAN, AS ;
SANSARE, SD .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION IN ENGLISH, 1992, 31 (09) :1189-1190
[8]   Oxidative conversion of methane to syngas over LaNiO3 perovskite with or without simultaneous steam and CO2 reforming reactions: Influence of partial substitution of La and Ni [J].
Choudhary, VR ;
Uphade, BS ;
Belhekar, AA .
JOURNAL OF CATALYSIS, 1996, 163 (02) :312-318
[9]   A STUDY OF CARBON DEPOSITION ON CATALYSTS DURING THE PARTIAL OXIDATION OF METHANE TO SYNTHESIS GAS [J].
CLARIDGE, JB ;
GREEN, MLH ;
TSANG, SC ;
YORK, APE ;
ASHCROFT, AT ;
BATTLE, PD .
CATALYSIS LETTERS, 1993, 22 (04) :299-305
[10]   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