CATALYTIC REACTION OF METHANE WITH CARBON-DIOXIDE OVER SUPPORTED PALLADIUM

被引:164
作者
ERDOHELYI, A
CSERENYI, J
PAPP, E
SOLYMOSI, F
机构
[1] ATTILA JOZSEF UNIV,INST SOLID STATE & RADIOCHEM,POB 168,H-6701 SZEGED,HUNGARY
[2] HUNGARIAN ACAD SCI,REACT KINET RES GRP,H-6701 SZEGED,HUNGARY
基金
匈牙利科学研究基金会;
关键词
CARBON DIOXIDE HYDROGENATION; KINETICS; METHANE REFORMING; PALLADIUM;
D O I
10.1016/0926-860X(94)85071-2
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
The reforming of methane with carbon dioxide has been investigated at 673-773 K on supported palladium catalysts in a fixed-bed continuous-flow reactor. In addition, the dissociation of carbon dioxide and methane, and the reactivity of die surface carbon formed have also been examined. The dissociation of carbon dioxide, detected by infrared spectroscopy, occurred at the lowest temperature, 373 K, on Pd/TiO2. It was greatly promoted by the presence of methane. The decomposition of methane at the temperature of the CH4 + CO2 reaction (ca. 773 K) proceeded initially at a high rate yielding hydrogen and small amounts of ethane and ethene. The deposition of surface carbon was also observed, which was hydrogenated only above 720 K. The reaction between carbon dioxide and methane occurred rapidly above 673 K to give carbon monoxide and hydrogen with a ratio of 1.3-1.7. Very little carbon was deposited during the reaction of a stoichiometric gas mixture. Kinetic parameters of the reaction were determined and a possible reaction mechanism is proposed.
引用
收藏
页码:205 / 219
页数:15
相关论文
共 32 条
[1]   PARTIAL OXIDATION OF METHANE TO SYNTHESIS GAS-USING CARBON-DIOXIDE [J].
ASHCROFT, AT ;
CHEETHAM, AK ;
GREEN, MLH ;
VERNON, PDF .
NATURE, 1991, 352 (6332) :225-226
[2]  
AYERS WM, 1988, ACS S SER AM CHEM SO
[3]  
BEEBE TP, 1986, SURF SCI, V173, pL606, DOI 10.1016/0039-6028(86)90186-X
[4]  
BIBBY DM, 1988, STUDIES SURFACE SCI, V36
[5]   CHEMISORPTION OF CARBON-MONOXIDE ON PALLADIUM SINGLE-CRYSTAL SURFACES - IR SPECTROSCOPIC EVIDENCE FOR LOCALIZED SITE ADSORPTION [J].
BRADSHAW, AM ;
HOFFMANN, FM .
SURFACE SCIENCE, 1978, 72 (03) :513-535
[6]   EFFECTS OF SUPPORT ON THE ADSORPTION AND DISSOCIATION OF CO AND ON THE REACTIVITY OF SURFACE CARBON ON RH CATALYSTS [J].
ERDOHELYI, A ;
SOLYMOSI, F .
JOURNAL OF CATALYSIS, 1983, 84 (02) :446-460
[7]   CATALYTIC-HYDROGENATION OF CO2 OVER SUPPORTED PALLADIUM [J].
ERDOHELYI, A ;
PASZTOR, M ;
SOLYMOSI, F .
JOURNAL OF CATALYSIS, 1986, 98 (01) :166-177
[8]   ACTIVATION OF CH4 AND ITS REACTION WITH CO2 OVER SUPPORTED RH CATALYSTS [J].
ERDOHELYI, A ;
CSERENYI, J ;
SOLYMOSI, F .
JOURNAL OF CATALYSIS, 1993, 141 (01) :287-299
[9]   EFFECTS OF METAL SUPPORT INTERACTIONS ON THE CHEMISORPTION OF H-2 AND CO ON PD/SIO2 AND PD/LA2O3 [J].
HICKS, RF ;
YEN, QJ ;
BELL, AT .
JOURNAL OF CATALYSIS, 1984, 89 (02) :498-510
[10]  
LUNSFORD JH, 1993, 10TH P INT C CAT BUD, P103