Methane partial oxidation over NiO MgO solid solution catalysts

被引:195
作者
Ruckenstein, E [1 ]
Hul, YH [1 ]
机构
[1] SUNY Buffalo, Dept Chem Engn, Amherst, NY 14260 USA
关键词
NiO MgO; solid solution; partial oxidation of methane; hot layer; mechanism of partial oxidation of methane;
D O I
10.1016/S0926-860X(99)00047-2
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 following issues regarding the partial oxidation of methane to synthesis gas, over NiO/MgO solid solution catalysts, at a very high space velocity of the feed gas (CH4/O-2=2/1, GHSV=720 000 cm(3)/g h), were investigated: (i) the effect of the solid solution formation between NiO and MgO on the reaction; (ii)the effect of the composition of the catalyst; and (iii) the reaction mechanism. It was found that the mechanical mixtures of NiO and MgO have low activity and selectivity; however, their activity and selectivity became higher with increasing calcination time, due to the formation of a NiO-MgO solid solution. In contrast, the solid solution catalysts prepared via impregnation provided high activity and selectivity, as well as high stability over a large range of NiO concentrations. However, the activity was low for too low concentrations of NiO in NiO/MgO and the catalyst was no longer stable for too high concentrations of NiO. By comparing, under the same reaction conditions, the rate of partial oxidation of methane for CH4/O-2=2/1 to that of the reforming reaction of a mixture CH4/H2O/ COP obtained from the former by complete combustion, one could conclude that the pyrolysis mechanism was dominant at 700 degrees C and 750 degrees C, but at 850 degrees C, the combustion reforming mechanism also played a part. (C) 1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:85 / 92
页数:8
相关论文
共 44 条
[1]   Partial oxidation of methane to synthesis gas on a Rh/TiO2 catalyst in a fast flow porous membrane reactor [J].
Alibrando, M ;
Hahm, HS ;
Wolf, EE .
CATALYSIS LETTERS, 1997, 49 (1-2) :1-12
[2]   CONVERSION OF METHANE BY OXIDATIVE COUPLING [J].
AMENOMIYA, Y ;
BIRSS, VI ;
GOLEDZINOWSKI, M ;
GALUSZKA, J ;
SANGER, AR .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1990, 32 (03) :163-227
[3]   Effect of calcination on the structure of Ni/MgO catalyst: An x-ray diffraction study [J].
Arena, F ;
Frusteri, F ;
Parmaliana, A ;
Plyasova, L ;
Shmakov, AN .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1996, 92 (03) :469-471
[4]   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
[5]   A theoretical investigation of methane dissociation on Rh(111) [J].
Au, CT ;
Liao, MS ;
Ng, CF .
CHEMICAL PHYSICS LETTERS, 1997, 267 (1-2) :44-50
[6]  
Bart J. C., 1987, CATAL TODAY, V2, P1
[7]   Potential of zeolite supported rhodium catalysts for the CO2 reforming of CH4 [J].
Bhat, RN ;
Sachtler, WMH .
APPLIED CATALYSIS A-GENERAL, 1997, 150 (02) :279-296
[8]   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
[9]   Partial oxidation of methane to synthesis gas via the direct reaction scheme over Ru/TiO2 catalyst [J].
Boucouvalas, Y ;
Zhang, ZL ;
Verykios, XE .
CATALYSIS LETTERS, 1996, 40 (3-4) :189-195
[10]   Primary reaction steps and active surface sites in the rhodium-catalyzed partial oxidation of methane to CO and H-2 [J].
Buyevskaya, OV ;
Walter, K ;
Wolf, D ;
Baerns, M .
CATALYSIS LETTERS, 1996, 38 (1-2) :81-88