Vapor phase methylation of pyridine with CO-H2 over metal catalysts

被引:5
作者
Fujita, S [1 ]
Hiyoshi, N [1 ]
Takezawa, N [1 ]
机构
[1] Hokkaido Univ, Grad Sch Engn, Div Engn & Mat Sci, Sapporo, Hokkaido 0608628, Japan
关键词
methylation of pyridine; formation of methylpyridine; formation of dimethylpyridine; CO methanation; metal catalysts;
D O I
10.1016/S0926-860X(99)00189-1
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 title reaction was carried out over Ni, Ni/SiO2, Ni/Al2O3, Ni/ZrO2, Ni/MgO, Co/SiO2, Ru/SiO2, Rh/SiO2, Pt/SiO2 and Pd/SiO2 catalysts. Over Ni, Ni/SiO2, Ni/Al2O3, Ni/ZrO2 and Ni/MgO, 2-methylpyridine is produced with high selectivity along with small amounts of 2,6-dimethylpyridine and methane. Methylation occurs selectively at carbon atoms adjacent to a nitrogen atom. The order of the catalytic activity is Ni/Al2O3 > Ni/ZrO2 > Ni > Ni/SiO2 > Ni/MgO. It was found that 2,6-dimethylpyridine is produced via methylation of 2-methylpyridine, and that methylation of pyridine with CO-H-2 and CO methanation are parallel reactions. CHx species produced from CO-H-2 are consumed effectively for methylation of pyridine. Over Co/SiO2 and Ru/SiO2, although methylation occurs, the yield is very low. Over Rh/SiO2, Pt/SiO2 and Pd/SiO2, methylation is not observed. Differences in the yields of the catalysts are discussed. (C) 1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:323 / 327
页数:5
相关论文
共 31 条
[1]  
BAKER JA, 1980, J CATAL, V78, P165
[2]   FORMATION OF METHYLENE INTERMEDIATES BY HYDROGENATION OF SURFACE CARBON ON RU(001) [J].
BARTEAU, MA ;
FEULNER, P ;
STENGL, R ;
BROUGHTON, JQ ;
MENZEL, D .
JOURNAL OF CATALYSIS, 1985, 94 (01) :51-59
[3]   LOW-TEMPERATURE CATALYTIC HOMOLOGATION OF METHANE ON PLATINUM, RUTHENIUM AND COBALT [J].
BELGUED, M ;
AMARIGLIO, H ;
PAREJA, P ;
AMARIGLIO, A ;
SAINTJUST, J .
CATALYSIS TODAY, 1992, 13 (2-3) :437-445
[4]   INCORPORATION OF SURFACE CARBON INTO HYDROCARBONS DURING FISCHER-TROPSCH SYNTHESIS - MECHANISTIC IMPLICATIONS [J].
BILOEN, P ;
HELLE, JN ;
SACHTLER, WMH .
JOURNAL OF CATALYSIS, 1979, 58 (01) :95-107
[5]   ELECTRON SPECTROSCOPIC STUDIES OF PYRIDINE ON METAL-SURFACES [J].
BRIDGE, ME ;
CONNOLLY, M ;
LLOYD, DR ;
SOMERS, J ;
JAKOB, P ;
MENZEL, D .
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY, 1987, 43 (12) :1473-1478
[6]   HREELS, ARUPS AND XPS OF PYRIDINE ON NI(110) [J].
COHEN, MR ;
MERRILL, RP .
SURFACE SCIENCE, 1991, 245 (1-2) :1-11
[7]   CHEMISORBED PYRIDINE ON NI(001) - A HIGH-RESOLUTION ELECTRON-ENERGY LOSS STUDY OF VIBRATIONAL AND ELECTRONIC EXCITATIONS [J].
DINARDO, NJ ;
AVOURIS, P ;
DEMUTH, JE .
JOURNAL OF CHEMICAL PHYSICS, 1984, 81 (04) :2169-2180
[8]   EVIDENCE FOR INTERMEDIATES INVOLVED IN FISCHER-TROPSCH SYNTHESIS OVER RU [J].
EKERDT, JG ;
BELL, AT .
JOURNAL OF CATALYSIS, 1980, 62 (01) :19-25
[9]   CATALYTIC REACTION OF METHANE WITH CARBON-DIOXIDE OVER SUPPORTED PALLADIUM [J].
ERDOHELYI, A ;
CSERENYI, J ;
PAPP, E ;
SOLYMOSI, F .
APPLIED CATALYSIS A-GENERAL, 1994, 108 (02) :205-219
[10]   EVIDENCE FOR CHX SURFACE SPECIES AFTER THE HYDROGENATION OF CO OVER AN FE(110) SINGLE-CRYSTAL SURFACE [J].
ERLEY, W ;
MCBREEN, PH ;
IBACH, H .
JOURNAL OF CATALYSIS, 1983, 84 (01) :229-234