PREPARATION AND FISCHER-TROPSCH REACTION OF HIGHLY-REDUCED COBALT CLUSTERS IN COBALT-EXCHANGED ZEOLITE

被引:9
作者
CHUNG, JS
YUN, HG
KOH, DJ
KIM, YG
机构
[1] Department of Chemical Engineering, Pohang Institute of Science and Technology (POSTECH/RIST), P.O. Box 125
来源
JOURNAL OF MOLECULAR CATALYSIS | 1993年 / 79卷 / 1-3期
关键词
ALKALI IMPREGNATION; COBALT CLUSTERS; FISCHER-TROPSCH REACTION; ZEOLITE;
D O I
10.1016/0304-5102(93)85102-Y
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
Impregnation of 3-5 M NaOH solution into cobalt ion-exchanged Y zeolite using the incipient wetness method enables the preparation of highly reduced cobalt clusters entrapped inside zeolite pores after the catalyst is reduced with hydrogen gas. TEM and ferromagnetic resonance experiments reveal that the cobalt clusters are extremely small and uniform in size. Reaction measurements on these catalysts show an enhanced production of linear forms of hydrocarbons such as 1-olefins and n-paraffins. The catalysts also exhibit a bimodal distribution in the selectivity pattern in which one maximum is observed at C6 with another at C-16. The formation of high-order linear hydrocarbons above C-10 is attributed to an increased chance for the chain growth owing to a hold-up effect of reaction intermediates, especially 1-olefins, which are accumulated deep inside zeolite pores during the reaction. The accumulated amount of hydrocarbon products, ranging from C1-C18, was found to be 2.3 X 10(-3) mol/g cat (about 10 vol.% of total pore volume in zeolite crystallite when the average density is assumed to be that of C-12) after reaction for 10 h. The formation of hydrocarbon isomers is related with acidic sites on the exterior surface of the zeolite particle.
引用
收藏
页码:199 / 215
页数:17
相关论文
共 27 条
[1]   SMALL PARTICLES IN ZEOLITES AS SELECTIVE CATALYSTS FOR THE HYDROCONDENSATION OF CARBON-MONOXIDE [J].
BALLIVETTKATCHENKO, D ;
TKATCHENKO, I .
JOURNAL OF MOLECULAR CATALYSIS, 1981, 13 (01) :1-10
[2]   IRON ALLOY FISCHER-TROPSCH CATALYSTS .6. FECO ON ZSM-5 [J].
BUTT, JB ;
LIN, TA ;
SCHWARTZ, LH .
JOURNAL OF CATALYSIS, 1986, 97 (01) :261-263
[3]  
CULLITY BD, 1972, INTRO MAGNETIC MAT, P414
[4]   DIFFUSION OF LINEAR PARAFFINS AND CYCLOHEXANE IN NAX AND 5A ZEOLITE CRYSTALS [J].
EIC, M ;
RUTHVEN, DM .
ZEOLITES, 1988, 8 (06) :472-479
[5]   SHAPE-SELECTIVE FISCHER-TROPSCH SYNTHESIS CATALYZED BY ZEOLITE-ENTRAPPED COBALT CLUSTERS [J].
FRAENKEL, D ;
GATES, BC .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1980, 102 (07) :2478-2480
[6]   STRUCTURE SENSITIVITY AND ITS EFFECTS ON PRODUCT DISTRIBUTION IN CO HYDROGENATION ON COBALT ALUMINA [J].
FU, L ;
BARTHOLOMEW, CH .
JOURNAL OF CATALYSIS, 1985, 92 (02) :376-387
[7]   CRYSTAL-STRUCTURE OF CO2+ EXCHANGED Y-TYPE ZEOLITES [J].
GALLEZOT, P ;
IMELIK, B .
JOURNAL DE CHIMIE PHYSIQUE ET DE PHYSICO-CHIMIE BIOLOGIQUE, 1974, 71 (02) :155-163
[8]   REDUCTION OF SUPPORTED IRON CATALYSTS STUDIED BY MOSSBAUER-SPECTROSCOPY [J].
HUANG, YY ;
ANDERSON, JR .
JOURNAL OF CATALYSIS, 1975, 40 (02) :143-153
[9]   CATALYSIS BY SUPPORTED CLUSTERS - CHARACTERIZATION OF HIGHLY DISPERSED ZEROVALENT IRON COVERED WITH DISSOCIATED CO OBTAINED BY THERMAL-DECOMPOSITION OF [HFE3(CO)11]- AND FE3(CO)12 SUPPORTED ON MAGNESIA [J].
HUGUES, F ;
DALMON, JA ;
BUSSIERE, P ;
SMITH, AK ;
BASSET, JM ;
OLIVIER, D .
JOURNAL OF PHYSICAL CHEMISTRY, 1982, 86 (26) :5136-5144
[10]   METALLIC COBALT AND IRON PARTICLES IN LARGE AND MEDIUM PORE ZEOLITES - METHODS OF GENERATION AND FERROMAGNETIC-RESONANCE CHARACTERIZATION [J].
ITON, LE ;
BEAL, RB ;
HAMOT, PJ .
JOURNAL OF MOLECULAR CATALYSIS, 1984, 27 (1-2) :95-109