Stability of supported transition metal catalysts in the hydrogenation of nitriles

被引:52
作者
Huang, YY [1 ]
Adeeva, V [1 ]
Sachtler, WMH [1 ]
机构
[1] Northwestern Univ, Ctr Catalysis & Surface Sci, VN Ipatieff Lab, Evanston, IL 60201 USA
关键词
acetonitrile hydrogenation; butyronitrile hydrogenation; transition metals; metal agglomeration; overlayer formation;
D O I
10.1016/S0926-860X(99)00457-3
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
Gas phase hydrogenation of acetonitrile and butyronitrile over supported transition metal catalysts was carried out in a gas phase microflow reactor at 1 and 10 bar; butyronitrile was also hydrogenated in a stirred autoclave at an initial pressure of 24 bar Catalyst stability is higher in the Liquid phase than in the gas phase operation, suggesting desorption of site blocking molecules into the liquid. Agglomeration of metal particles has been detected by TEM and EDX; with Pt/NaY it starts at 110 degrees C, with Ru/NaY it is obvious at 160 degrees C. Metal agglomeration and formation of an overlayer contribute to catalyst deactivation. Ru/zeolite catalysts are more active than Ru/Al2O3, both in the gas and the liquid phase. No significant effect of support acidity on the selectivity of the reaction has been detected; the results give no indication of carbide or nitrile formation as major causes of catalyst deactivation. (C) 2000 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:73 / 85
页数:13
相关论文
共 37 条
[11]   FLASH DECOMPOSITION OF ETHYLENE AND ACETYLENE ON IRIDIUM [J].
HANSEN, RS ;
ARTHUR, JR ;
MIMEAULT, VJ ;
RYE, RR .
JOURNAL OF PHYSICAL CHEMISTRY, 1966, 70 (09) :2787-&
[12]   GAS-PHASE HYDROGENATION OF ACETONITRILE ON RANEY-NICKEL CATALYSTS - REACTIVE HYDROGEN [J].
HOCHARD, F ;
JOBIC, H ;
MASSARDIER, J ;
RENOUPREZ, AJ .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1995, 95 (02) :165-172
[13]   ENANTIOSELECTIVITY OF NICKEL CATALYSTS MODIFIED WITH TARTARIC ACID OR NICKEL TARTRATE COMPLEXES [J].
HOEK, A ;
SACHTLER, WMH .
JOURNAL OF CATALYSIS, 1979, 58 (02) :276-286
[14]  
HOEK A, 1981, P 7 INT C CAT TOK 19, P376
[15]   Concerted reaction mechanism in deuteration and H/D exchange of nitriles over transition metals [J].
Huang, YY ;
Sachtler, WMH .
JOURNAL OF CATALYSIS, 1999, 184 (01) :247-261
[16]   H/D exchange of amines and acetonitrile over transition metal catalysts [J].
Huang, YY ;
Sachtler, WMH .
JOURNAL OF PHYSICAL CHEMISTRY B, 1998, 102 (34) :6558-6565
[17]  
HUANG YY, IN PRESS J CATAL
[18]   HYDROGEN RELEASE FROM Ni/FAUJASITE CATALYSTS [J].
Jiang, H. J. ;
Tzou, M. S. ;
Sachtler, W. H. M. .
CATALYSIS LETTERS, 1988, 1 (04) :99-107
[19]  
KINDLER K, 1933, ARCH PHARM, V27, P439
[20]  
KOBYLINSKI TP, 1974, T SOC AUTO ENG, V83, P1089