Use of hydrotalcites as catalytic precursors of multimetallic mixed oxides.: Application in the hydrogenation of acetylene

被引:53
作者
Monzón, A [1 ]
Romeo, E
Royo, C
Trujillano, R
Labajos, FM
Rives, V
机构
[1] Univ Zaragoza, Dept Ingn Quim & Tecnol Medio Ambiente, E-50009 Zaragoza, Spain
[2] Univ Salamanca, Dept Quim Inorgan, E-37008 Salamanca, Spain
关键词
Ni catalysts; selective hydrogenation of acetylene; spinel; hydrotalcite; ZnO; support modification; coke formation; coking kinetic modelling;
D O I
10.1016/S0926-860X(99)00101-5
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 effect of the Ni/Zn molar ratio on the activity, selectivity, and coke formation of NiO . ZnO . Al2O3 catalysts (modified with Fe3+ or Cr3+) during acetylene hydrogenation has been studied. Coke formation is decreased significantly in the presence of ZnO, and a similar effect is also found when the catalysts are doped with Cr3+ instead of with Fe3+. An optimum Ni/Zn ratio for activity, selectivity and coke formation performance has been found. The existence of this maximum implies the necessity of adding ZnO to the support in order to modulate the catalytic properties of Ni. Furthermore, if the Ni concentration is increased, the conversion, selectivity, and yield to ethylene not only fails to increase, but actually decreases, while coke formation simultaneously increases. The existence of the above-mentioned optimum is the consequence of a minimum concentration of the hydrogenolytic (naked) metallic sites, the majority being hydrogenating metallic sites covered by a monolayer of ethylidines. A kinetic model of coke growth is proposed assuming the existence of two types of coke associated with the hydrogenolitic and hydrogenating sites respectively. (C) 1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:53 / 63
页数:11
相关论文
共 49 条
[1]   STEAM REFORMING OF METHANE ON REDUCED NON-STOICHIOMETRIC NICKEL ALUMINATE CATALYSTS [J].
ALUBAID, A ;
WOLF, EE .
APPLIED CATALYSIS, 1988, 40 (1-2) :73-85
[2]   COPRECIPITATED NICKEL-ALUMINA CATALYSTS FOR METHANATION AT HIGH-TEMPERATURE .2. VARIATION OF TOTAL AND METALLIC AREAS AS A FUNCTION OF SAMPLE COMPOSITION AND METHOD OF PRETREATMENT [J].
ALZAMORA, LE ;
ROSS, JRH ;
KRUISSINK, EC ;
VANREIJEN, LL .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1981, 77 :665-681
[3]   Reduction of 4-nitrotoluene over Fe-Mg-Al lamellar double hydroxides [J].
Auer, SM ;
Grunwaldt, JD ;
Köppel, RA ;
Baiker, A .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1999, 139 (2-3) :305-313
[4]  
BHATTACHARYYA A, 1994, STUD SURF SCI CATAL, V88, P207
[5]   Catalytic reforming of methane with carbon dioxide over nickel catalysts .1. Catalyst characterization and activity [J].
Bradford, MCJ ;
Vannice, MA .
APPLIED CATALYSIS A-GENERAL, 1996, 142 (01) :73-96
[6]   HYDROTALCITE-TYPE ANIONIC CLAYS: PREPARATION, PROPERTIES AND APPLICATIONS [J].
Cavani, F. ;
Trifiro, F. ;
Vaccari, A. .
CATALYSIS TODAY, 1991, 11 (02) :173-301
[7]   CONVERSION OF METHANE AND CARBON-DIOXIDE INTO SYNTHESIS GAS OVER ALUMINA-SUPPORTED NICKEL-CATALYSTS - EFFECT OF NI-AL2O3 INTERACTIONS [J].
CHEN, YG ;
REN, J .
CATALYSIS LETTERS, 1994, 29 (1-2) :39-48
[8]   PREPARATION AND CHARACTERIZATION OF NICKEL ALUMINUM MIXED OXIDES OBTAINED BY THERMAL-DECOMPOSITION OF HYDROTALCITE-TYPE PRECURSORS [J].
CLAUSE, O ;
REBOURS, B ;
MERLEN, E ;
TRIFIRO, F ;
VACCARI, A .
JOURNAL OF CATALYSIS, 1992, 133 (01) :231-246
[9]   C-1-C-6 ALCOHOLS FROM SYNTHESIS GAS ON COPPER COBALT CATALYSTS [J].
COURTY, P ;
DURAND, D ;
FREUND, E ;
SUGIER, A .
JOURNAL OF MOLECULAR CATALYSIS, 1982, 17 (2-3) :241-254
[10]  
COURTY P, 1983, STUD SURF SCI CATAL, V16, P485