Transient response study of the ammoxidation of propene and propane on an Sb-V-oxide catalyst

被引:15
作者
Nilsson, R [1 ]
Andersson, A [1 ]
机构
[1] LUND UNIV,CTR CHEM,DEPT CHEM ENGN 2,S-22100 LUND,SWEDEN
关键词
D O I
10.1021/ie970226j
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
The reaction pathways in the ammoxidation of propene and of propane over an Sb-V-oxide catalyst were studied by analyzing the modes of transient responses of reactants and products resulting from step changes from inert gas to reactant feed. The pathway from propane to acrylonitrile begins with the oxidative dehydrogenation of propane to form propene. After readsorption, the propene is then transformed into adsorbed acrolein, which eventually reacts with an NHx surface species to form acrylonitrile. The adsorption of propane is rate limiting for the propane conversion, but the desorption of water formed from the propene is slow and determines the product distribution. The response modes for the direct oxidation and ammoxidation of propene are consistent with the desorption of water being rate limiting. A comparison of the experimental responses viith responses simulated under the assumption that the formation of an allylic intermediate is rate determining reveals an important difference in profiles, indicating this step to not be rate determining. The results show that substantial qualitative information concerning the reaction pathways can be obtained from the analysis of transient profile modes.
引用
收藏
页码:5207 / 5219
页数:13
相关论文
共 31 条
[1]   MECHANISM STUDIES OF THE CATALYTIC OXIDATION OF PROPYLENE [J].
ADAMS, CR ;
JENNINGS, TJ .
JOURNAL OF CATALYSIS, 1964, 3 (06) :549-558
[2]  
ANDERSSON A, 1985, ADSORPTION CATALYSIS, V21, P381
[3]   TRANSIENT METHOD AND ELEMENTARY STEPS IN HETEROGENEOUS CATALYSIS [J].
BENNETT, CO .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1976, 13 (02) :121-148
[4]  
BRAZDIL JR, 1989, Patent No. 4871706
[5]   Kinetic isotope effect in the ammoxidation of propane over an alumina supported vanadium antimony oxide catalyst [J].
Brazdil, LC ;
Ebner, AM ;
Brazdil, JF .
JOURNAL OF CATALYSIS, 1996, 163 (01) :117-121
[6]  
Buchholz SA, 1996, ACS SYM SER, V638, P259
[7]   SURFACE INTERMEDIATES IN SELECTIVE PROPYLENE OXIDATION AND AMMOXIDATION OVER HETEROGENEOUS MOLYBDATE AND ANTIMONATE CATALYSTS [J].
BURRINGTON, JD ;
KARTISEK, CT ;
GRASSELLI, RK .
JOURNAL OF CATALYSIS, 1984, 87 (02) :363-380
[8]   KINETICS AND REACTION NETWORK IN PROPANE AMMOXIDATION TO ACRYLONITRILE ON V-SB-AL BASED MIXED OXIDES [J].
CATANI, R ;
CENTI, G ;
TRIFIRO, F ;
GRASSELLI, RK .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1992, 31 (01) :107-119
[9]   MODIFICATION OF THE SURFACE REACTIVITY OF VANADIUM ANTIMONATE CATALYSTS DURING CATALYTIC PROPANE AMMOXIDATION [J].
CENTI, G ;
PERATHONER, S .
APPLIED CATALYSIS A-GENERAL, 1995, 124 (02) :317-337
[10]   Surface chemistry of V-Sb-oxide in relation to the mechanism of acrylonitrile synthesis from propane .1. Chemisorption and transformation of possible intermediates [J].
Centi, G ;
Marchi, F ;
Perathoner, S .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1996, 92 (24) :5141-5149