Influence of syngas composition on the transient behavior of a Fischer-Tropsch continuous slurry reactor

被引:31
作者
Bremaud, M
Fongarland, P
Anfray, J
Jallais, S
Schweich, D
Khodakov, AY
机构
[1] Univ Sci & Tech Lille Flandres Artois, Lab Catalyse Lille, F-59655 Villeneuve Dascq, France
[2] Lab Genie Proc Catalyt, F-69616 Villeurbanne, France
[3] AIR LIQUIDE, CRCD, F-78354 Jouy En Josas, France
关键词
syngas; Fischer-Tropsch; slurry; CATALYSTS; WATER; DEACTIVATION; KINETICS;
D O I
10.1016/j.cattod.2005.07.126
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The influence of syngas composition on the initial behaviour of a Co/Al2O3 catalyst in Fischer-Tropsch reaction has been studied in a continuous perfectly mixed slurry reactor for an inlet H-2/CO ratio between 1.6 and 3.35 keeping other conditions constant (T = 220 degrees C, P = 2 MPa). Significantly different behaviors of initial deactivation for CO conversion have been observed with different H-2/CO ratios. It was observed that the deactivation increases with increase in H-2/CO ratio and in carbon monoxide conversion. The computed liquid concentrations of CO, H-2 and H2O have shown that water is the most abundant species in the liquid phase of the reactor during our experiments. The concentration of the water produced by the FT reaction seems to be the key parameter responsible of the initial behavior and then of the initial deactivation. For moderate levels of water (C-H2O(L)/C-H2(L) < 4 corresponding to P-H2O/P-H2 < 0.4), a simple kinetic model assuming a reversible oxidation of cobalt active sites by water in competition with their reduction by hydrogen seems to represent satisfactorily the initial behaviour of the catalyst. For higher water concentrations, the irreversible deactivation should be probably taken into consideration. (c) 2005 Elsevier B.V. All rights reserved.
引用
收藏
页码:137 / 142
页数:6
相关论文
共 13 条
[1]  
[Anonymous], 1990, Chemical Reactor Analysis and Design
[2]   The application of Mossbauer emission spectroscopy to industrial cobalt based Fischer-Tropsch catalysts [J].
Crajé, MWJ ;
van der Kraan, AM ;
van de Loosdrecht, J ;
van Berge, PJ .
CATALYSIS TODAY, 2002, 71 (3-4) :369-379
[3]   Study of the effect of water on alumina supported cobalt Fischer-Tropsch catalysts [J].
Hilmen, AM ;
Schanke, D ;
Hanssen, KF ;
Holmen, A .
APPLIED CATALYSIS A-GENERAL, 1999, 186 (1-2) :169-188
[4]   Fischer-Tropsch synthesis XAFS XAFS studies of the effect of water on a Pt-promoted Co/Al2O3 catalyst [J].
Jacobs, G ;
Das, TK ;
Patterson, PM ;
Li, JL ;
Sanchez, L ;
Davis, BH .
APPLIED CATALYSIS A-GENERAL, 2003, 247 (02) :335-343
[5]   Fischer-Tropsch synthesis:: effect of water on the deactivation of Pt promoted Co/Al2O3 catalysts [J].
Li, JL ;
Zhan, XD ;
Zhang, YQ ;
Jacobs, G ;
Das, T ;
Davis, BH .
APPLIED CATALYSIS A-GENERAL, 2002, 228 (1-2) :203-212
[6]   Characterization of Fischer-Tropsch liquids for vapor-liquid equilibria calculations [J].
Marano, JJ ;
Holder, GD .
FLUID PHASE EQUILIBRIA, 1997, 138 (1-2) :1-21
[7]   Wax composition transients during Fischer-Tropsch synthesis [J].
Pinna, D ;
Tronconi, E ;
Lietti, L ;
Zennaro, R ;
Forzatti, P .
JOURNAL OF CATALYSIS, 2003, 214 (02) :251-260
[8]   Modeling of surface structure of supported catalysts. Application to deactivation of FT reactors [J].
Qin, Q ;
Ramkrishna, D .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2004, 43 (12) :2912-2921
[9]   The effect of water on cobalt Fischer-Tropsch catalysts studied by steady-state isotopic transient kinetic analysis (SSITKA) [J].
Rothaemel, M ;
Hanssen, KF ;
Blekkan, EA ;
Schanke, D ;
Holmen, A .
CATALYSIS TODAY, 1997, 38 (01) :79-84
[10]   Transient initial kinetic regimes of Fischer-Tropsch synthesis [J].
Schulz, H ;
Schaub, G ;
Claeys, M ;
Riedel, T .
APPLIED CATALYSIS A-GENERAL, 1999, 186 (1-2) :215-227