Modeling heterogeneous and homogeneous reactions in the high-temperature catalytic combustion of methane

被引:34
作者
Goralski, CT [1 ]
Schmidt, LD [1 ]
机构
[1] Univ Minnesota, Dept Chem Engn & Mat Sci, Minneapolis, MN 55455 USA
关键词
methane catalysis; natural-gas conversion; catalytic combustion; short-contact-time reactor; reactor modeling;
D O I
10.1016/S0009-2509(99)00169-4
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
A high-temperature, short-contact-time catalytic methane combustor is modeled as a plug-flow tubular reactor including both homogeneous and heterogeneous chemistry. The gas-phase chemistry is modeled with GRI-mech 2.11 and the heterogeneous chemistry is modeled using an elementary 19-step mechanism for combustion of methane on platinum. Calculations are made at a variety of pressures, temperatures, compositions: and catalyst pore sizes to determine their effects on the reactor exhaust compositions. Comparisons are made between results for cases where only homogeneous chemistry is allowed, only heterogeneous chemistry is allowed, and where both mechanisms are allowed. II is found that the homogeneous chemistry in all cases is significantly inhibited by the heterogeneous chemistry, although alone each of these mechanisms takes place on similar time scales. This inhibition is a result of the adsorption of radical species from the gas phase to the surface of the catalyst, which prevents initiation df the gas-phase free-radical chain reactions. (C) 1999 Elsevier Science Ltd. All rights reserved.
引用
收藏
页码:5791 / 5807
页数:17
相关论文
共 12 条
[1]   VODE - A VARIABLE-COEFFICIENT ODE SOLVER [J].
BROWN, PN ;
BYRNE, GD ;
HINDMARSH, AC .
SIAM JOURNAL ON SCIENTIFIC AND STATISTICAL COMPUTING, 1989, 10 (05) :1038-1051
[2]   THE NUMERICAL-SOLUTION OF SOME KINETICS MODELS WITH VODE AND CHEMKIN-II [J].
BYRNE, GD ;
DEAN, AM .
COMPUTERS & CHEMISTRY, 1993, 17 (03) :297-302
[3]  
DEUTSCHMANN O, 1999, IN PRESS AM I CHEM E
[4]  
DEUTSCHMANN O, 1996, P 26 S COMB NAPL IT
[5]  
DEUTSCHMANN OD, 1998, 27 INT C COMB BOULD
[6]   EFFECT OF PRESSURE ON 3 CATALYTIC PARTIAL OXIDATION REACTIONS AT MILLISECOND CONTACT TIMES [J].
DIETZ, AG ;
SCHMIDT, LD .
CATALYSIS LETTERS, 1995, 33 (1-2) :15-29
[7]  
Frenklach M., 1995, OSTI200217
[8]   FINITE-ELEMENT MODEL FOR A CATALYTIC MONOLITH REACTOR [J].
HAYES, RE ;
KOLACZKOWSKI, ST ;
THOMAS, WJ .
COMPUTERS & CHEMICAL ENGINEERING, 1992, 16 (07) :645-657
[9]  
Kee R. J., 1991, CHEMKIN 2 FORTRAN CH
[10]   Isothermal chain-branching, reaction exothermicity, and transport interactions in the stability of methane/air mixtures [J].
Park, YK ;
Vlachos, DG .
COMBUSTION AND FLAME, 1998, 114 (1-2) :214-230