Complete and partial catalytic oxidation of methane over substrates with enhanced transport properties

被引:48
作者
Lyubovsky, M [1 ]
Karim, H [1 ]
Menacherry, P [1 ]
Boorse, S [1 ]
LaPierre, R [1 ]
Pfefferle, WC [1 ]
Roychoudhury, S [1 ]
机构
[1] Precis Combust Inc, N Haven, CT 06473 USA
关键词
mass transfer rate; catalytic combustion; partial oxidation; syngas; natural gas;
D O I
10.1016/S0920-5861(03)00231-1
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The development of improved substrate properties for catalytic combustion has been an area of much interest in recent years. Towards this end, Precision Combustion Inc. has developed novel short channel length, high cell density substrates (trademarked Microlith((R))) and high surface area ceramic coatings for them. These substrates avoid substantial boundary layer buildup and greatly enhance heat and mass transfer rates in reactors. The high cell density of these substrates results in high amount of the catalyst per unit of reactor volume. In this paper we examine the performance of these substrates coated with precious metal catalysts for the catalytic combustion and reforming of methane. Under fuel-lean operating conditions the surface temperature of Pd-based catalyst supported on Microlitho((R)) substrate and the temperature of the gas exiting the reactor remain stable at similar to800 degreesC over a wide range of inlet conditions. This is attributed to combination of enhanced transport properties and characteristics of Pd-PdO transformation. Preheating of the gas mixture in the Microlitho((R)) reactor was sufficient to stabilize a downstream premixed flame with NOx CO, and UHC emissions in the single digit ppm range. Microlitho((R)) substrates were also examined for partial oxidation of methane under fuel-rich conditions. The enhanced transport properties of the Microlitho((R)) substrate allowed complete conversion of methane with surface temperature not exceeding material limits at 93% selectivity to partial oxidation products. High flow rate of reactants result in extremely high power densities and syngas output. The catalyst performance was observed to be stable over 500h of operation. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码:183 / 197
页数:15
相关论文
共 19 条
[1]   Primary reaction steps and active surface sites in the rhodium-catalyzed partial oxidation of methane to CO and H-2 [J].
Buyevskaya, OV ;
Walter, K ;
Wolf, D ;
Baerns, M .
CATALYSIS LETTERS, 1996, 38 (1-2) :81-88
[2]   RHODIUM-CATALYZED PARTIAL OXIDATION OF METHANE TO CO AND H-2 - TRANSIENT STUDIES ON ITS MECHANISM [J].
BUYEVSKAYA, OV ;
WOLF, D ;
BAERNS, M .
CATALYSIS LETTERS, 1994, 29 (1-2) :249-260
[3]  
CARTER RN, 1997, P MRS S, V454
[4]   PARTIAL OXIDATION OF METHANE TO CARBON-MONOXIDE AND HYDROGEN OVER A NI/AL2O3 CATALYST [J].
DISSANAYAKE, D ;
ROSYNEK, MP ;
KHARAS, KCC ;
LUNSFORD, JH .
JOURNAL OF CATALYSIS, 1991, 132 (01) :117-127
[5]  
FUJITANI Y, 1978, Patent No. 4087259
[6]   Modeling homogeneous and heterogeneous chemistry in the production of syngas from methane [J].
Goralski, CT ;
O'Connor, RP ;
Schmidt, LD .
CHEMICAL ENGINEERING SCIENCE, 2000, 55 (08) :1357-1370
[7]   SYNTHESIS GAS-FORMATION BY DIRECT OXIDATION OF METHANE OVER RH MONOLITHS [J].
HICKMAN, DA ;
HAUPFEAR, EA ;
SCHMIDT, LD .
CATALYSIS LETTERS, 1993, 17 (3-4) :223-237
[8]  
JACOBS L, 1996, Patent No. 5510056
[9]  
KOLACZKOWSKI ST, 1995, T I CHEM ENG-LOND, V73, P168
[10]  
KRAEMER G, 1997, P INT C JOINT POW GE