Steam reforming of methane, ethane, propane, butane, and natural gas over a rhodium-based catalyst

被引:169
作者
Schaedel, Benjamin T. [1 ]
Duisberg, Matthias [2 ]
Deutschmann, Olaf [1 ]
机构
[1] Univ Karlsruhe, Inst Chem Technol & Polymer Chem, D-76131 Karlsruhe, Germany
[2] Umicore AG & Co KG, D-63403 Hanau, Germany
关键词
Steam reforming; Detailed mechanism; Rh; Numerical simulation; Hydrogen production; Natural gas; SURFACE-REACTION MECHANISM; PARTIAL OXIDATION; COMBUSTION; SIMULATION; ACTIVATION; ADSORPTION; CONVERSION; HYDROGEN; BEHAVIOR; REACTOR;
D O I
10.1016/j.cattod.2009.01.008
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Steam reforming of methane, ethane, propane, butane, and a sulfur-free natural gas is studied over a rhodium-based monolithic honeycomb catalyst. The product distribution is analyzed as function of temperature (250-900 degrees C) and steam-to-carbon ratio (2.2-4) for two honeycomb channel densities (600 and 900 cpsi) and an uncoated monolith by gas chromatography and mass spectroscopy. The reactive flow in the single monolith channel is modeled by a two-dimensional flow field description coupled with detailed reaction mechanisms modeling surface and gas-phase kinetics. Ethane, propane, and butane are converted at much lower temperature than methane, also in natural gas mixtures. An impact of the presence of the higher hydrocarbons on methane conversion in steam reforming of natural gas is found. Steam reforming in the pure gas phase occurs only above 600 degrees C and the product spectrum differs from that of catalytic conversion. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:42 / 51
页数:10
相关论文
共 48 条
[1]   Temperature profiles and residence time effects during catalytic partial oxidation and oxidative steam reforming of propane in metallic microchannel reactors [J].
Aartun, I ;
Venvik, HJ ;
Holmen, A ;
Pfeifer, P ;
Görke, O ;
Schubert, K .
CATALYSIS TODAY, 2005, 110 (1-2) :98-107
[2]  
BAUMANN F, 2004, P 13 INT C CAT PAR
[3]  
Cao CS, 2005, CATAL TODAY, V110, P92, DOI 10.1016/j.cattod.2005.09.004
[4]   Detailed surface reaction mechanism in a three-way catalyst [J].
Chatterjee, D ;
Deutschmann, O ;
Warnatz, J .
FARADAY DISCUSSIONS, 2001, 119 :371-384
[5]   ONE-STEP AND EXTRAPOLATION METHODS FOR DIFFERENTIAL-ALGEBRAIC SYSTEMS [J].
DEUFLHARD, P ;
HAIRER, E ;
ZUGCK, J .
NUMERISCHE MATHEMATIK, 1987, 51 (05) :501-516
[6]   Modeling the partial oxidation of methane in a short-contact-time reactor [J].
Deutschmann, O ;
Schmidt, LD .
AICHE JOURNAL, 1998, 44 (11) :2465-2477
[7]  
Deutschmann O, 2007, HDB HETEROGENEOUS CA
[8]  
Deutschmann O, 2007, DETCHEM SOFTWARE PAC
[9]   A multistep surface mechanism for ethane oxidative dehydrogenation on Pt- and Pt/Sn-coated monoliths [J].
Donsì, F ;
Williams, KA ;
Schmidt, LD .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2005, 44 (10) :3453-3470
[10]   Simulation of the natural gas steam reforming process for PEFC systems [J].
Echigo, M ;
Tabata, T .
JOURNAL OF CHEMICAL ENGINEERING OF JAPAN, 2004, 37 (06) :723-730