Ignition in alkane oxidation on noble-metal catalysts

被引:111
作者
Veser, G
Ziauddin, M
Schmidt, LD
机构
[1] Univ Minnesota, Dept Chem Engn & Mat Sci, Minneapolis, MN 55455 USA
[2] Univ Stuttgart, Inst Chem Verfahrenstech, D-70199 Stuttgart, Germany
关键词
catalytic hydrocarbon oxidation; noble metal catalysts; ignition/extinction; homogeneous-heterogeneous reactions;
D O I
10.1016/S0920-5861(98)00302-2
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The ignition behavior in the oxidation of four simple alkanes (methane, ethane, propane and isobutane) with air on a platinum-foil catalyst, as well as that of ethane/air mixtures on four noble-metal foil catalysts (Pt, Pd, Ph, and Ir) was studied at atmospheric pressure over the entire range of fuel-to-air ratios. While, Pd showed the widest range of surface flammability, ignition temperatures for ethane/air mixtures were lowest on Pt. Both, Rh and Ir deactivated rapidly under fuel-lean conditions and ignited considerably higher than Pd and Pt. The surface ignition temperatures were found to correlate well with the C-H bond energy of the hydrocarbon and the metal-oxygen bond energy of the noble metal. A very simple analytical model was able to reproduce the dependence of surface ignition temperatures on fuel-to-air ratios, yielding apparent activation energies for the surface reactions and indicating an oxygen-covered surface before catalytic ignition due to strong site competition between the hydrocarbon and oxygen on the catalyst surface. (C) 1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:219 / 228
页数:10
相关论文
共 26 条
[1]   BOND ENERGIES [J].
BENSON, SW .
JOURNAL OF CHEMICAL EDUCATION, 1965, 42 (09) :502-&
[2]   SOME INNOVATIVE ASPECTS IN THE PRODUCTION OF MONOMERS VIA CATALYZED OXIDATION PROCESSES [J].
CAVANI, F ;
TRIFIRO, F .
APPLIED CATALYSIS A-GENERAL, 1992, 88 (02) :115-135
[3]   CATALYTIC IGNITION OF FUEL OXYGEN NITROGEN MIXTURES OVER PLATINUM [J].
CHO, P ;
LAW, CK .
COMBUSTION AND FLAME, 1986, 66 (02) :159-170
[4]  
CUSUMANO JA, 1992, CHEMTECH, P482
[5]  
Eigenberger G., 1994, INT CHEM ENG, V34, P4
[6]   CATALYTIC CHEMISTRY OF SUPPORTED PALLADIUM FOR COMBUSTION OF METHANE [J].
FARRAUTO, RJ ;
HOBSON, MC ;
KENNELLY, T ;
WATERMAN, EM .
APPLIED CATALYSIS A-GENERAL, 1992, 81 (02) :227-237
[7]   GAS-PHASE AND CATALYTIC IGNITION OF METHANE AND ETHANE IN AIR OVER PLATINUM [J].
GRIFFIN, TA ;
PFEFFERLE, LD .
AICHE JOURNAL, 1990, 36 (06) :861-870
[8]   DEHYDROGENATION, HYDROGENATION, EXCHANGE AND COMBUSTION REACTIONS OF AROMATIC-HYDROCARBONS ON PD(100) [J].
GUO, XC ;
MADIX, RJ .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1995, 91 (20) :3685-3694
[9]  
HIAM L, 1968, J CATAL, V9, P272
[10]   PARTIAL OXIDATION OF ALKANES OVER NOBLE-METAL COATED MONOLITHS [J].
HUFF, M ;
TORNIAINEN, PM ;
SCHMIDT, LD .
CATALYSIS TODAY, 1994, 21 (01) :113-128