Kinetics of catalytic oxidation of methane, ethane and propane over palladium oxide

被引:36
作者
Xin, Yuxuan [1 ]
Wang, Hai [2 ]
Law, Chung K. [1 ,3 ]
机构
[1] Princeton Univ, Dept Mech & Aerosp Engn, Princeton, NJ 08544 USA
[2] Univ So Calif, Dept Aerosp & Mech Engn, Los Angeles, CA 90089 USA
[3] Tsinghua Univ, Ctr Combust Energy, Beijing 100084, Peoples R China
关键词
Catalytic combustion; Pd-based catalyst; Alkane oxidation; Surface chemistry model; COMBUSTION; IGNITION; HYDROCARBONS; MIXTURES; SURFACE;
D O I
10.1016/j.combustflame.2013.10.023
中图分类号
O414.1 [热力学];
学科分类号
摘要
Catalytic oxidation of methane, ethane and propane over a palladium oxide (PdO) surface was investigated experimentally by wire microcalorimetry. The oxidation rate was determined for each reactant at atmospheric pressure in the temperature range of 600-800 K. The apparent kinetic parameters were extracted from the experimental measurements. It is shown that the oxidation of these hydrocarbons over the PdO surface proceeds with a similar mechanism: they undergo dissociative adsorption followed by the conversion of surface fragments to final products. A detailed surface reaction model is proposed, and the kinetic parameters of the crucial reactions are deduced from the present experimental observations. The catalytic oxidation rates are found to increase in the order of methane, ethane and propane. This observation is consistent with density functional theory calculations and may be correlated with the C-H bond energies of the corresponding surface intermediates. (C) 2013 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
引用
收藏
页码:1048 / 1054
页数:7
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