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A wire microcalorimetric study of catalytic ignition of methane–air mixtures over palladium oxide
Authors:Taichang Zhang  Delin Zhu  Nan Yao  Fei Qi  Chung K Law
Institution:aDepartment of Mechanical and Aerospace Engineering, Princeton University, Princeton, NJ 08544, USA;bPrinceton Institute for the Science and Technology of Materials, Princeton University, Princeton, NJ 08544, USA;cNational Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, PR China
Abstract:Catalytic ignition and heat release of methane oxidation over a Pd wire covered with a 1–2 μm PdO surface layer were investigated by wire microcalorimetry over the temperature range of 600–770 K and pressure range of 0.5–4 atm. Ignition temperatures and heat release rates for different methane concentrations (1–4 vol.% in dry air) were determined, showing that the ignition temperatures decrease with increasing the methane concentration and increasing ambient pressure. At total pressure of 1 atm and 2% methane concentration, the global activation energy for the catalytic reaction is 21.5 ± 0.9 kcal/mol and 14.3 ± 0.2 kcal/mol in the temperature ranges of 600–670 K and 670–770 K, respectively. The reaction order for methane is 0.9 ± 0.1 over the temperature range of 630–770 K.
Keywords:Palladium oxide  Methane  Catalytic oxidation  Kinetics
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