期刊
COMBUSTION AND FLAME
卷 157, 期 3, 页码 421-435出版社
ELSEVIER SCIENCE INC
DOI: 10.1016/j.combustflame.2009.07.012
关键词
Catalytic combustion; Ignition; Gas-surface reaction; Kinetic modeling; Microscopy; Flow reactor; Particle size distribution
类别
资金
- Air Force Office of Scientific Research [FA9550-08-1-0400]
- AFOSR STTR [FA8650-06-C-2673, FA9550-07-0106]
Catalytic ignition of methane over the surfaces of freely-suspended and in situ generated palladium nanoparticles was investigated experimentally and numerically. The experiments were conducted in a laminar flow reactor. The palladium precursor was a compound (Pd(THD)(2), THD: 2,2,6,6-tetramethyl-3,5-heptanedione) dissolved in toluene and injected into the flow reactor as a fine aerosol, along with a methane-oxygen-nitrogen mixture. For experimental conditions chosen in this study, non-catalytic, homogeneous ignition was observed at a furnace temperature of similar to 1123 K, whereas ignition of the same mixture with the precursor was found to be similar to 973 K. In situ production of Pd/PdO nanoparticles was confirmed by scanning mobility, transmission electron microscopy and X-ray photoelectron spectroscopy analyses of particles collected at the reactor exit. The catalyst particle size distribution was log-normal. Depending on the precursor loading, the median diameter ranged from 10 to 30 nm. The mechanism behind catalytic ignition was examined using a combined gas-phase and gas-surface reaction model. Simulation results match the experiments closely and suggest that palladium nanocatalyst significantly shortens the ignition delay times of methane-air mixtures over a wide range of conditions. (C) 2009 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
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