Fanggang Zhang, Dong Han, John Mantzaras, Chung K. Law, Ran Sui
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引用次数: 0
Abstract
The catalytic total oxidation of propane over platinum was investigated experimentally and numerically at pressures of 1–7 bar and catalyst temperatures up to 700 K. A wire microcalorimeter was employed to determine the global rate parameters of the catalytic reaction within the kinetically controlled regime. For 1 bar pressure, the dissociative adsorption of CH on Pt and its subsequent decomposition were modeled as two lumped steps based on global reaction parameters. A detailed and thermodynamically consistent catalytic mechanism was constructed by incorporating these lumped steps with an existing atmospheric-pressure H-C elementary reaction model. Two-dimensional CFD simulations using the developed global and detailed reaction mechanisms closely reproduced the measured heat release rates. The intricate dependence of catalytic ignition and reactivity on pressure was further elucidated. Ignition temperatures were found to be linearly correlated to pressures, due to the weaker net adsorption of oxygen compared to that of propane, which progressively aggravated at higher pressures and in turn hindered ignition. More importantly, a non-monotonic pressure dependence of the CH catalytic reactivity on Pt, which gradually diminishes with increasing temperatures, is reported for the first time. The temperature range of this non-monotonic behavior (< 650 K) is of special importance for part-load and idling operations of gas turbines using hybrid hetero-/homogeneous combustion approaches and for normal operations of recuperative microreactors. Thus, this work provides key information for the design and optimization of such devices utilizing Pt as catalyst.
期刊介绍:
The Proceedings of the Combustion Institute contains forefront contributions in fundamentals and applications of combustion science. For more than 50 years, the Combustion Institute has served as the peak international society for dissemination of scientific and technical research in the combustion field. In addition to author submissions, the Proceedings of the Combustion Institute includes the Institute''s prestigious invited strategic and topical reviews that represent indispensable resources for emergent research in the field. All papers are subjected to rigorous peer review.
Research papers and invited topical reviews; Reaction Kinetics; Soot, PAH, and other large molecules; Diagnostics; Laminar Flames; Turbulent Flames; Heterogeneous Combustion; Spray and Droplet Combustion; Detonations, Explosions & Supersonic Combustion; Fire Research; Stationary Combustion Systems; IC Engine and Gas Turbine Combustion; New Technology Concepts
The electronic version of Proceedings of the Combustion Institute contains supplemental material such as reaction mechanisms, illustrating movies, and other data.