Homogeneous combustion of fuel-lean H2/O2/N2 mixtures over platinum at elevated pressures and preheats

The gas-phase combustion of H-2/O-2/N-2 mixtures over platinum was investigated experimentally and numerically at fuel-lean equivalence ratios up to 0.30, pressures up to 15 bar and preheats up to 790 K. In situ 1-D spontaneous Raman measurements of major species concentrations and 2-D laser induced fluorescence (LIF) of the OH radical were applied in an optically accessible channel-flow catalytic reactor, leading to the assessment of the underlying heterogeneous (catalytic) and homogeneous (gas-phase) combustion processes. Simulations were carried out with a 2-D elliptic code that included elementary hetero-/homogeneous chemical reaction schemes and detailed transport. Measurements and predictions have shown that as pressure increased above 10 bar the preheat requirements for significant gas-phase hydrogen conversion raised appreciably, and for p = 15 bar (a pressure relevant for gas turbines) even the highest investigated preheats were inadequate to initiate considerable gas-phase conversion. Simulations in channels with practical geometrical confinements of 1 mm indicated that gas-phase combustion was altogether suppressed at atmospheric pressure, wall temperatures as high as 1350 K and preheats up to 773 K. While homogeneous ignition chemistry controlled gaseous combustion at atmospheric pressure, flame propagation characteristics dictated the strength of homogeneous combustion at the highest investigated pressures. The decrease in laminar burning rates for p >= 8 bar led to a push of the gaseous reaction zone close to the channel wall, to a subsequent leakage of hydrogen through the gaseous reaction zone, and finally to catalytic conversion of the escaped fuel at the channel walls. Parametric studies delineated the operating conditions and geometrical confinements under which gas-phase conversion of hydrogen could not be ignored in numerical modeling of catalytic combustion. (C) 2010 The Combustion Institute. Published by Elsevier Inc. All rights reserved.