An experimental and numerical investigation of the hetero-/homogeneous combustion of fuel-rich hydrogen/air mixtures over platinum

The hetero-/homogeneous combustion of hydrogen/air mixtures over platinum was investigated experimentally and numerically in a channel-flow configuration at fuel-rich equivalence ratios ranging from 2 to 7, pressures up to 5 bar and wall temperatures 760–1200 K. Experiments involved in situ one-dimensional Raman measurements of major gas-phase species concentrations over the catalyst boundary layer and planar laser induced fluorescence (LIF) of the OH radical, while simulations included an elliptic 2-D model with detailed heterogeneous and homogeneous reaction mechanisms. The employed reaction schemes reproduced the measured catalytic reactant consumption, the onset of homogeneous ignition, and the post-ignition flame shapes at all examined conditions. Although below a critical pressure, which depended on temperature, the intrinsic gas-phase kinetics of hydrogen dictated lower reactivity for the fuel-rich stoichiometries when compared to fuel-lean ones, homogeneous ignition was still more favorable for the rich stoichiometries due to the lower molecular transport of the deficient oxygen reactant that resulted in modest catalytic reactant consumption over the gaseous induction zone. Above the critical pressure, the intrinsic gaseous hydrogen kinetics yielded higher reactivity for the rich stoichiometries, which resulted in vigorous gaseous combustion at pressures up to 5 bar, in contrast to lean stoichiometry studies whereby homogeneous combustion was altogether suppressed above 3 bar. Computations at fuel-rich stoichiometries in practical channel geometries indicated that homogeneous combustion was not of concern for reactor thermal management, since the larger than unity Lewis number of the deficient oxygen reactant confined the flames to the core of the channel, away from the solid walls.