Effects of hydrogen preconversion on the homogeneous ignition of fuel-lean H2/O2/N2/CO2 mixtures over platinum at moderate pressures

The impact of fractional hydrogen preconversion on the subsequent homogeneous ignition characteristics of fuel-lean (equivalence ratio φ = 0.30) H2/O2/N2/CO2 mixtures over platinum was investigated experimentally and numerically at pressures of 1, 5 and 8 bar. Experiments were performed in an optically accessible channel-flow reactor and involved Raman measurements of major species over the catalyst boundary layer and planar laser induced fluorescence (LIF) of the OH radical. Simulations were carried out with a 2-D elliptic code that included detailed hetero-/homogeneous chemistry. The predictions reproduced the LIF-measured onset of homogeneous ignition and the Raman-measured transport-limited catalytic hydrogen consumption. For 0% preconversion and wall temperatures in the range 900 K ⩽ Tw ⩽ 1100 K, homogeneous ignition was largely suppressed for p ⩾ 5 bar due to the combined effects of intrinsic gas-phase hydrogen kinetics and the competition between the catalytic and gas-phase pathways for fuel consumption. A moderate increase of preconversion to 30% restored homogeneous combustion for p ⩾ 5 bar, despite the fact that the water formed due to the upstream preconversion inhibited homogeneous ignition. The catalytically-produced water inhibited gas-phase combustion, particularly at higher pressures, and this kinetic inhibition was exacerbated by the diffusional imbalance of hydrogen that led to over-stoichiometric amounts of water in the near-wall hot ignitable regions. Radical adsorption/desorption reactions hindered the onset of homogeneous ignition and this effect was more pronounced at 1 bar. On the other hand, over the post-ignition reactor length, radical adsorption/desorption reactions significantly suppressed gas-phase combustion at 5 and 8 bar while their impact at 1 bar was weaker. By increasing hydrogen preconversion, the attained superadiabatic surface temperatures could be effectively suppressed. An inverse catalytically stabilized thermal combustion (CST) concept has been proposed, with gas-phase ignition achieved in an upstream porous burner via radiative and heat conduction feedback from a follow-up catalytic reactor. This arrangement moderated the superadiabatic surface temperatures and required modest or no preheat of the incoming mixture.