Effects of H2S addition on hydrogen ignition behind reflected shock waves: Experiments and modeling

Abstract

Hydrogen sulfide is a common impurity that can greatly change the combustion properties of fuels, even when present in small concentrations. However, the combustion chemistry of H2S is still poorly understood, and this lack of understanding subsequently leads to difficulties in the design of emission-control and energy-production processes. During this study, ignition delay times were measured behind reflected shock waves for mixtures of 1% H2/1% O2 diluted in Ar and doped with various concentration of H2S (100, 400, and 1600ppm) over large pressure (around 1.6, 13, and 33atm) and temperature (1045–1860K) ranges. Results typically showed a significant increase in the ignition delay time due to the addition of H2S, in some cases by a factor of 4 or more over the baseline mixtures with no H2S. The magnitude of the increase is highly dependent on the temperature and pressure. A detailed chemical kinetics model was developed using recent, up-to-date detailed-kinetics mechanisms from the literature and by changing a few reaction rates within their reported error factor. This updated model predicts well the experimental data obtained during this study and from the shock-tube literature. However, flow reactor data from the literature were poorly predicted when H2S was a reactant. This study highlights the need for a better estimation of several reaction rates to better predict H2S oxidation chemistry and its effect on fuel combustion. Using the kinetics model for sensitivity analyses, it was determined that the decrease in reactivity in the presence of H2S is because H2S initially reacts before the H2 fuel does, mainly through the reaction H2S+H⇄SH+H2, thus taking H atoms away from the main branching reaction H+O2⇄OH+O and inhibiting the ignition process.