Reaction kinetics for high pressure hydrogen oxy-combustion in the presence of high levels of H2O and CO2

Abstract

Novel shock tube experimental ignition delay time (IDT) data are provided to delineate the impact of high concentrations (45% by mole) of H2O and CO2 on IDTs of stoichiometric 4% H2. Ignition delay experiments were conducted using a high- and a low-pressure shock tube facility. High-pressure experiments were performed at pressures of 37-43.8 bar and temperatures of 1084-1242 K in four different bath gases, namely: Ar, 45%H2O/Ar, 30%H2O/15%CO2/Ar, and 45%CO2/Ar. Low-pressure experiments were conducted at 2.1-2.7 bar and 926-1198 K in Ar and 45%CO2/Ar bath gases. Impacts of non-ideal ignition phenomena that may occur in the presence of large amounts of H2O and CO2 were also analyzed. A minimally-tuned H2/CO reaction mechanism, CanMECH 1.0, targeting high-pressure combustion in the presence of large concentrations of H2O and CO2 is presented. The mechanism is constructed from unadjusted kinetic rate parameters from theoretical / experimental elementary reaction rate determinations. The only adjusted rate in CanMECH 1.0 is the much disputed Ar-specific low-pressure-limit pre-exponential factor of H + O2 (+Ar) = HO2 (+Ar) within the uncertainty bounds of the source rate. Validity of CanMECH 1.0 is confirmed against shock tube IDT data of this work, as well as selected H2 and H2/CO shock tube IDT datasets from literature. The performance of the model is compared to Keromnes et al. model (Combust. Flame 160 (2013) 995-1011). CanMECH 1.0 outperformed Keromnes et al. for 16 datasets out of 26 and exhibited a similar performance for another two. In particular, CanMECH 1.0 outperformed Keromnes et al. in predicting shock tube IDTs for H2O- and CO2-laden reactive mixtures, as well as all IDT data at pressures of 17-43.8 bar, which are of distinct value to pressurized oxy-fuel combustion applications relevant to this work.