The effects of CO2/CH4 ratio on soot formation for autothermal reforming of methane at elevated pressure

Abstract

Autothermal reforming of methane (ATR) technique is a promising technology for H2 production. Soot formed in the combustion region of ATR may deactivate the downstream catalyst used to enhance the reforming reactions. In this work, the effects of CO2/CH4 ratio on soot production and main gas-phase components involved in reforming reactions were investigated by experiment and numerical simulations in laminar inverse coflow diffusion flames, at conditions close to ATR. The CO2/CH4 ratio ranges from 0.27 to 4.90, and the pressure ranges from 1 atm to 10 atm. The oxidant consists 70% O2 and 30% N2 to mimic the oxy-combustion in the ATR process. The soot, polycyclic aromatic hydrocarbon (PAHs), OH* distribution, and flame structure were measured using planar laser-induced incandesce, planar laser-induced fluorescence, OH* luminescence, and flame luminescence, respectively. High fidelity simulations with a reduced gas-phase kinetic mechanism and soot aerosol models were also undertaken to supplement the findings. The results show that soot formation is suppressed by a higher CO2/CH4 ratio, while the level of soot reduction is attenuated as the pressure increases. The peak soot volume fraction increases with the flame height, and then levels off. PAHs concentration monotonically increases with flame height. The spatial distributions of PAH and soot along flame height were not well captured by numerical simulations, and the used physical based soot inception model is expected to account for the discrepancy. The peak soot volume fraction correlates with CO2/CH4 ratio by an exponentially decaying function, with the exponent decreasing with increasing pressure. A similar trend of PAHs concentration along with CO2/CH4 ratio was also observed. Non-sooting flame is achievable at elevated pressure if the CO2/CH4 ratio is higher than 4.0, at the expense of lowering the syngas yield in the combustion region. The simulations also predicted that the flame temperature and concentration of H2 and CO decrease with CO2/CH4 ratio.