Modeling the high-temperature catalytic partial oxidation of methane over platinum gauze: Detailed gas-phase and surface chemistries coupled with 3D flow field simulations

Abstract: The high-temperature catalytic partial oxidation (CPO) of methane over a platinum gauze reactor was modeled by three-dimensional numerical simulations of the flow field coupled with heat transport as well as detailed gas-phase and surface reaction mechanisms. Model results agree well with data of CPO experiments over Pt-gauzes in the literature, confirming the presence of strong mass and heat-transport limitations. The conversions of CH4 and O2 increase with an increased contact time and were practically constant in the temperature range of 1000–1200K. The selectivity to CO linearly increases with temperature. H2 was only observed above 1200K, below this temperature H2O was the only hydrogen-containing product. The contribution of heterogeneous steps in the overall process is prominent, but in the later stages of the reactor, gas-phase reactions become significant at certain conditions of temperature, pressure, and residence time. For example, simulations predicted some gas-phase production of ethane and ethylene via methane oxidative coupling at elevated pressure and residence time. The study shows that today''s CFD tools allow the implementation of detailed homogeneous and heterogeneous reaction schemes even for complex catalyst geometries. [Copyright &y& Elsevier]