Performance Projection of a High-Temperature CO2 Transport Membrane Reactor for Combined CO2 Capture and Methane-to-Ethylene Conversion

Abstract

Direct conversion of methane into ethylene through the oxidative coupling of methane (OCM) is a technically important reaction. However, conventional co-fed fixed-bed OCM reactors still face serious challenges in conversion and selectivity. In this paper, we apply a finite element model to simulate OCM reaction in a plug-flow CO2/O2 transport membrane (CTM) reactor with a directly captured CO2 and O2 mixture as a soft oxidizer. The CTM is made of three phases: molten carbonate, 20% Sm-doped CeO2, and LiNiO2. The membrane parameters are first validated by CO2/O2 flux data obtained from CTM experiments. The OCM reaction is then simulated along the length of tubular plug-flow reactors filled with a La2O3-CaO-modified CeO2 catalyst bed, while a mixture of CO2/O2 is gradually added through the wall of the tubular membrane. A 12-step OCM kinetic mechanism is considered in the model for the catalyst bed and validated by data obtained from a co-fed fixed-bed reactor. The modeled results indicate a much-improved OCM performance by membrane reactor in terms of C2-yield and CH4 conversion rate over the state-of-the-art, co-fed, fixed-bed reactor. The model further reveals that improved performance is fundamentally rooted in the gradual methane conversion with CO2/O2 offered by the plug-flow membrane reactor.