Intrinsic microkinetic effects of spray-drying and SiC co-support on Mn–Na2WO4/SiO2 catalysts used in oxidative coupling of methane†
Abstract
This paper presents a microkinetic model to evaluate the effects of a silicon carbide (SiC) co-support and the shaping method on Mn–Na2WO4/SiO2 catalysts used for the oxidative coupling of methane. The model considers mass transfer, catalytic, and gas-phase kinetics, and it is trained with experimental values (product composition) of three Mn–Na2WO4 catalysts for calculating the kinetic parameters using catalytic descriptors while maintaining thermodynamic consistency. The catalysts were an SiO2-supported catalyst prepared through impregnation and two SiO2–SiC-supported catalysts (with βSiC and α + βSiC) prepared via spray-drying. Our analysis shows how the type of SiC and preparation method affect the textural properties and result in distinct CH3˙ radical oxidation, HO2˙ quenching, C2H4 oxidation, and COX transformation pathways, eventually leading to CH4 conversion and C2 selectivity. Our approach facilitates the assessment of the effects of the promoter and support on individual and global reaction networks.