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At high temperatures, the oxidative coupling of methane (OCM) is an attractive approach for catalytic conversion of methane into value-added chemicals. Experiments with a Pt/Al2O3-coated catalytic honeycomb monolith were conducted with varying CH4/O2 ratios, N2 dilution at atmospheric pressure, and very short contact times. The reactor was modeled by a multiscale approach using a parabolic two-dimensional flow field description in the monolithic channels coupled with a heat balance of the monolithic structure, and multistep surface reaction mechanisms as well as elementary-step, gas phase reaction mechanisms. The contribution of heterogeneous and homogeneous reactions, both of which are important for the optimization of C2 products, is investigated using a combination of experimental and computational methods. The oxidation of methane, which takes place over the platinum catalyst, causes the adiabatic temperature increase required for the generation of CH3 radicals in the gas phase, which are essential for the formation of C2 species. Lower CH4/O2 ratios result in higher C2 selectivity. However, the presence of OH radicals at high temperatures facilitates subsequent conversion of C2H2 at a CH4/O2 ratio of 1.4. Thereby, C2 species selectivity of 7% was achieved at CH4/O2 ratio of 1.6, with 35% N2 dilution.

Oxidative Coupling of Methane over Pt/Al2O3 at High Temperature: Multiscale Modeling of the Catalytic Monolith