Due to the uprising worldwide concern towards global warming and the installation of the carbon tax, there is an increasing interest in the dry reforming of methane (DRM) since it transforms two greenhouse gases like CO2 and CH4 to a higher value product such as syngas (CO and H2) (Equation 1). The DRM is a highly endothermic reaction and needs significant temperature to obtain significant conversion (ca. 650 °C). CH4 + CO2 → 2CO + 2H2 DH ° = +247 kJ.mol-1 (1) In this contribution, present our work DRM reaction on Ru (0001) surface, following our previous works in the field. Ru is one of the most active monometallic catalysts for the reaction, therefore we evaluated its performance using density functional theory (DFT) and kinetic Montecarlo Simulations. DFT results show that the activation energy of CO2 via direct dissociation is lower than that of CH4 by 19 kJ mol–1 and therefore the latter is more energy demanding than the former. After the CH4 activation, the mechanism can proceed via the HCO* intermediate formation via CH + O reaction, which is less energy demanding than the direct C + O coupling. According to the results based on the sequential energy profile shown in Figure 1, the CH4 activation is the most energetically demanding step of the DRM reaction. Finally, we also evaluated the selectivity of Ru catalyst surface to dry reforming through microkinetic Montecarlo simulations to evaluate the interplay between the key reaction steps and understand in more detail the DRM reaction on the Ru(0001) model surface.

Dry reforming of methane on Ru (0001): DFT calculations and microkinetic Montecarlo simulation

ACS Fall 2021

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