Descriptor Design in the Computational Screening of Ni-based Catalysts with Balanced Activity and Stability for the Dry Reforming of Methane Reaction

Dry reforming of methane (DRM) is an important reaction in the actual environmental and energy crisis context. It enables the production of syngas from CO2 and CH4 reforming. While Ni catalyst presents a high activity regarding this process, it often suffers from deactivation. It was found that the Sn-doped Ni catalyst can avoid carbon deposition, but a decrease in DRM reactivity was also observed. In this work, we used density functional theory calculations in combination with microkinetic modeling firstly in order to understand how Sn doping affects the resistance to carbon deposition and the surface catalytic activities of Ni. Based on the understandings, we found that an ideal dopant should give rise to a proper adsorption energy of carbon, such that (i) the C* formation process, e.g. CH4 dissociation, is rate controlling to improve the carbon resistance, and (ii) relatively low dissociation barriers of CH4 and CO2 can be achieved to maintain a good activity. Therefore, the adsorption energy of carbon...