The dry reforming of methane (DRM) is an attractive process due to its simultaneous consumption of two potent greenhouse gases and production of syngas, which is a crucial starting material for many value-added chemicals. However, DRM is a highly endothermic reaction and on the industrial scale requires high operating temperatures and catalytic reactors, which are subject to poisoning by carbon deposition. Alternative methods that utilize milder reaction conditions have been investigated, including the use of plasma reactors. The combination of a plasma discharge with a traditional DRM catalyst has been reported to demonstrate energy efficiency and product selectivity that exceed the sum of the individual processes. This effect is not well understood, and there is a lack of fundamental knowledge regarding the interaction between the plasma species and the catalyst. We have carried out ab initio calculations of various plasma discharge species (CH3, CH4, CO, CO2, H, O) on single crystal surfaces of nickel in an effort to identify mechanisms responsible for the reported plasma-catalysis synergistic effects. We investigate adsorption and co-adsorption energies for these plasma species, as well as surface reaction barriers and pathways.

Ab initio studies of plasma: Surface interactions in the plasma-catalytic dry reforming of methane

251st National Meeting (2016)

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