Theoretical and experimental study of methane steam reforming reactions over nickel catalyst

In this work we perform DFT theoretical calculations of methane and steam interactions on Ni(1 1 1) surface. The calculations allow us to improve our understanding of the competition between these reactants by catalytic sites in methane steam reforming (MSR) process. For this purpose we compare theoretical results with kinetic measurements of MSR on a Ni(II)–Al(III) catalyst prepared from lamellar double hydroxides as precursor. This comparison shows that, for low H2O/CH4 ratios methane and water intermediate species adsorb on different catalytic sites. While CHO species adsorbs on top of Ni atom, OH one occupies preferentially a tri-coordinate surface site. On the other hand, for high H2O/CH4 ratios a competency between these species by Ni sites would establish, diminishing methane conversion. In addition competition between methane and steam for Ni sites would lead to a decrease in CO production. Nevertheless, intermediate species adsorbed on different active sites would produce CO2, whatever the steam/methane ratio. Thus, it would be optimum steam concentration in hydrocarbon feed and active sites distribution on catalyst surface, which could maximize H2 production and minimize CO selectivity. The theoretical findings agree with kinetic measurements, which show that maximum methane conversion depends on steam partial pressure in the feed; whereas always, selectivity to CO2 increases and to CO diminishes