Influence of the mobility of oxygen in a complex oxide carrier on the mechanism of partial oxidation of methane

The catalytic partial oxidation of methane was studied over single channels of monolith catalysts Pt/PrCeZrO/alpha-Al(2)O(3) and Pt/GdCeZrO/alpha-Al(2)O(3) using the temporal analysis of products (TAP) and kinetic transients. Effects of catalyst composition, oxidation state, time offset between O(2) and CH(4) pulses on activity, selectivity and dynamics of product formation were elucidated. Realization of the direct pyrolysis-CH(4) partial oxidation route was reliably established. This route is favored by optimum lattice/surface oxygen mobility and reactivity controlled by the dopant type (Gd, Pr) and oxidation state of the complex cerium/zirconium oxide.