Abstract

The focus of this study was to elucidate the synergy of MOx (M = La, Ba and Zr) and phosphorus additives in Pd/γ-Al2O3 catalyst towards methane oxidation. It was revealed that the MOx addition as a second promoter positively influenced catalyst performance. The generation of extra MOx-PdO interface facilitated the crystallization of PdO grains as a result of the change in the interfacial tension and then the contact angles of palladium nanoparticles, yielding enhanced reducing property jointly with richer palladium step sites, which preferred catalysts with superior activity. Moreover, MOx dopant provided more surface oxygen species over catalysts due to its electron-donating effect, inhibited the OH/H2O accumulation and gave lower surface acidity/basicity ratio, improving both activity and moisture-tolerance. Amongst, Pd/La-PAl manifested the optimum activity and excellent durability during 60-h on-stream reaction. It completely catalyzed methane oxidation at around 310 °C after In situ reaction activation and treatment in methane atmosphere.

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