Synergistic Effects of Ternary PdO-CeO2-OMS-2 Catalyst Afford High Catalytic Performance and Stability in the Reduction of NO with CO.

Abstract

We developed a robust ternary PdO-CeO2-OMS-2 catalyst with excellent catalytic performance in the selective reduction of NO with CO using a strategy based on combining components that synergistically interact leading to an effective abatement of these toxic gases. The catalyst affords 100% selectivity to N2 at the nearly full conversion of NO and CO at 250 °C, high stability in the presence of H2O, and a remarkable SO2 tolerance. To unravel the origin of the excellent catalytic performance, the structural and chemical properties of the PdO-CeO2-OMS-2 nanocomposite were analyzed in the as-prepared and used state of the catalyst, employing a series of pertinent characterization methods and specific catalytic tests. The experimental as well as theoretical results, based on density-functional theory calculations suggest that CO and NO follow different reaction pathways, CO is preferentially adsorbed and oxidized at Pd sites (PdII and Pd0), while NO decomposes on the ceria surface. Lattice oxygen vacancies at the interfacial perimeter of PdO-CeO2 and PdO-OMS-2, and the diffusion of oxygen and oxygen vacancies are proposed to play a critical role in this multicenter reaction system.