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Oxidation of nitric oxide (NO) for subsequent efficient reduction in selective catalytic reduction or lean NO(x) trap devices continues to be a challenge in diesel engines because of the low efficiency and high cost of the currently used platinum (Pt)-based catalysts. We show that mixed-phase oxide materials based on Mn-mullite (Sm, Gd)Mn(2)O(5) are an efficient substitute for the current commercial Pt-based catalysts. Under laboratory-simulated diesel exhaust conditions, this mixed-phase oxide material was superior to Pt in terms of cost, thermal durability, and catalytic activity for NO oxidation. This oxide material is active at temperatures as low as 120°C with conversion maxima of ~45% higher than that achieved with Pt. Density functional theory and diffuse reflectance infrared Fourier transform spectroscopy provide insights into the NO-to-NO(2) reaction mechanism on catalytically active Mn-Mn sites via the intermediate nitrate species.

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Steady-state IR measurements for adsorption of only CO and under WGS reaction indicate that formates are present on the surface of partially reduced ceria, in contrast to a recent study, and that they are strongly limited at high CO conversions. At low temperatures and conversions, the formates are close to the equilibrium adsorption/desorption coverages obtained from CO adsorption alone. The formates are close to saturation at low temperatures. These IR results favor the bidentate formate mechanism in explaining WGS. However, more kinetic studies are required and over a wider range of temperatures. While low-temperature kinetic studies have found a zero-order dependency for CO and related this to saturation of a noble metal surface, this study indicates that one cannot rule out the possibility of the formate mechanism on this basis, as CO is also close to saturation as an adsorbed formate at the low temperatures used in previous studies.